75 results on '"Lian X"'
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2. Study on Printability Evaluation of Alginate/Silk Fibroin/Collagen Double-Cross-Linked Inks and the Properties of 3D Printed Constructs.
- Author
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Feng H, Song Y, Lian X, Zhang S, Bai J, Gan F, Lei Q, Wei Y, and Huang D
- Subjects
- Biocompatible Materials chemistry, Animals, Tissue Scaffolds chemistry, Glucuronic Acid chemistry, Hexuronic Acids chemistry, Materials Testing, Cross-Linking Reagents chemistry, Tissue Engineering methods, Bioprinting methods, Methacrylates chemistry, Humans, Alginates chemistry, Fibroins chemistry, Printing, Three-Dimensional, Collagen chemistry, Ink
- Abstract
In recent years, biological 3D printing has garnered increasing attention for tissue and organ repair. The challenge with 3D-printing inks is to combine mechanical properties as well as biocompatibility. Proteins serve as vital structural components in living systems, and utilizing protein-based inks can ensure that the materials maintain the necessary biological activity. In this study, we incorporated two natural biomaterials, silk fibroin (SF) and collagen (COL), into a low-concentration sodium alginate (SA) solution to create novel composite inks. SF and COL were modified with glycidyl methacrylate (GMA) to impart photo-cross-linking properties. The UV light test and
1 H NMR results demonstrated successful curing of silk fibroin (SF) and collagen (COL) after modification and grafting. Subsequently, the printability of modified silk fibroin (RSFMA)/SA with varying concentration gradients was assessed using a set of three consecutive printing models, and the material's properties were tested. The research results prove that the addition of RSFMA and ColMA enhances the printability of low-concentration SA solutions, with the Pr values increasing from 0.85 ± 0.02 to 0.90 ± 0.03 and 0.92 ± 0.02, respectively, and the mechanical strength increasing from 0.19 ± 0.01 to 0.28 ± 0.01 and 0.38 ± 0.01 MPa; cytocompatibility has also been improved. Furthermore, rheological tests indicated that all of the inks exhibited shear thinning properties. CCK-8 experiments demonstrated that the addition of ColMA increased the cytocompatibility of the ink system. Overall, the utilization of SF and COL-modified SA materials as inks represents a promising advancement in 3D-printed ink technology.- Published
- 2024
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3. Electrohydrodynamic Printing of Microscale Fibrous Scaffolds with a Sinusoidal Structure for Enhancing the Contractility of Cardiomyocytes.
- Author
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Lei Q, Jia J, Guan X, Han K, Liu J, Duan R, Lian X, and Huang D
- Abstract
Mimicking the curved collagenous fibers in the cardiac extracellular matrix to fabricate elastic scaffolds in vitro is important for cardiac tissue engineering. Here, we developed sinusoidal polycaprolactone (PCL) fibrous scaffolds with commendable flexibility and elasticity to enhance the contractility of primary cardiomyocytes by employing melt-based electrohydrodynamic (EHD) printing. Microscale sinusoidal PCL fibers with an average diameter of ∼10 μm were printed to mimic the collagenous fibers in the cardiac ECM. The sinusoidal PCL fibrous scaffolds were EHD-printed in a layer-by-layer manner and exhibited outstanding flexibility and elasticity compared with the straight ones. The sinusoidal PCL scaffolds provided an elastic microenvironment for the attaching and spreading of primary cardiomyocytes, which facilitated their synchronous contractive activities. Primary cardiomyocytes also showed improved gene expression and maturation on the sinusoidal PCL scaffolds under electrical stimulation for 5 days. It is envisioned that the proposed flexible fibrous scaffold with biomimetic architecture may serve as a suitable patch for tissue regeneration and repair of damaged hearts after myocardial infarction.
- Published
- 2024
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4. Controllable Iodoplumbate-Coordination of Hybrid Lead Iodide Perovskites via Additive Engineering for High-Performance Solar Cells.
- Author
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Wang K, Liu H, Huang Q, Duan Z, Wang J, Zhao C, Lian X, Liu R, Su Y, Guan X, Zhang Y, Lv W, Zhou H, Huang G, Shen Y, Zhang H, and Xie F
- Abstract
The crystallization and growth of perovskite crystals are two crucial factors influencing the performance of perovskite solar cells (PSCs). Moreover, iodoplumbate complexes such as PbI
2 , PbI3 - , and PbI4 2- in perovskite precursor solution dictate both the quality of perovskite crystals and the optoelectrical performance of PSCs. Here, we propose an iodoplumbate-coordination strategy that employs pentafluorophenylsulfonyl chloride (PTFC) as an additive to tailor the crystal quality. This strategy directly affects the thermodynamics and kinetics of perovskite crystal formation by regulating hydrogen bonds or coordination bonds with Pb2+ or I- ions. Subsequently, the synergistic effect of the PTFC and FA+ complex was beneficial for intermediate-to-perovskite phase transition, improving the crystalline quality and reducing the defect density in the perovskite film to suppress nonradiative recombination loss. Consequently, the treated PSCs achieved a power conversion efficiency (PCE) of 24.61%, demonstrating enhanced long-term stability under both light and thermal stress. The developed device retained 92.53% of its initial PCE after 1200 h of continuous illumination and 88.6% of its initial PCE after 600 h of 85 °C thermal stability tests, respectively, both conducted in N2 atmospheres.- Published
- 2024
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5. Photoelectrochemical Synthesis of Hydrogen Peroxide from Saline Water via the Two-Electron Water Oxidation Reaction.
- Author
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Guo W, Li M, Wang S, He Y, Zhou Y, and Lian X
- Abstract
Hydrogen peroxide (H
2 O2 ) production on the anode is more valuable than oxygen and chlorine evolution for photoelectrochemical saline water splitting. In this work, by the introduction of bicarbonate (HCO3 - ), H2 O2 is produced from saline water (2 M KHCO3 + 0.5 M NaCl aqueous solution) via the two-electron water oxidation reaction by a photoanode of bismuth vanadate (BiVO4 ). Furthermore, the Faradaic efficiency (FE) and accumulation for H2 O2 are improved by coating antimony tetroxide (Sb2 O4 ) on BiVO4 . A H2 O2 FE of 26% at 1.54 V vs RHE is obtained by Sb2 O4 /BiVO4 and 49 ppm of H2 O2 is accumulated after a 135 min chronoamperometry. Similar to that in KHCO3 pure water solution, infrared spectroscopy and electrochemical analysis confirm that HCO3 - plays a surface-mediating role in the formation of H2 O2 in KHCO3 saline water solution. The presence of HCO3 - in the electrolyte is able to not only increase the photocurrent density but also effectively inhibit the chlorine evolution reaction.- Published
- 2024
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6. Modeling of Nanomaterials for Supercapacitors: Beyond Carbon Electrodes.
- Author
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Bi S, Knijff L, Lian X, van Hees A, Zhang C, and Salanne M
- Abstract
Capacitive storage devices allow for fast charge and discharge cycles, making them the perfect complements to batteries for high power applications. Many materials display interesting capacitive properties when they are put in contact with ionic solutions despite their very different structures and (surface) reactivity. Among them, nanocarbons are the most important for practical applications, but many nanomaterials have recently emerged, such as conductive metal-organic frameworks, 2D materials, and a wide variety of metal oxides. These heterogeneous and complex electrode materials are difficult to model with conventional approaches. However, the development of computational methods, the incorporation of machine learning techniques, and the increasing power in high performance computing now allow us to tackle these types of systems. In this Review, we summarize the current efforts in this direction. We show that depending on the nature of the materials and of the charging mechanisms, different methods, or combinations of them, can provide desirable atomic-scale insight on the interactions at play. We mainly focus on two important aspects: (i) the study of ion adsorption in complex nanoporous materials, which require the extension of constant potential molecular dynamics to multicomponent systems, and (ii) the characterization of Faradaic processes in pseudocapacitors, that involves the use of electronic structure-based methods. We also discuss how recently developed simulation methods will allow bridges to be made between double-layer capacitors and pseudocapacitors for future high power electricity storage devices.
- Published
- 2024
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7. Photocycloaddition of Zero-Dimensional Metal Halide Hybrids with Reversible Photochromism.
- Author
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Liu X, Chen C, Xiao Y, Li X, Xu K, Lian X, Zhang JZ, and Luo B
- Abstract
In this work, two zero-dimensional (0D) metal halide hybrids L
2 ZnBr4 [ 1 , L = ( E )-4-(2-(1 H -pyrrol-3-yl)vinyl)-1-methylpyridin-1-ium] and L6 Pb3 Br12 ( 2 ) were prepared, which demonstrated photochromism and photoinduced cracking. Upon irradiation at 450 nm, a single crystal-to-single crystal transformation occurred as a result of the [2 + 2] photocycloaddition of L . Interestingly, compared to the complete photocycloaddition of L in 1 , only two-thirds of L monomers could be photodimerized in 2 because of the difference in L orientation. 1 shows reversible photochromic behavior including rapid response time, few cracks, high conversion rate, and good reaction reversibility, while 2 exhibits no significant color change but distinct photoinduced cracking because of the large local lattice strain induced by inhomogeneous and anisotropic deformation. Moreover, the photocycloaddition of L results in the distinct shift of photoluminescence of 1 and 2 , attributed to the variation in conjugation of π electrons and distortion of metal halide clusters. As a proof-of-concept, reversible optical writing is demonstrated for 1 . These findings provide new insights into the design of stimuli-responsive multifunctional materials.- Published
- 2024
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8. Tuning MXene Properties through Cu Intercalation: Coupled Guest/Host Redox and Pseudocapacitance.
