167 results on '"Ye, W."'
Search Results
2. Shock-Induced Ignition of Methane, Ethane, and Methane/Ethane Mixtures Sensitized by NO2.
- Author
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Zhang, X., Ye, W., Shi, J. C., Wu, X. J., Zhang, R. T., and Luo, S. N.
- Published
- 2017
- Full Text
- View/download PDF
3. Experimental and Kinetic Modeling Study of CH3OCH3 Ignition Sensitized by NO2.
- Author
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Ye, W., Shi, J. C., Zhang, R. T., Wu, X. J., Zhang, X., Qi, M. L., and Luo, S. N.
- Published
- 2016
- Full Text
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4. Ignition Delay Time Measurements on CH4/CH3Cl/O2/Ar Mixtures for Kinetic Analysis.
- Author
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Shi, J. C., Ye, W., Bie, B. X., Long, X. J., Zhang, R. T., Wu, X. J., and Luo, S. N.
- Published
- 2016
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5. Carbon Nanotubes Connecting and Encapsulating MoS 2 -Doped SnO 2 Nanoparticles as an Excellent Lithium Storage Performance Anode Material.
- Author
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Jiang C, Ye W, Xu H, Feng Z, Xiong D, and He M
- Abstract
Doping and carbon encapsulation modifications have been proven to be effective methods for enhancing the lithium storage performance of batteries. The hydrothermal method and ball milling are commonly used methods for material synthesis. In this study, a composite anode material rich in carbon nanotubes (CNTs) conductive tubular network connection and encapsulation of SnO
2 -MoS2 @CNTs (SMC) was synthesized by combining these two methods. In this highly conductive network, nano-SnO2 particles are uniformly dispersed and embedded in MoS2 with a layered structure, and the obtained SnO2 -MoS2 composite material is tightly connected and encapsulated by the tubular network of CNTs. It is worth noting that the incorporation of layered MoS2 not only effectively anchors the SnO2 nanoparticles, but also provides a broader space for lithium-ion movement due to the larger interlayer spacing. The conductive network of CNTs shortens the diffusion path of electrons and Li+ and provides more diffusion channels. The reversible capacity of the SnO2 -MoS2 @CNTs nanocomposite material remains at 1069.3 mA h g-1 after 320 cycles at 0.2 A g-1 , and it exhibits excellent long-term cycling stability, maintaining 904.5 mA h g-1 after 1000 cycles at 1.0 A g-1 . The composite material demonstrates excellent pseudocapacitive contribution rate performance, with a contribution rate of 87% at 2.0 mV s-1 . The results indicate that SnO2 -MoS2 @CNTs has excellent electrochemical lithium storage performance and is a promising anode material for lithium-ion batteries.- Published
- 2024
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6. Cluster-Level Heterostructure of PMo 12 /Cu for Efficient and Selective Electrocatalytic Hydrogenation of High-Concentration 5-Hydroxymethylfurfural.
- Author
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Cao X, Ding Y, Chen D, Ye W, Yang W, and Sun L
- Abstract
Electrochemical hydrogenation of aldehyde molecules, exemplified by 5-hydroxymethylfurfural (HMF), offers a sustainable approach for synthesizing higher value-added alcohols. However, severe coupling side reactions impede its practical implementation at high concentrations. In this work, a cluster-level heterostructure of a PMo
12 /Cu catalyst is synthesized by loading Keggin-type phosphomolybdic acid (H3 PMo12 O40 , PMo12 ) onto Cu nanowires. The catalyst exhibits high selectivity in electrocatalytic hydrogenation (ECH) of HMF to 2,5-bishydroxymethylfuran (BHMF) under an unprecedentedly high substrate concentration of 1.0 M. Under -0.3 V (vs RHE) with 1.0 M HMF, PMo12 /Cu shows a Faradaic efficiency as high as 98% with an excellent productivity of 4.35 mmol cm-2 h-1 toward BHMF, much higher than those on the pristine Cu nanowires. Mechanism studies and density functional theory calculations demonstrate that the heterostructural interface of PMo12 /Cu serves as an active reaction center for the ECH. The unique electronic properties and geometric structure promote the dissociative reduction of water molecules to generate H* and reduce HMF with a decreased reaction energy barrier, which is responsible for exceptional reactivity and selectivity.- Published
- 2024
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7. Cation-Triggered Growth of Nanowires for Enhanced Oxygen Evolution Reaction.