- Author
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Wee S, Lian X, Vorobyeva E, Tayal A, Roddatis V, La Mattina F, Gomez Vazquez D, Shpigel N, Salanne M, and Lukatskaya MR
- Abstract
MXenes are 2D transition metal carbides, nitrides, and/or carbonitrides that can be intercalated with cations through chemical or electrochemical pathways. While the insertion of alkali and alkaline earth cations into Ti
3 C2 Tx MXenes is well studied, understanding of the intercalation of redox-active transition metal ions into MXenes and its impact on their electronic and electrochemical properties is lacking. In this work, we investigate the intercalation of Cu ions into Ti3 C2 Tx MXene and its effect on its electronic and electrochemical properties. Using X-ray absorption spectroscopy (XAS) and ab initio molecular dynamics (AIMD), we observe an unusual phenomenon whereby Cu2+ ions undergo partial reduction upon intercalation from the solution into the MXene. Furthermore, using in situ XAS, we reveal changes in the oxidation states of intercalated Cu ions and Ti atoms during charging. We show that the pseudocapacitive response of Cu-MXene originates from the redox of both the Cu intercalant and Ti3 C2 Tx host. Despite highly reducing potentials, Cu ions inside the MXene show an excellent stability against full reduction upon charging. Our findings demonstrate how electronic coupling between Cu ions and Ti3 C2 Tx modifies electrochemical and electronic properties of the latter, providing the framework for the rational design and utilization of transition metal intercalants for tuning the properties of MXenes for various electrochemical systems.- Published
- 2024
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9. Control of Zeolite Local Polarity toward Efficient Xenon/Krypton Separation.
- Author
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Liu S, Lian X, Yue B, Xu S, Wu G, Chai Y, Zhang Y, and Li L
- Abstract
The inherent inertness and striking physicochemical similarities of krypton and xenon pose significant challenges to their separation. Reported herein is the efficient xenon capture and xenon/krypton adsorptive separation by transition metal-free zeolites under ambient conditions. The polarized environment of zeolite, denoted as local polarity, can be tuned by changing the topology, framework composition, and counter-cations, which in turn correlates with the guest-host interaction and separation performance. Chabazite zeolite with a framework Si/Al ratio of 2.5 and Ca
2+ as the counter-cations, namely, Ca-CHA-2.5, is developed as a state-of-the-art zeolite adsorbent, showing remarkable performance, i.e. , high dynamic xenon uptake, high xenon/krypton separation selectivity, and good recyclability, in the adsorptive separation of the xenon/krypton mixture. Grand Canonical Monte Carlo simulation reveals that extraframework Ca2+ cations act as the primary binding sites for xenon and can stabilize xenon molecules together with the chabazite framework, whereas krypton molecules are stabilized by weak guest-host interaction with the zeolite framework.- Published
- 2024
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10. Revealing the Mechanism of Ink Flaking from Surfaces of Palm Leaves ( Corypha umbraculifera ).
- Author
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Lian X, Yu C, Han W, Li B, Zhang M, Wang Y, and Li L
- Abstract
Palm leaves are the primary literary support in South and Southeast Asia before the widespread use of paper. However, palm leaf manuscripts face the threat of information loss due to the persistent issue of ink flaking during long-term preservation. Herein, we focus on studying the botanical structure, surface properties, and surface composition of palm leaves to gain an insightful understanding of the mechanism of ink flaking. According to the surface energy analysis, the surface of palm leaves is dominated by the dispersive component due to the presence of hydrophobic substances, resulting in the weak interaction between the handwriting and palm leaves. Moreover, the accumulation of silicon on palm leaves creates a "cuticle-silicon double layer", leading to a dense structure that hinders deep ink absorption. These two main reasons are considered to cause the ink flaking easily, which is further proven by the ink flaking test with the simulated palm leaf manuscripts. To the best of our knowledge, this is the first in-depth technical study on the adhesion performance of handwriting on plant leaves. This work also provides a theoretical basis for the study of the deterioration, adhesive repair, enhancement of flexibility, handwriting reinforcement, and beyond, which contributes to the conservation of precious palm leaf manuscripts.
- Published
- 2024
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11. Nanosphere Chain Model of Magnetic Fluid and Its Dynamic Performance.
- Author
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Wang K, Liu B, Lian X, Xuan S, Deng H, and Gong X
- Abstract
The magnetorheological effect is a critically important mechanical property of magnetic fluids. Accurately capturing the macroscopic properties of magnetorheological fluids with elongated particle forms, such as nanosphere chains, remains a challenging task, particularly due to the complexities arising from particle asymmetry. Traditional particle dynamics primarily utilize spherical particles as computational units, but this approach can lead to significant inaccuracies, especially when analyzing nonspherical magnetorheological fluids, due to the neglect of particle asymmetry. In this work, an advanced particle dynamics model has been developed by integrating the rotation and collision of these asymmetric particles, specifically tailored for the configuration of nanosphere chains. This model exhibits a significant reduction in error by a factor of 3.883, compared to conventional particle models. The results demonstrate that alterations in the geometric characteristics of magnetic nanosphere chains can cause changes in mesoscopic structures and magnetic potential energy, thereby influencing the mechanical properties at the macroscopic level. This work has developed an accurate mesoscopic simulation method for calculating chain-type magnetorheological fluids, establishing a connection between mesoscopic structures and macroscopic properties, and unveiling the tremendous potential for accelerating the design of next-generation magnetic fluids using this approach.
- Published
- 2024
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12. Mitigation Measures Could Aggravate Unbalanced Nitrogen and Phosphorus Emissions from Land-Use Activities.
- Author
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Tian Y, Hu Y, Su M, Jia Q, Lian X, and Jiao L
- Subjects
- Ecosystem, Agriculture, Food, China, Nitrogen analysis, Phosphorus analysis
- Abstract
Socioeconomic factors and mitigation potentials are essential drivers of the dynamics of nutrient emissions, yet these drivers are rarely examined at broad spatiotemporal scales. Here, we combine material flow analysis and geospatial analysis to examine the past and future changes of nitrogen and phosphorus emissions in China. Results show that anthropogenic nitrogen and phosphorus emissions increased by 17% and 32% during 2000-2019, respectively. Meanwhile, many regions witnessed decreasing nitrogen emissions but rising phosphorus discharged to waterbody, leading to a 20% decrease in the nitrogen/phosphorus ratio. In addition to many prominent factors like fertilizer use, the increasing impervious land area around cities is a notable factor driving the emissions, indicating the urgency to limit building expansion, especially in North China Plain and other less-developed regions. Improving land-use efficiency and consuming behaviors could reduce nitrogen and phosphorus emissions by 65-77% in 2030, but the nitrogen/phosphorus ratio will increase unintendedly due to larger reduction potentials for phosphorus, which may deteriorate the aquatic ecosystem. We highlight that nitrogen and phosphorus emissions should be reduced with coordinated but differentiated measures by prioritizing nitrogen reduction through cropland and food-system management.
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- 2024
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13. Acetate Ions Facilitated Immobilization of Highly Dispersed Transition Metal Oxide Nanoclusters in Mesoporous Silica.
- Author
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Wang N, Li X, Lian X, Zhuang Q, Wang J, Li J, Qian H, Miao K, Wang Y, Luo X, and Feng G
- Abstract
The immobilization of tiny active species within inert mesoporous silica imparts a range of functions, enhancing their applicability. A significant obstacle is the spontaneous migration and aggregation of these species within the mesopores, which threaten their uniform distribution. To address this, we propose a postmodification method that involves grafting transition metal oxide nanoclusters into silica mesopores via interfacial condensation, catalyzed by acetate ions. Specifically, CuO nanoclusters, in the form of oligomeric [O
1- x -Cu2 -(OH)2 x ]n 2+ , have a strong interaction with the silica framework. This interaction inhibits their growth and prevents mesopore blockage. Theoretical calculation results reveal that the acetate ion promotes proton transfer among various hydroxy species, lowering the free energy and thereby facilitating the formation of Cu-O-Si bonds. This technique has also been successfully applied to the encapsulation of four other types of transition metal oxide nanoclusters. Our encapsulation strategy effectively addresses the challenge of dispersing transition metal oxides in mesoporous silica, offering a straightforward and widely applicable method for enhancing the functionality of mesoporous materials.- Published
- 2024
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14. Multicolor Fluorescent Inks Based on Lanthanide Hybrid Organogels for Anticounterfeiting and Logic Circuit Design.
- Author
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Lian X, Chang R, Huang G, Peng Y, Wang K, Zhang J, Yao B, and Niu H
- Abstract
With the rapid development of information technology, the encrypted storage of information is becoming increasingly important for human life. The luminescent materials with a color-changed response under physical or chemical stimuli are crucial for information coding and anticounterfeiting. However, traditional fluorescent materials usually face problems such as a lack of tunable fluorescence, insufficient surface-adaptive adhesion, and strict synthesis conditions, hindering their practical applications. Herein, a series of luminescent lanthanide hybrid organogels (Ln-MOGs) were rapidly synthesized using a simple method at room temperature through the coordination between lanthanide ions and 2,6-pyridinedicarboxylic acid and 5-aminoisophthalic acid. And the multicolor fluorescent inks were also prepared based on the Ln-MOG and hyaluronic acid, with the advantages of being easy to write, color-adjustable, and water-responsive discoloration, which has been applied to paper-based anticounterfeiting technology. Inspired by the responsiveness of the fluorescent inks to water, we designed a logic system that can realize single-input logic operations (NOT and PASS1) and double-input logic operations (NAND, AND, OR, NOR, XOR). The encryption of a binary code can be actualized utilizing different luminescent response modes based on the logic circuit system. By adjusting the energy sensitization and luminescence mechanism of lanthanide ions in the gel structure, the information reading and writing ability of the fluorescent inks were verified, which has great potential in the field of multicolor pattern anticounterfeiting and information encryption.
- Published
- 2024
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15. ProtWave-VAE: Integrating Autoregressive Sampling with Latent-Based Inference for Data-Driven Protein Design.
- Author
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Praljak N, Lian X, Ranganathan R, and Ferguson AL
- Subjects
- Phylogeny, Mutation, Amino Acid Sequence, Proteins, Genetic Techniques
- Abstract
Deep generative models (DGMs) have shown great success in the understanding and data-driven design of proteins. Variational autoencoders (VAEs) are a popular DGM approach that can learn the correlated patterns of amino acid mutations within a multiple sequence alignment (MSA) of protein sequences and distill this information into a low-dimensional latent space to expose phylogenetic and functional relationships and guide generative protein design. Autoregressive (AR) models are another popular DGM approach that typically lacks a low-dimensional latent embedding but does not require training sequences to be aligned into an MSA and enable the design of variable length proteins. In this work, we propose ProtWave-VAE as a novel and lightweight DGM, employing an information maximizing VAE with a dilated convolution encoder and an autoregressive WaveNet decoder. This architecture blends the strengths of the VAE and AR paradigms in enabling training over unaligned sequence data and the conditional generative design of variable length sequences from an interpretable, low-dimensional learned latent space. We evaluated the model's ability to infer patterns and design rules within alignment-free homologous protein family sequences and to design novel synthetic proteins in four diverse protein families. We show that our model can infer meaningful functional and phylogenetic embeddings within latent spaces and make highly accurate predictions within semisupervised downstream fitness prediction tasks. In an application to the C-terminal SH3 domain in the Sho1 transmembrane osmosensing receptor in baker's yeast, we subject ProtWave-VAE-designed sequences to experimental gene synthesis and select-seq assays for the osmosensing function to show that the model enables synthetic protein design, conditional C-terminus diversification, and engineering of the osmosensing function into SH3 paralogues.
- Published
- 2023
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16. Fast Interfacial Polymerization for Stabilizing Emulsion Droplets with Polymer Films beyond Emulsifiers.
- Author
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Lian X and Wang Y
- Abstract
Stabilizing emulsion droplets with amphiphilic emulsifiers are the current prevailing method, but the extensive use of such amphiphilic substances has caused widespread concerns. In this Perspective, three traditional methods for the stabilization of emulsion droplets according to the type of emulsifiers used are outlined, and the emphasis is placed on the mechanism of steric hindrance for emulsion stabilization. Then, we provide a concise introduction and discussion of the fast interfacial polymerization method as a new strategy for preparing stable emulsifier-free emulsion droplets with a polymer film, including its research background, current progress, and possible development directions. It is anticipated that this paper will promote the development of emulsifier-free emulsion production via fast interfacial polymerization and other related methods.
- Published
- 2023
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17. Uniformly Hybrid Surface Containing Adjustable Hydrophobic/Hydrophilic Components Obtained by Programmed Strain for Synergistic Anti-Icing.
- Author
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Wang W, Chen Z, Lian X, Yang Z, Fu B, and Wang Y
- Abstract
Sufficient efforts have been put into the design of anti-icing materials to eliminate the icing hazard. Among the currently approved anti-icing concepts, hydrophilic/hydrophobic hybrid anti-icing materials inspired by antifreeze proteins show excellent properties in inhibiting ice nucleation, inhibiting ice crystal growth, and reducing ice adhesion. However, it is still a great challenge to accurately regulate the hydrophilic and hydrophobic hybrid components of the coating surface to clarify the synergistic mechanism. This work proposes a strain-manipulated surface modification strategy, and an anti-icing coating with adjustable hydrophilic/hydrophobic hybrid components prepared by combining chemical vapor deposition and siloxane chemistry is obtained. According to the ice resistance experiment at -15 °C, the performance of anti-icing is closely related to the proportion of hydrophilic and hydrophobic hybrids. The icing delay time and ice adhesion strength of the material with the optimal hydrophilic/hydrophobic components are 280 s and 18.6 kPa, respectively. These unique properties can be attributed to the synergistic effect of hydrophilic and hydrophobic structures on the regulation of interfacial water.
- Published
- 2023
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18. Association of Short-Term Co-Exposure to Particulate Matter and Ozone with Mortality Risk.
- Author
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Guo J, Zhou J, Han R, Wang Y, Lian X, Tang Z, Ye J, He X, Yu H, Huang S, and Li J
- Subjects
- Particulate Matter analysis, China epidemiology, Environmental Exposure analysis, Mortality, Ozone analysis, Air Pollutants analysis, Air Pollution analysis
- Abstract
A complex regional air pollution problem dominated by particulate matter (PM) and ozone (O
3 ) needs drastic attention since the levels of O3 and PM are not decreasing in many parts of the world. Limited evidence is currently available regarding the association between co-exposure to PM and O3 and mortality. A multicounty time-series study was used to investigate the associations of short-term exposure to PM1 , PM2.5 , PM10 , and O3 with daily mortality from different causes, which was based on data obtained from the Mortality Surveillance System managed by the Jiangsu Province Center for Disease Control and Prevention of China and analyzed via overdispersed generalized additive models with random-effects meta-analysis. We investigated the interactions of PM and O3 on daily mortality and calculated the mortality fractions attributable to PM and O3 . Our results showed that PM1 is more strongly associated with daily mortality than PM2.5 , PM10 , and O3 , and percent increases in daily all-cause nonaccidental, cardiovascular, and respiratory mortality were 1.37% (95% confidence interval (CI), 1.22-1.52%), 1.44% (95% CI, 1.25-1.63%), and 1.63% (95% CI, 1.25-2.01%), respectively, for a 10 μg/m3 increase in the 2 day average PM1 concentration. We found multiplicative and additive interactions of short-term co-exposure to PM and O3 on daily mortality. The risk of mortality was greatest among those with higher levels of exposure to both PM (especially PM1 ) and O3 . Moreover, excess total and cardiovascular mortality due to PM1 exposure is highest in populations with higher O3 exposure levels. Our results highlight the importance of the collaborative governance of PM and O3 , providing a scientific foundation for pertinent standards and regulatory interventions.- Published
- 2023
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19. STAMP-Based Digital CRISPR-Cas13a for Amplification-Free Quantification of HIV-1 Plasma Viral Loads.
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Nouri R, Jiang Y, Politza AJ, Liu T, Greene WH, Zhu Y, Nunez JJ, Lian X, and Guan W
- Subjects
- Humans, Viral Load methods, RNA, Viral genetics, RNA, Viral analysis, Sensitivity and Specificity, HIV-1 genetics, HIV Infections diagnosis
- Abstract
Quantification of HIV RNA in plasma is critical for identifying the disease progression and monitoring the effectiveness of antiretroviral therapy. While RT-qPCR has been the gold standard for HIV viral load quantification, digital assays could provide an alternative calibration-free absolute quantification method. Here, we reported a S elf-digitization T hrough A utomated M embrane-based P artitioning (STAMP) method to digitalize the CRISPR-Cas13 assay (dCRISPR) for amplification-free and absolute quantification of HIV-1 viral RNAs. The HIV-1 Cas13 assay was designed, validated, and optimized. We evaluated the analytical performances with synthetic RNAs. With a membrane that partitions ∼100 nL of reaction mixture (effectively containing 10 nL of input RNA sample), we showed that RNA samples spanning 4 orders of dynamic range between 1 fM (∼6 RNAs) to 10 pM (∼60k RNAs) could be quantified as fast as 30 min. We also examined the end-to-end performance from RNA extraction to STAMP-dCRISPR quantification using 140 μL of both spiked and clinical plasma samples. We demonstrated that the device has a detection limit of approximately 2000 copies/mL and can resolve a viral load change of 3571 copies/mL (equivalent to 3 RNAs in a single membrane) with 90% confidence. Finally, we evaluated the device using 140 μL of 20 patient plasma samples (10 positives and 10 negatives) and benchmarked the performance with RT-PCR. The STAMP-dCRISPR results agree very well with RT-PCR for all negative and high positive samples with C
t < 32. However, the STAMP-dCRISPR is limited in detecting low positive samples with Ct > 32 due to the subsampling errors. Our results demonstrated a digital Cas13 platform that could offer an accessible amplification-free quantification of viral RNAs. By further addressing the subsampling issue with approaches such as preconcentration, this platform could be further exploited for quantitatively determining viral load for an array of infectious diseases.- Published
- 2023
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20. Direct Synthesis of Aliphatic Polyesters with Pendant Hydroxyl Groups from Bio-Renewable Monomers: A Reactive Precursor for Functionalized Biomaterials.