- Author
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Wang L, Ye W, Zhang Z, Hua Y, Cai C, Zhang Z, Wu Y, Wang K, Yang W, Shi W, and Hao J
- Abstract
The oxygen evolution reaction (OER), which occurs in a variety of energy-related devices, necessitates optimization of the reaction pathways for efficient and scalable deployment. Nevertheless, fully harnessing the advanced structure of synthetic electrocatalysts remains a significant challenge due to the inevitable surface reconstruction process during OER. Here we present an efficient and flexible method to control the surface reconstruction process by engineering an electrolyte containing trace Co
2+ cation. This controllable reconstruction process enhances fast charge transfer, facilitates electroactive species transport, and exposes the inner active site, significantly improving the OER kinetics. An impressive 60% increase in current density at an applied potential of 2.2 V (vs RHE) confirms its remarkable contribution to the performance. The identification of cation-triggered reconstruction for the formation of a well-defined surface provides a novel insight into understanding electrolyte engineering and offers a viable pathway to address activity and stable concerns in electrocatalysts.- Published
- 2024
- Full Text
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8. DrugFlow: An AI-Driven One-Stop Platform for Innovative Drug Discovery.
- Author
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Shen C, Song J, Hsieh CY, Cao D, Kang Y, Ye W, Wu Z, Wang J, Zhang O, Zhang X, Zeng H, Cai H, Chen Y, Chen L, Luo H, Zhao X, Jian T, Chen T, Jiang D, Wang M, Ye Q, Wu J, Du H, Shi H, Deng Y, and Hou T
- Subjects
- Molecular Docking Simulation, Quantitative Structure-Activity Relationship, Algorithms, Drug Design, Software, Humans, Cloud Computing, Drug Discovery methods, Artificial Intelligence
- Abstract
Artificial intelligence (AI)-aided drug design has demonstrated unprecedented effects on modern drug discovery, but there is still an urgent need for user-friendly interfaces that bridge the gap between these sophisticated tools and scientists, particularly those who are less computer savvy. Herein, we present DrugFlow, an AI-driven one-stop platform that offers a clean, convenient, and cloud-based interface to streamline early drug discovery workflows. By seamlessly integrating a range of innovative AI algorithms, covering molecular docking, quantitative structure-activity relationship modeling, molecular generation, ADMET (absorption, distribution, metabolism, excretion and toxicity) prediction, and virtual screening, DrugFlow can offer effective AI solutions for almost all crucial stages in early drug discovery, including hit identification and hit/lead optimization. We hope that the platform can provide sufficiently valuable guidance to aid real-word drug design and discovery. The platform is available at https://drugflow.com.
- Published
- 2024
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9. Synthesis of Monodispersed Pd Nanoparticles and Ultrathin Twisty Pd Nanowire Networks for Electrooxidation of Ethanol.
- Author
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Liao X, Lao X, Li Z, Yang L, Ye W, and Guo P
- Abstract
In recent years, preparing precious metal catalysts with a controllable morphology has become a hot research topic for researchers. In this study, monodispersed palladium (Pd) nanoparticles (NP) and ultrathin Pd twisty nanowire networks (TNN) were synthesized in a solvothermal system using N , N -dimethylformamide (DMF) and oleylamine (OAm) as solvents, Transmission electron microscopy (TEM) images reveal the successful synthesis of nanoparticles and ultrathin TNN microstructures. Electrochemical data show that the current densities of Pd-NP and Pd-TNN for the ethanol oxidation reaction (EOR) reach 1878 mA mg
-1 and 1765 mA mg-1 , respectively. Compared to commercial Pd/C, Pd-TNN and Pd-NP exhibit better catalytic stability, lower electron transfer barriers, and more resistance to catalyst poisoning. Temperature, pH value, and ethanol concentration are all favorable for the EOR. According to the experimental data, the mechanism of enhanced electrocatalytic activity of Pd-NP and Pd-TNN catalysts for ethanol oxidation is discussed. This paper presents a method for preparing catalysts with stabilized structures to develop Pd-based catalysts for electrocatalytic oxidation reactions.- Published
- 2024
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10. Versatile Composite Binder with Fast Lithium-Ion Transport for LiCoO 2 Cathodes.