- Author
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Shan P, Lian X, Lu W, Yin X, Lu Y, Zhang M, Wen X, Xin G, Li Z, and Li Z
- Subjects
- Polyethylene Glycols, Hydroxyl Radical, Polyesters, Biocompatible Materials
- Abstract
Introducing desired functionalities into biomaterials is an effective way to obtain functionalized biomaterials. A versatile platform with the possibility of postsynthesis functionalization is highly desired but challenging in biomedical engineering. In this work, linear aliphatic polyesters with pendant hydroxyl (PEOH) groups were directly synthesized using renewable malic acid/tartaric acid as raw materials under mild conditions through the polyesterification reaction promoted by 1,1,3,3-tetramethylguanidine (TMG). The hydroxyl groups on PEOH provide an active stepping stone for the fabrication of demanded functionalized polyesters. We demonstrated the possibility of the PEOH as a reactive precursor for functional group transformation, coupling of bioactive molecules, and formation of crosslinking networks. Moreover, a theranostic nanoplatform (mPEG-b-(P7-asp&TPV)-b-mPEG NPs) was synthesized using PEOH as a reactive stepping stone by the programmable combination of the above functionalization methods. Overall, these hydroxyl-containing polyesters have great potential in biological applications.
- Published
- 2023
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21. "Urban Respiration" Revealed by Atmospheric O 2 Measurements in an Industrial Metropolis.
- Author
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Liu X, Huang J, Wang L, Lian X, Li C, Ding L, Wei Y, Chen S, Wang Y, Li S, and Shi J
- Subjects
- Humans, Environmental Monitoring, China, Gases, Particulate Matter analysis, Air Pollutants analysis, Air Pollution analysis, Environmental Pollutants
- Abstract
Urban regions, which "inhale" O
2 from the air and "exhale" CO2 and atmospheric pollutants, including harmful gases and fine particles, are the largest sinks of atmospheric O2 , yet long-term O2 measurements in urban regions are currently lacking. In this study, we report continuous measurements of atmospheric O2 in downtown Lanzhou, an industrial metropolis in northwestern China. We found declines in atmospheric O2 associated with deteriorated air quality and robust anticorrelations between O2 and gaseous oxides. By combining O2 and pollutants measurements with a Lagrangian atmospheric transport model, we quantitatively break down "urban respiration" (ΔO2URB ) into human respiration (ΔO2RES ) and fossil fuel combustion (ΔO2FF ). We found increased ΔO2FF contribution (from 66.92% to 72.50%) and decreased ΔO2RES contribution (from 33.08 to 27.50%) as O2 declines and pollutants accumulate. Further attribution of ΔO2FF reveals intracity transport of atmospheric pollutants from industrial sectors and suggests transportation sectors as the major O2 sink in downtown Lanzhou. The varying relationships between O2 and pollutants under different conditions unfold the dynamics of urban respiration and provide insights into the O2 and energy consumption, pollutant emission, and intracity atmospheric transport processes.- Published
- 2023
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22. Nanocatalytic Hydrogel with Rapid Photodisinfection and Robust Adhesion for Fortified Cutaneous Regeneration.
- Author
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Su Y, Zhang X, Wei Y, Gu Y, Xu H, Liao Z, Zhao L, Du J, Hu Y, Lian X, Chen W, Deng Y, and Huang D
- Subjects
- Skin, Anti-Bacterial Agents pharmacology, Hydrogels pharmacology, Wound Healing
- Abstract
Chronic inflammation caused by invasive bacterial infections severely interferes with the normal healing process of skin regeneration. Hypoxia of the infection microenvironment (IME) seriously affects the antibacterial effect of photodynamic therapy in phototherapy. To address this serious issue, a nanocatalytic hydrogel with an enhanced phototherapy effect consisting of a hydrogel polyvinyl alcohol (PVA) scaffold, MXene/CuS bio-heterojunction, and polydopamine (PDA) for photothermal antibacterial effects and promoting skin regeneration is designed. The MXene/CuS bio-heterojunction has a benign photothermal effect. Singlet oxygen (
1 O2 ) and hydroxyl radicals (·OH) were generated under near-infrared light, which made the hydrogel system have good antioxidant and antibacterial properties. The addition of PDA further improves the biocompatibility and endows the nanocatalytic hydrogel with adhesion. Additionally, in vivo assays display that the nanocatalytic hydrogel has good skin regeneration ability, including ability to kill bacteria, and promotes capillary angiogenesis and collagen deposition. This work proposes an approach for nanocatalyzed hydrogels with an activated IME response to treat wound infections by enhancing the phototherapeutic effects.- Published
- 2023
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23. Calcium Phosphate Bone Cements Incorporated with Black Phosphorus Nanosheets Enhanced Osteogenesis.
- Author
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Ma S, Wei Y, Sun R, Xu H, Liu X, Wang Y, Liang Z, Hu Y, Lian X, Ma X, and Huang D
- Subjects
- Calcium Phosphates pharmacology, Bone Regeneration, Osteogenesis, Bone Cements pharmacology
- Abstract
For decades, calcium phosphate bone cements (CPCs) showed impressive advantages for their good biocompatibility, injectability, and osteoconductivity in the bone repair field. However, it is still difficult to prepare CPCs with outstanding antibacterial and self-curing properties, sufficient phosphorus release, and osteoinductivity for clinical application. Herein, we used partially crystallized calcium phosphate and dicalcium phosphate anhydrate particles incorporated with black phosphorous nanosheets to prepare calcium phosphate bone cements (CPCs). The curing time, compressive strength, photothermal properties, and degradation performance of BP/CPC were investigated. In addition, the cytocompatibility and osteoinductivity of BP/CPC were evaluated by cell adhesion, cytotoxicity, alkaline phosphatase detection, alizarin red staining, and western blot assay. The results indicated that BP/CPC showed adjustable curing time, good cytocompatibility, outstanding photothermal properties, and osteoinductivity, suggesting their potential application for bone regeneration.
- Published
- 2023
- Full Text
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24. Curved π-Conjugated Helical Carbon Frameworks: Syntheses, Structural Analyses, and Properties.
- Author
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Zhang J, Chen H, Qin X, Duan H, Zhang X, Kong X, Lian X, Ding H, Yi H, Tan Y, Xiao D, Du P, and Xu P
- Abstract
Two enantiomers with helical carbon frameworks ( M - HCFa and P - HCFa ) and their conformational isomers ( M - HCFb and P - HCFb ) have been synthesized and characterized. The single-crystal analysis revealed the novel structures in which three propeller blades spiro-fused on two central benzene rings. The optical properties were further investigated, and stable bipolar electrochemiluminescence emissions were discovered for the first time existing in helical carbon frameworks, which provide new insights into the future development of high-performance molecular luminescent devices.
- Published
- 2022
- Full Text
- View/download PDF
25. Weakening Ligand-Liquid Affinity to Suppress the Desorption of Surface-Passivated Ligands from Perovskite Nanocrystals.