- Author
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Ye W, He W, Long J, Chen P, Ding B, Dou H, and Zhang X
- Abstract
The low ionic conductivity of LiCoO
2 limits the rate performance of the overall electrode. Here, a polymeric composite binder composed of poly(vinylidene fluoride) (PVDF) and poly(ethylene oxide) (PEO) is reported to efficiently improve the ion transport in the LiCoO2 electrode. This is where the lithium-ion transport channel constructed by oxygen atoms of PEO can afford the electrode a lithium-ion transport number ( tLi ) as high as 0.70 with the optimized composite binder in a mass ratio of 1:1 (O5F5), significantly higher than that of traditional PVDF (0.44). As a result, the O5F5 binder endows the LiCoO+ 2 electrode with an impressive capacity of 90 mAh g-1 even at 15 C, which is twice as high as the PVDF electrode. In addition, the initial Coulombic efficiency of the LiCoO2 electrode with the O5F5 binder is close to 100% and the capacity retention is 91% after 100 cycles at 1 C. This study overcomes the problem of slow ion conductivity of the LiCoO2 electrode, providing an easy method for developing high-rate cathode binders.- Published
- 2024
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11. Molecular Pharmacology of Selective Na V 1.6 and Dual Na V 1.6/Na V 1.2 Channel Inhibitors that Suppress Excitatory Neuronal Activity Ex Vivo.
- Author
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Goodchild SJ, Shuart NG, Williams AD, Ye W, Parrish RR, Soriano M, Thouta S, Mezeyova J, Waldbrook M, Dean R, Focken T, Ghovanloo MR, Ruben PC, Scott F, Cohen CJ, Empfield J, and Johnson JP
- Subjects
- Humans, Neurons metabolism, Brain metabolism, Seizures drug therapy, Seizures metabolism, Action Potentials physiology, Voltage-Gated Sodium Channels metabolism, Epilepsy metabolism
- Abstract
Voltage-gated sodium channel (Na
V ) inhibitors are used to treat neurological disorders of hyperexcitability such as epilepsy. These drugs act by attenuating neuronal action potential firing to reduce excitability in the brain. However, all currently available NaV -targeting antiseizure medications nonselectively inhibit the brain channels NaV 1.1, NaV 1.2, and NaV 1.6, which potentially limits the efficacy and therapeutic safety margins of these drugs. Here, we report on XPC-7724 and XPC-5462, which represent a new class of small molecule NaV -targeting compounds. These compounds specifically target inhibition of the NaV 1.6 and NaV 1.2 channels, which are abundantly expressed in excitatory pyramidal neurons. They have a > 100-fold molecular selectivity against NaV 1.1 channels, which are predominantly expressed in inhibitory neurons. Sparing NaV 1.1 preserves the inhibitory activity in the brain. These compounds bind to and stabilize the inactivated state of the channels thereby reducing the activity of excitatory neurons. They have higher potency, with longer residency times and slower off-rates, than the clinically used antiseizure medications carbamazepine and phenytoin. The neuronal selectivity of these compounds is demonstrated in brain slices by inhibition of firing in cortical excitatory pyramidal neurons, without impacting fast spiking inhibitory interneurons. XPC-5462 also suppresses epileptiform activity in an ex vivo brain slice seizure model, whereas XPC-7224 does not, suggesting a possible requirement of Nav1.2 inhibition in 0-Mg2+ - or 4-AP-induced brain slice seizure models. The profiles of these compounds will facilitate pharmacological dissection of the physiological roles of NaV 1.2 and NaV 1.6 in neurons and help define the role of specific channels in disease states. This unique selectivity profile provides a new approach to potentially treat disorders of neuronal hyperexcitability by selectively downregulating excitatory circuits.- Published
- 2024
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12. Design, Synthesis, and Biological Evaluation of Pierardine Derivatives as Novel Brain-Penetrant and In Vivo Potent NMDAR-GluN2B Antagonists for Ischemic Stroke Treatment.
- Author
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Lin G, Xu Q, Li J, Chu Z, Ma X, Zhu Q, Zhao Y, Mo J, Ye W, Shao L, Fang T, He M, Yue S, and Dai M
- Subjects
- Humans, Receptors, N-Methyl-D-Aspartate metabolism, Brain metabolism, Structure-Activity Relationship, Ischemic Stroke
- Abstract
A series of structurally novel GluN2B NMDAR antagonists were designed, synthesized, and biologically evaluated as anti-stroke therapeutics by optimizing the chemical structure of Pierardine , the active ingredient of traditional Chinese medicine Dendrobium aphyllum (Roxb.) C. E. Fischer identified via in silico screening. The systematic structure-activity relationship study led to the discovery of 58 with promising NMDAR-GluN2B binding affinity and antagonistic activity. Of the two enantiomers, S -58 exhibited significant inhibition (IC
50 = 74.01 ± 12.03 nM) against a GluN1/GluN2B receptor-mediated current in a patch clamp assay. In addition, it displayed favorable specificity over other subtypes and off-target receptors. In vivo , S -58 exerted therapeutic efficacy comparable to that of the approved GluN2B NMDAR antagonist ifenprodil and excellent safety profiles. In addition to the attractive in vitro and in vivo potency, S -58 exhibited excellent brain exposure. In light of these merits, S -58 has been advanced to further preclinical investigation as a potential anti-stroke candidate.- Published
- 2024
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13. Iodine-Mediated δ-Amination of sp 3 C-H Bonds.