- Author
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Zheng L, Li X, Lian X, Xu R, Liu X, Xuan T, Zeng R, Ni WX, and Luo B
- Subjects
- Ligands, Amines, Glycyrrhizic Acid, Nanoparticles, Quantum Dots
- Abstract
The interfacial migration of surface-bound ligands highly affects the colloidal stability and optical quality of semiconductor nanocrystals, of which the underlying mechanism is not fully understood. Herein, colloidal CsPbBr
3 perovskite nanocrystals (PNCs) with fragile dynamic equilibrium of ligands are taken as the examples to reveal the important role of balancing ligand-solid/solvent affinity in suppressing the desorption of ligands. As a micellar surfactant, glycyrrhizic acid (GA) with bulky hydrophobic and hydrophilic groups exhibits a relatively smaller diffusion coefficient (∼440 μm2 /s in methanol) and weaker ligand-liquid affinity than that of conventional alkyl amine and carboxy ligands. Consequently, hydrophilic GA-passivated PNCs (PNCs-GA) show excellent colloidal stability in various polar solvents with dielectric constant ranging from 2.2 to 32.6 and efficient photoluminescence with a quantum yield of 85.3%. Due to the suppressed desorption of GA, the morphological and optical properties of PNCs-GA are well maintained after five rounds purification and two months long-term storage. At last, hydrophilic PNCs-GA are successfully patterned through inkjet- and screen-printing technology. These findings offer deep insights into the interfacial chemistry of colloidal NCs and provide a universal strategy for preparing high-quality hydrophilic PNCs.- Published
- 2022
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- View/download PDF
26. Experimental Study of Dual-Fuel Diesel/Natural Gas High-Pressure Injection.
- Author
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Lei Y, Wu Y, Qiu T, Zhou D, Lian X, and Jin W
- Abstract
Dual-fuel diesel/natural gas direct-injection engine is promising and highly attractive due to its low-carbon emission and high thermal efficiency, and both high-pressure diesel and natural gas injections are critical for air-fuel mixing. This study presents an optical experimental investigation on the high-pressure dual-fuel diesel/methane injection process based on a constant-volume vessel test rig. The results show that the diesel penetration process of the dual-fuel injection experiences two stages: Stage I, the diesel tip penetration S
diesel , the diesel spray area Adiesel , and the diesel spray perimeter Cdiesel of the dual-fuel injection are smaller than those of the single diesel injection. Stage II, both the diesel and methane continue to penetrate forward, and Sdiesel , Adiesel , and Cdiesel of the dual-fuel injection become larger than those of the single diesel injection do. The diesel injection pressure causes effect on the dual-fuel spray penetration. The diesel injection pressure directly causes linear influence on the two-stage dual-fuel injection characteristic. As the diesel injection pressure increases, the diesel spray meets the methane jet advancer and the cross point occurs linearly earlier. Furthermore, the dual-fuel injection is asymmetric and the methane gas jet enhances this asymmetry so that the spray cone shifts to the side of the methane gas jet., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)- Published
- 2022
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27. Enhancing Chromatographic Performance of Immobilized Angiotensin II Type 1 Receptor by Strain-Promoted Alkyne Azide Cycloaddition through Genetically Encoded Unnatural Amino Acid.
- Author
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Zuo H, Li T, Zhang D, Ma J, Zhang Z, Ou Y, Lian X, Yin J, Li Q, and Zhao X
- Subjects
- Cycloaddition Reaction, Receptor, Angiotensin, Type 1 genetics, Amino Acids, Proteins, Azides chemistry, Alkynes chemistry
- Abstract
During integration to the solid surface, the effects of tags introduced for bioorthogonal reactions on protein activity have received far less investigation. This represents the major challenge of improving the performance of the immobilized protein-based assays. Herein, the relationship between the fusion tags and their reaction efficiency in mediating the assay performance was realized by determining the chromatographic performance using genetically encoded azide-alkyne cycloaddition, and Halo- and SNAP-tagged bioorthogonal reactions for synthesizing immobilized angiotensin II type 1 receptor (AT
1 R). We demonstrated that immobilization with the incorporation of unnatural amino acid in the receptor minimizes the peak tailings and broadenings of irbesartan, fimasartan, losartan, and tasosartan, while attachment via large tags (SNAP and Halo) leads to serious asymmetry peaks. Upon the first immobilization, the association constants of the four drugs to AT1 R appeared to be 1 order of magnitude greater than the other two attachments. Such enhancement is likely reasoned by the improved association rate constants and the relatively identical dissociation rates due to the small tag. While demonstrating improved chromatographic performance, the immobilized AT1 R prepared by the genetically encoded azide-alkyne reaction was applied in analyzing Uncaria Schreber nom. cons. extract, which identified hynchophylline as a specific ligand binding to the receptor. As immobilized proteins move toward diverse assays, our findings provide an unprecedented insight into the relation between fusion tags and their reaction efficiency in mediating the assay performance, which is thus dedicated to the creation of a protein-functionalized surface for precisely determining the drug-protein interaction and discovering the specific partner of the protein.- Published
- 2022
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28. Iodine-Oxidized Diene-Based Rubbers as Anti-icing and Deicing Polymer Coatings.
- Author
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Fu B, Ma Y, Li R, Lian X, Liao S, and Wang Y
- Abstract
In an effort to prevent or minimize icing hazards, techniques and materials for icing inhibition and deicing have always been highly favored throughout human history. This work discovers the integrated anti-icing and deicing effects of poly(styrene- b -butadiene- b -styrene) triblock rubber (SBS) after its easy oxidation in iodine vapor. Iodine oxidation happens on the block of polybutadiene, featured by the conversion of SBS from hydrophobic to amphiphilic and the improved capability of photothermal conversion. The oxidized SBS can serve as a polymer coating, which possesses intriguing abilities to delay the kinetics of icing on its surface and repel the ice under light illumination. According to characterizations of surface chemistry and mechanical performance, iodine oxidation is assumed to involve the processes of iodine coordination to unsaturated bonds, the formation of radical cations as a result of the redox reaction between iodine and unsaturated carbon-carbon bonds, improved light absorption owing to the formation of polyiodide anions, and intermolecular coupling of radical cations. The appearance of polar moieties/species within the oxidized SBS is attributed to the delayed ice nucleation. The significant photothermal capacity in visible and near-infrared windows enables the iodine-oxidized SBS coating to remove the adhered ice by melting under light illumination when the icing process is inevitable, even at an extremely low temperature (-25 °C).
- Published
- 2022
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29. Biodegradable and Light-Responsive Polymeric Nanoparticles for Environmentally Safe Herbicide Delivery.
- Author
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Shan P, Lu Y, Lu W, Yin X, Liu H, Li D, Lian X, Wang W, Li Z, and Li Z
- Subjects
- 2,4-Dichlorophenoxyacetic Acid, Delayed-Action Preparations pharmacology, Drug Carriers, Drug Delivery Systems, Humans, Polymers, Herbicides pharmacology, Nanoparticles
- Abstract
The low utilization efficiency of pesticides exerts an adverse impact on the environment and human health. Polymer-related controlled-release nanosized pesticide systems provide a promising and efficient way to overcome the problem. In this work, a biodegradable and light-responsive amphiphilic polymer was synthesized via 1,1,3,3-tetramethylguanidine-promoted polyesterification under mild conditions (low temperature, no vacuum, and no inert gas protection). We used this polymer to fabricate a light-triggered controlled-release nanosized pesticide system. The herbicide, 2,4-dichlorophenoxyacetic acid (2,4-D), was selected as a model drug to show its potential as a controlled-release pesticide system. It was found that the 2,4-D-loaded polymeric nanoparticles were stable without the treatment of UV, while the release rate of 2,4-D from the nanoparticles gradually increased after treatment with UV light. Pot trial showed that the 2,4-D-loaded polymer nanoparticles showed a good herbicidal effect. Finally, toxicity studies suggested that the polymer can reduce toxicity to nontarget organisms.
- Published
- 2022
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30. Unraveling Catalytic Reaction Mechanism by In Situ Near Ambient Pressure X-ray Photoelectron Spectroscopy.
- Author
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Lian X, Gao J, Ding Y, Liu Y, and Chen W
- Abstract
Probing surface chemistry during reactions closer to realistic conditions is crucial for the understanding of mechanisms in heterogeneous catalysis. Near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) is one of the state-of-the-art surface-sensitive techniques used to characterize catalyst surfaces in gas phases. This Perspective begins with a brief overview of the development of the NAP-XPS technique and its representative applications in identifying the active sites at a molecular level. Next, recent in situ NAP-XPS investigations of several model catalysts in the CO
2 hydrogenation reaction are mainly discussed. Finally, we highlight the major challenges facing NAP-XPS and future improvements to facilities for probing intermediates with higher resolutions under real ambient pressure reactions in heterogeneous catalysis.- Published
- 2022
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31. Temporal Expression of Transcription Factor ID2 Improves Natural Killer Cell Differentiation from Human Pluripotent Stem Cells.
- Author
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Jung J, Chang Y, Jin G, Lian X, and Bao X
- Subjects
- Cell Differentiation genetics, Humans, Immunity, Innate, Inhibitor of Differentiation Protein 2 genetics, Inhibitor of Differentiation Protein 2 metabolism, Killer Cells, Natural metabolism, Pluripotent Stem Cells metabolism, Transcription Factors metabolism
- Abstract
Natural killer (NK) cells are one type of innate lymphoid cells, and NK cell-based immunotherapy serves as a potentially curative therapy for cancers. However, the lack of reliable resources for a large amount of NK cells required for clinical infusion has limited the broader application of NK cells in targeted immunotherapy. Substantial effort has thus been made to generate NK-like cells from human pluripotent stem cells (hPSCs), but detailed molecular mechanisms regulating NK cell differentiation remain elusive, preventing us from developing robust strategies for NK cell production. Here, we genetically engineered hPSCs with inducible overexpression of transcription factors NFIL3 , ID2 , or SPI1 via CRISPR/Cas9-mediated gene knock-in and investigated their temporal roles during NK cell differentiation. Our results demonstrated ID2 overexpression significantly promoted NK cell generation compared with NFIL3 and SPI1 overexpression under a chemically defined, feeder-free culture condition. The resulting ID2 hPSC-derived NK cells exhibited various mature NK-specific markers and displayed effective tumor-killing activities, comparable to NK cells derived from wildtype hPSCs. Our study provides a new platform for efficient NK cell production, serving as a realistic off-the-shelf cell source for targeted cancer immunotherapy.
- Published
- 2022
- Full Text
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32. Purification of MDI Isomers Using Dynamic Falling Film Melt Crystallization: Experiment and Molecular Simulation.
- Author
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Lian X, He P, Wang L, Cao Y, Huang K, Xu S, Chen J, and Li H
- Abstract
In this work, the isomer mixture of 4,4'-diphenylmethane diisocyanate (MDI) and 2,4'-MDI was separated and purified by dynamic falling film melt crystallization, and 99.3% purity and 50.8% yield of 4,4'-MDI could be obtained under optimized conditions. The separation mechanism was simulated by density functional theory (DFT) and molecular dynamics (MD) simulation. Results showed that compared with 2,4'-MDI, 4,4'-MDI molecules could form a more stable and symmetrical crystal structure due to their stronger charge density symmetry and electrostatic potential energy. Furthermore, the separation phenomenon and the formation of the crystal structure were observed according to the radial distribution function (RDF) and orientation correlation function obtained from MD simulation. Finally, the attachment energy (AE) model was used to observe and compare different crystal surfaces; it was proposed that the aggregation of 4,4'-MDI was attributed to the polar attraction between isocyanate groups according to the results of the orientation correlation function. It was also observed that compared with 2,4'-MDI, 4,4'-MDI molecules on the (110) crystal surface were easier to form crystal structures., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)
- Published
- 2022
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33. Epitaxial Growth of Ultraflat Bismuthene with Large Topological Band Inversion Enabled by Substrate-Orbital-Filtering Effect.
- Author
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Sun S, You JY, Duan S, Gou J, Luo YZ, Lin W, Lian X, Jin T, Liu J, Huang Y, Wang Y, Wee ATS, Feng YP, Shen L, Zhang JL, Chen J, and Chen W
- Abstract
Quantum spin Hall (QSH) systems hold promises of low-power-consuming spintronic devices, yet their practical applications are extremely impeded by the small energy gaps. Fabricating QSH materials with large gaps, especially under the guidance of design principles, is essential for both scientific research and practical applications. Here, we demonstrate that large on-site atomic spin-orbit coupling can be directly exploited via the intriguing substrate-orbital-filtering effect to generate large-gap QSH systems and experimentally realized on the epitaxially synthesized ultraflat bismuthene on Ag(111). Theoretical calculations reveal that the underlying substrate selectively filters Bi p
z orbitals away from the Fermi level, leading pxy orbitals with nonzero magnetic quantum numbers, resulting in large topological gap of ∼1 eV at the K point. The corresponding topological edge states are identified through scanning tunneling spectroscopy combined with density functional theory calculations. Our findings provide general strategies to design large-gap QSH systems and further explore their topology-related physics.- Published
- 2022
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34. Life Cycle Exposure to Environmentally Relevant Concentrations of Diphenyl Phosphate (DPhP) Inhibits Growth and Energy Metabolism of Zebrafish in a Sex-Specific Manner.
- Author
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Chen Q, Lian X, An J, Geng N, Zhang H, Challis JK, Luo Y, Liu Y, Su G, Xie Y, Li Y, Liu Z, Shen Y, Giesy JP, and Gong Y
- Subjects
- Animals, Biphenyl Compounds, Energy Metabolism, Female, Life Cycle Stages, Male, Phosphates, Flame Retardants, Zebrafish
- Abstract
Due to commercial uses and environmental degradation of aryl phosphate esters, diphenyl phosphate (DPhP) is frequently detected in environmental matrices and is thus of growing concern worldwide. However, information on potential adverse effects of chronic exposure to DPhP at environmentally realistic concentrations was lacking. Here, we investigated the effects of life cycle exposure to DPhP on zebrafish at environmentally relevant concentrations of 0.8, 3.9, or 35.6 μg/L and employed a dual-omics approach (metabolomics and transcriptomics) to characterize potential modes of action. Exposure to DPhP at 35.6 μg/L for 120 days resulted in significant reductions in body mass and length of male zebrafish, but did not cause those same effects to females. Predominant toxicological mechanisms, including inhibition of oxidative phosphorylation, down-regulation of fatty acid oxidation, and up-regulation of phosphatidylcholine degradation, were revealed by integrated dual-omics analysis and successfully linked to adverse outcomes. Activity of succinate dehydrogenase and protein content of carnitine O -palmitoyltransferase 1 were significantly decreased in livers of male fish exposed to DPhP, which further confirmed the proposed toxicological mechanisms. This study is the first to demonstrate that chronic, low-level exposure to DPhP can retard growth via inhibiting energy output in male zebrafish.
- Published
- 2021
- Full Text
- View/download PDF
35. Self-Shaping Microemulsion Gels for Cultural Relic Cleaning.
- Author
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Yang Y, Lian X, Yang Z, Zhou Y, Zhang X, and Wang Y
- Abstract
Cleaning is a foundational and essential operation of protection and restoration of cultural relics, which is also the key step of follow-up works. To overcome the problems of uncontrollable diffusion of cleaning solvents and poor coverage of the cleaning solvent carriers on rough surfaces, here, we propose a strategy of using a self-shaping microemulsion gel that is prepared via emulsifying oleophilic solvents into the specific shear-thinning hydrogel structures. The gel can adaptively cover rough surfaces during the cleaning process coupled with avoidance of unnecessary diffusion of the cleaning solvents, and the mechanical reinforcement of in situ polymerized double-network gels enables its easy peeling off from the surfaces without leaving determinable residues. As a representative demonstration, Paraloid B72, a widely used material for the repair and reinforcement of cultural relics, is employed as a model discolored coating, which can be effectively removed from the rough surface of simulated cultural relics after treatment with the resulting gels. Convincingly, the strategy of constructing agarose/polyacrylamide hybrid double-network gels with shear-thinning and self-shaping performances for the cleaning of cultural relics not only improves the convenience and accuracy of operation but also exhibits an efficient cleaning effect, which will greatly expand the application of microemulsion gels in the cleaning of rough surfaces of cultural relics.
- Published
- 2021
- Full Text
- View/download PDF
36. Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH 3 (CH 2 ) 4 NH 3 ]CdBr 4 Perovskite.
- Author
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Wu J, Li X, Lian X, Su B, Pang J, Li MD, Xia Z, Zhang JZ, Luo B, and Huang XC
- Abstract
Antimony-based metal halide hybrids have attracted enormous attention due to the stereoactive 5s
2 electron pair that drives intense triplet broadband emission. However, energy/charge transfer has been rarely achieved for Sb3+ -doped materials. Herein, Sb3+ ions are homogeneously doped into 2D [NH3 (CH2 )4 NH3 ]CdBr4 perovskite (Cd-PVK) using a wet-chemical method. Compared to the weak singlet exciton emission of Cd-PVK at 380 nm, 0.01% Sb3+ -doped Cd-PVK exhibits intense triplet emission located at 640 nm with a near-unity quantum yield. Further increasing the doping concentration of Sb3+ completely quenches singlet exciton emission of Cd-PVK, concurrently with enhanced Sb3+ triplet emission. Delayed luminescence and femtosecond-transient absorption studies suggest that Sb3+ emission originates from exciton transfer (ET) from Cd-PVK host to Sb3+ dopant, while such ET cannot occur with Pb2+ -doped Cd-PVK because of the mismatch of energy levels. In addition, density function theory calculations indicate that the introduced Sb3+ likely replace the Cd2+ ions along with the deprotonation of butanediammonium for charge balance, instead of generating Cd2+ vacancies. This work provides a deeper understanding of the ET of Sb3+ -doped Cd-PVK and suggests an effective strategy to achieve efficient triplet Sb3+ emission beyond 0D Cl-based hybrids.- Published
- 2021
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37. Structural Transformation and Second-Harmonic-Generation Activity in Rare-Earth and d 0 Transition-Metal Oxysulfides RE 3 NbS 3 O 4 (RE = Ce, Sm, Gd, Dy).
- Author
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Lian X, Lu ZT, Yao WD, Yang SH, Liu W, Tang RL, and Guo SP
- Abstract
Investigations of inorganic compounds with mixed anions have drawn much attention. Here, three oxysulfides, Sm
3 NbS3 O4 ( 1 ), Gd3 NbS3 O4 ( 2 ), and Dy3 NbS3 O4 ( 3 ), are obtained by solid-state reactions. 1 and 2 crystallize in the polar space group Pna 21 , while 3 crystallizes in the centric space group Pnma . The anionic frameworks of 1 and 2 are built by isolated distorted [NbS2 O4 ]7- octahedra, while [NbS3 O4 ]9- is used for 3 . 1 and 2 exhibit phase-matchable second-harmonic-generation (SHG) effects of about 0.3 and 0.4 × AGS at 2.1 μm. The [NbS2 O4 ]7- octahedron was first used as a SHG-active motif for nonlinear-optical (NLO) materials. A systematic analysis of the transformation between these crystal structures, NLO performances, and magnetic behaviors, as well as first-principles theoretical studies, is presented. This work enriches the study on relatively rarely explored NLO-active metal oxysulfides.- Published
- 2021
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38. Human Cancer Cell Membrane-Cloaked Fe 3 O 4 Nanocubes for Homologous Targeting Improvement.
- Author
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Zhang L, Xu H, Cheng Z, Wei Y, Sun R, Liang Z, Hu Y, Zhao L, Lian X, Li X, and Huang D
- Subjects
- Biomimetics, Cell Membrane, HeLa Cells, Humans, Nanoparticles, Neoplasms drug therapy
- Abstract
Surface modification of nanoparticles with cellular protein components is a new biomimetic modification strategy, which utilizes the inherent affinity between homologous cells to introduce the same surface molecules into nanoparticles to improve the targeting performance. In this study, oleic acid (OA)-coated Fe
3 O4 nanocubes were prepared by a high-temperature thermal decomposition method and modified by 3, 4-dihydroxyphenylpropionic acid (DHCA); then, HeLa cell membranes were introduced onto the surface of the nanocubes through mixed coextrusion to try to endow them with the targeting function of natural cells. The results show that the prepared Fe3 O4 nanocubes have high monodispersity, excellent water solubility, and biocompatibility. Moreover, the Fe3 O4 nanocubes encapsulated by cellular protein show an obvious core-shell structure and the specific targeting property to HeLa cells is improved significantly, which is expected to be used in clinical targeted diagnosis and treatment of cancer.- Published
- 2021
- Full Text
- View/download PDF
39. Monodispersed Ruthenium Nanoparticles on Nitrogen-Doped Reduced Graphene Oxide for an Efficient Lithium-Oxygen Battery.
- Author
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Dai W, Liu Y, Wang M, Lin M, Lian X, Luo Y, Yang J, and Chen W
- Abstract
Lithium-oxygen batteries with ultrahigh energy densities have drawn considerable attention as next-generation energy storage devices. However, their practical applications are challenged by sluggish reaction kinetics aimed at the formation/decomposition of discharge products on battery cathodes. Developing effective catalysts and understanding the fundamental catalytic mechanism are vital to improve the electrochemical performance of lithium-oxygen batteries. Here, uniformly dispersed ruthenium nanoparticles anchored on nitrogen-doped reduced graphene oxide are prepared by using an in situ pyrolysis procedure as a bifunctional catalyst for lithium-oxygen batteries. The abundance of ruthenium active sites and strong ruthenium-support interaction enable a feasible discharge product formation/decomposition route by modulating the surface adsorption of lithium superoxide intermediates and the nucleation and growth of lithium peroxide species. Benefiting from these merits, the electrode provides a drastically increased discharge capacity (17,074 mA h g
-1 ), a decreased charge overpotential (0.51 V), and a long-term cyclability (100 cycles at 100 mA g-1 ). Our observations reveal the significance of the dispersion and coordination of metal catalysts, shedding light on the rational design of efficient catalysts for future lithium-oxygen batteries.- Published
- 2021
- Full Text
- View/download PDF
40. One-Pot Fabrication of Hollow Porphyrinic MOF Nanoparticles with Ultrahigh Drug Loading toward Controlled Delivery and Synergistic Cancer Therapy.
- Author
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Sun X, He G, Xiong C, Wang C, Lian X, Hu L, Li Z, Dalgarno SJ, Yang YW, and Tian J
- Subjects
- Animals, Antineoplastic Agents pharmacokinetics, Antineoplastic Agents therapeutic use, Breast Neoplasms drug therapy, Breast Neoplasms pathology, Coloring Agents administration & dosage, Coloring Agents pharmacokinetics, Coloring Agents therapeutic use, Doxorubicin pharmacokinetics, Doxorubicin therapeutic use, Drug Delivery Systems, Drug Liberation, Female, Indocyanine Green pharmacokinetics, Indocyanine Green therapeutic use, Mice, Inbred BALB C, Photochemotherapy, Mice, Antineoplastic Agents administration & dosage, Delayed-Action Preparations chemistry, Doxorubicin administration & dosage, Indocyanine Green administration & dosage, Metal-Organic Frameworks chemistry, Porphyrins chemistry
- Abstract
Hollow nanostructures have attracted significant research interest in drug delivery systems due to their high capacities for drug loading and unique physicochemical properties, showing great potential in specific biomedical applications. Herein, hollow porphyrinic metal-organic framework (H-PMOF) nanoparticles with a mesoporous spherical shell have been fabricated via a facile self-sacrificial ZIF-8 nanoparticle template strategy. The H-PMOF nanoplatform not only demonstrates a greatly enhanced photodynamic therapy efficacy compared with nonhollow porphyrinic MOF nanoparticles but also can be used as a superior drug carrier to co-load doxorubicin (DOX) and indocyanine green (ICG) with an ultrahigh drug-loading capacity of 635%. Furthermore, cancer cell membrane camouflage of the (DOX and ICG)@H-PMOF composite nanoparticles affords a biomimetic nanoplatform, that is, (DOX and ICG)@H-PMOF@mem (DIHPm for short), with an outstanding homologous tumor-targeting and immune-escaping ability. Interestingly, DIHPm shows both pH-controlled and near-infrared laser-triggered DOX release. Both in vitro and in vivo studies of DIHPm demonstrate an excellent imaging-guided synergistic photodynamic/photothermal/chemotherapy anticancer activity with negligible systemic toxicity. The development of the high-performance H-PMOF nanoplatform provides new insights into the design of MOF-based multifunctional nanomedicines for combination cancer therapy and precise theranostics.
- Published
- 2021
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41. Atom by Atom Condensation of Sn Single Clusters within Gold-Phosphorus Metal-Inorganic Porous Networks.
- Author
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Zhang JL, Zhao S, Sun S, Wang W, Ma Z, Lian X, Li Z, and Chen W
- Abstract
Surface supported single-atom catalysts (SACs) and single-cluster catalysts (SCCs) have been an area of rapidly growing interest due to their high efficiency of metal atom utilization and high selectivity and activity toward various catalytic reactions. However, achieving highly dispersed, structurally well-defined SACs and SCCs with high surface loadings while avoiding their sintering to larger nanoparticles (NPs) still remains a nontrivial challenge. Here, by utilizing a recently fabricated porous metal-inorganic gold-phosphorus (AuP) network, highly dispersed single Sn clusters with high surface density can be realized. This is attributed to a synergistic effect of the P
6 Au6 pores for providing the preferential binding sites to anchor Sn atoms and the role of P9 units as a blocking barrier to prevent the growth of Sn to larger NPs. The atom by atom condensation process of Sn single clusters with sizes ranging from monomers to heptamers as well as their binding configurations with the supporting surface are precisely identified at the atomic level, through the combination of a low-temperature scanning tunneling microscope and density functional theory calculations. Our approach opens new opportunities of utilizing metal-inorganic porous networks for the stabilization of highly dispersed and well-defined SACs and SCCs.- Published
- 2021
- Full Text
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42. KNa 2 ZrF 7 : A Mixed-Metal Fluoride Exhibits Phase-Matchable Second-Harmonic-Generation Effect and High Laser-Induced Damage Threshold.
- Author
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Lian X, Yao WD, Liu W, Tang RL, and Guo SP
- Abstract
Halides are one type of important IR nonlinear-optical material candidate. Here, a mixed alkali metal and d
0 transition-metal fluoride, namely, KNa2 ZrF7 , was obtained by a facile hydrothermal method. It crystallizes in an orthorhombic system with the polar space group Pmn 21 , and its pseudo -1D structure features isolated (ZrF7 )3- moncocapped trigonal prisms, which are ionically linked together by countercations K+ and Na+ , representing a new type of fluoride. The powder sample of KNa2 ZrF7 exhibits a moderate second-harmonic-generation response and a high laser-induced damage threshold. Besides, it can realize phase matchability and possesses a wide-IR transparent window. Thermal stability analysis suggests that KNa2 ZrF7 is a congruent compound. Structural comparisons with related fluorides and theoretical calculations are also presented in this work.- Published
- 2021
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43. Realization of a Buckled Antimonene Monolayer on Ag(111) via Surface Engineering.
- Author
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Sun S, Yang T, Luo YZ, Gou J, Huang Y, Gu C, Ma Z, Lian X, Duan S, Wee ATS, Lai M, Zhang JL, Feng YP, and Chen W
- Abstract
The degree of buckling of two-dimensional (2D) materials can have a dramatic impact on their corresponding electronic structures. Antimonene (β-phase), a new 2D material with air stability and promising electronic properties, has been engineered to adopt flat or two-heights-buckling geometries by employing different supporting substrates for epitaxial growth. However, studies of the antimonene monolayer with a more buckled configuration are still lacking. Here, we report the synthesis of an antimonene monolayer with a three-heights-buckling configuration overlaid on SbAg
2 surface alloy-covered Ag(111) by molecular beam epitaxy, in which the underlying surface alloy provides interfacial interactions to modulate the structure of the antimonene monolayer. The atomic structure of the synthesized antimonene has been precisely identified through a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. The successful fabrication of a buckled antimonene monolayer could provide a promising way to modulate the structures of 2D materials for future electronic and optoelectronic applications.- Published
- 2020
- Full Text
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44. Polymer Modification on the NiO x Hole Transport Layer Boosts Open-Circuit Voltage to 1.19 V for Perovskite Solar Cells.
- Author
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Lian X, Chen J, Shan S, Wu G, and Chen H
- Abstract
Inverted-structure perovskite solar cells (PVSCs) applying NiO
x as the hole transport layer (HTL) have attracted increasing attention. It is still a challenge to optimize the contact between NiOx and the perovskite layer and to suppress energy loss at the interface. In this study, interface engineering was carried out by modifying the NiOx layer with different polymers such as polystyrene, poly(methyl methacrylate) (PMMA), or poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) to improve the surface contact between NiOx and the perovskite, to decrease the defect states, and to make the energy level alignment better. The NiOx /PMMA-based device presents a Voc as high as 1.19 V because of the improved interfacial contact and the interaction of the carbonyl and methoxy group with Pb2+ . The NiOx /PTAA-based device with the structure ITO/NiOx /PTAA/(MAPbI3 )0.95 (MAPbBr2 Cl)0.05 /PCBM/BCP/Ag exhibits the highest power conversion efficiency of 21.56% with a high Voc of 1.19 V. The enhanced performance can be attributed to the deepened highest occupied molecular orbital level of NiOx /PTAA, which matched well with that of the perovskite and suppressed interface energy loss as well. This work provides a facile approach for efficiently improving the Voc of NiOx -based PVSCs.- Published
- 2020
- Full Text
- View/download PDF
45. Defect-Related Broadband Emission in Two-Dimensional Lead Bromide Perovskite Microsheets.
- Author
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Li X, Lian X, Pang J, Luo B, Xiao Y, Li MD, Huang XC, and Zhang JZ
- Abstract
Low-dimensional hybrid lead halide perovskites (LHPs) with broadband emission (BE) have been developed as promising candidates for single-source white-light-emitting diodes. However, the underlying origin of such BE is poorly understood. Herein, dual-emissive [NH
3 (CH2 )8 NH3 ]PbBr4 perovskite microsheets (PMSs) with good dispersibility are successfully prepared. Besides the general narrowband emission (NE) originating from free excitons, BE (∼522 nm) is generated under a Br-poor condition, which is not observed in the single-crystal sample. Unlike self-trapped exciton emission, the BE observed in PMSs is experimentally determined to be related to bromide vacancies (VBr ), thereby exhibiting quasisaturation under high excitation intensity. Femtosecond transient absorption spectroscopy first shows that the trapping time of the photogenerated electrons by acceptor-like VBr- is ∼15 ps, slower than that by surface defects (<1 ps). This study provides new insight into the underlying mechanism of BE and an effective approach to manipulating the optical properties of 2D perovskites.- Published
- 2020
- Full Text
- View/download PDF
46. Effect of pH or Metal Ions on the Oil/Water Interfacial Behavior of Humic Acid Based Surfactant.
- Author
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Lian X, Liao S, Yang Y, Zhang X, and Wang Y
- Abstract
Humic acid, a kind of widespread organic macromolecule on earth, is naturally formed through the microbial biodegradation of plant, animal, and microorganism residues. Because of the large number of active functional groups (phenolic hydroxyl and carboxyl), humic acid has been considered as a biocompatible, green, and low-cost biosurfactant recently. In this work, based on the sensitivity of humic acid to the external chemical environment, the oil/water interfacial behavior of sodium humate at different pH or in the presence of metal ions is closely investigated. Sodium humate is significantly enriched toward the oil/water interface at either low pH or high metal-ion concentration to adjust the properties of the prepared emulsion, but the mechanisms are proved to be different when considering the influence of pH and metal ions. Besides, to the best of our knowledge, humic acid based surfactant is proposed as a Pickering emulsifier for the first time, known as solid surfactant. This work promises the great potential of humic acid as a natural environment-responsive surfactant and has important implications for the application of humic acid based surfactant in industry and understanding of the role of humic acid in the natural environment.
- Published
- 2020
- Full Text
- View/download PDF
47. Redox-Driven Spontaneous Double Emulsion.
- Author
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Li R, Wang Z, Tao X, Jia J, Lian X, and Wang Y
- Abstract
The formation of spontaneous double emulsions is a peculiar phenomenon in emulsion systems. When compared to the traditional one-step and two-step methods for preparing double emulsions, spontaneous emulsification can not only steadily load uniform water droplets into an oil phase, but can also facilitate the preparation of emulsions with higher stability. However, the limited solubility of salts, which are typically used to modify osmotic pressure, in organic oils has inhibited the viability of this method for the preparation of W/O/W double emulsions. In this paper, a redox-driven spontaneous emulsification method is developed and investigated. Instead of employing oil-soluble salts, an oxidation reaction is implemented in the oil phase, which produces cation radicals and iodide counterions to generate osmotic pressure. Additionally, amphiphilic polymer chains are harnessed as stabilizers for the newly formed W/O interfaces. Various characterization methods have been used to elucidate the mechanism of both the oxidation reaction and the spontaneous formation of double emulsions.
- Published
- 2020
- Full Text
- View/download PDF
48. Antineoplastic Mitoxantrone Monitor: A Sandwiched Mixed Matrix Membrane (MMM) Based on a Luminescent MOF-Hydrogel Hybrid.
- Author
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Lian X, Zhang Y, Wang J, and Yan B
- Subjects
- Animals, Fluorescence Resonance Energy Transfer methods, Goats, Limit of Detection, Luminescence, Point-of-Care Testing, Antineoplastic Agents blood, Hydrogels chemistry, Luminescent Agents chemistry, Membranes, Artificial, Metal-Organic Frameworks chemistry, Mitoxantrone blood
- Abstract
A sandwiched mixed matrix membrane (MMM) based on a metal-organic framework-hydrogel hybrid exhibits eximious performance in the detection of mitoxantrone. Parts per billion-level sensitivity and good selectivity in serum among other analogous antineoplastics have been achieved. This flexible MMM can be used for point-of-care testing drugs in a biological medium.
- Published
- 2020
- Full Text
- View/download PDF
49. Inhibiting Cell Viability and Motility by Layer-by-Layer Assembly and Biomineralization.
- Author
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Wei Y, Xu H, Xu S, Su H, Zhang L, Sun R, Huang D, Zhao L, Wang K, Hu Y, and Lian X
- Abstract
Herein, we proposed a drug-free strategy named cell surface shellization to inhibit the motility of SKOV-3 and HeLa cells. We alternately deposited two- or three-layer cationic polyelectrolyte (PE) and anionic PE films on the surface of SKOV-3 and HeLa cells. Then, a mineral shell (calcium carbonate, CaCO
3 ) was formed on the surface of polymer shells via electrostatic force and biomineralization. The CCK-8 assay results and live/dead staining showed that the surface shells strongly aggravated the cytotoxicity. The monolayer scratch wound migration assay results and immunofluorescence staining results showed that the shells, especially the mineral shells, could efficiently inhibit the migration of SKOV-3 and HeLa cells without any anticancer drugs. The immunofluorescence results of the three small G proteins of the cells showed that the immunofluorescence intensity in SKOV-3 did not change. Preliminary results from our laboratory showed an increase in MMP-9 secreted by cancer cells after coating with films or mineral shells. It suggests that mechanisms that inhibit cell migration are related to the MMP signaling pathway. All the results indicated that shellization (films or nanomineral shells) but not limited to calcification can be used as one of the tools to change the function of cells., Competing Interests: The authors declare no competing financial interest., (Copyright © 2020 American Chemical Society.)- Published
- 2020
- Full Text
- View/download PDF
50. Designing Kagome Lattice from Potassium Atoms on Phosphorus-Gold Surface Alloy.
- Author
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Sun S, Zhao S, Luo YZ, Gu X, Lian X, Tadich A, Qi DC, Ma Z, Zheng Y, Gu C, Zhang JL, Li Z, and Chen W
- Abstract
Materials with flat bands are considered as ideal platforms to explore strongly correlated physics such as the fractional quantum hall effect, high-temperature superconductivity, and more. In theory, a Kagome lattice with only nearest-neighbor hopping can give rise to a flat band. However, the successful fabrication of Kagome lattices is still very limited. Here, we provide a new design principle to construct the Kagome lattice by trapping atoms into Kagome arrays of potential valleys, which can be realized on a potassium-decorated phosphorus-gold surface alloy. Theoretical calculations show that the flat band is less correlated with the neighboring trivial electronic bands, which can be further isolated and dominate around the Fermi energy with increased Kagome lattice parameters of potassium atoms. Our results provide a new strategy for constructing Kagome lattices, which serve as an ideal platform to study topological and more general flat band phenomena.
- Published
- 2020
- Full Text
- View/download PDF
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