- Author
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Ye W, Xiong H, Wang M, Chang J, and Yu W
- Abstract
We present a direct δ-amination reaction of sp
3 C-H bonds, employing molecular iodine (I2 ) as the sole oxidant under transition-metal-free conditions. This remote C-H functionalization approach is operationally simple and provides facile, efficient access to pyrrolidines and related heterocyclic derivatives from readily accessible substrates.- Published
- 2024
- Full Text
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14. In Situ Multicolor Imaging of Photocatalytic Degradation Process of Permanganate on Single Bismuth-Based Metal-Organic Frameworks.
- Author
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Li Y, Ye W, Yu H, and He Y
- Abstract
Bismuth-based metal-organic frameworks (Bi-MOFs) have emerged as important photocatalysts for pollutant degradation applications. Understanding the photocatalytic degradation mechanism is key to achieving technological advantage. Herein, we apply dark-field optical microscopy (DFM) to realize in situ multicolor imaging of the photocatalytic degradation process of permanganate (MnO
4 - ) on single CAU-17 Bi-MOFs. Three reaction kinetic processes such as surface adsorption, photocatalytic reduction, and disproportionation are revealed by combining the time-lapsed DFM images with optical absorption spectra, indicating that the photocatalytic reduction of purple MnO4 - first produces beige red MnO4 2- through a one-electron pathway, and then MnO4 2- disproportionates into yellow MnO2 on CAU-17. Meanwhile, we observe that the deposition of MnO2 cocatalysts enhances the surface adsorption reaction and the photocatalytic reduction of MnO4 - to MnO4 2- . Unexpectedly, it is found that isopropanol as a typical hole scavenger can stabilize MnO4 2- , avoiding disproportionation and causing the alteration of the photocatalytic reaction pathway from a one-electron avenue to a three-electron (1 + 2) process for producing MnO2 on CAU-17. This research opens up the possibility of comprehensively tracking and understanding the photocatalytic degradation reaction at the single MOF particle level.- Published
- 2024
- Full Text
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15. Facile Fabrication of Polymer Electrolytes with Branched Structure via Deep Eutectic Electrolyte-Enabled In Situ Polymerizations.
- Author
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Wang J, Zhang Y, Ye W, Guo K, Zhou X, and Xue Z
- Abstract
The demand for higher energy density in energy storage devices drives further research on lithium metal batteries (LMBs) because of the high theoretical capacity and low voltage of lithium metal anode. Polymer electrolytes (PEs) exhibit obvious advantages in combating volatilization and leakage compared with liquid electrolytes, which improves the safety of LMBs. However, it is still difficult to construct PEs with a stable electrolyte-electrode interface for high-performance and long-term life LMBs. Herein, the gel polymer electrolyte (GPE-SL) containing deep eutectic electrolyte (DEE) and branchlike polymer skeleton are designed and prepared by the DEE-induced in situ cationic and radical polymerizations. The DEE provides a smooth Li
+ migration pathway to ensure the electrochemical properties, and the multibrominated polymer matrix formed in situ enables a LiBr-rich solid electrolyte interphase (SEI) layer on lithium metal anode and prolongs the life span of LMBs. Hence, the Li|GPE-SL|LiFePO4 battery displays an excellent cycling stability with 84% capacity retention after 1200 cycles at 1C. This simple deep eutectic electrolyte-induced polymerization method provides a promising direction for high-performance LMBs with improved anode-electrolyte compatibility through the construction of a stable SEI layer in situ .- Published
- 2024
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16. Efficient Rh-Catalyzed Chemo- and Enantioselective Hydrogenation of 2-CF 3 -Chromen/Thiochromen-4-ones.
- Author
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Xie C, Guo Q, Wu X, Ye W, and Hou G
- Abstract
A Rh-catalyzed highly chemo- and enantioselective hydrogenation of 2-CF
3 -chromen/thiochromen-4-ones was successfully established achieving excellent selectivity and high turnover numbers. Under mild conditions, a series of 2-CF3 -chromen-4-ones were hydrogenated to provide the corresponding chiral 2-CF3 -chroman-4-ones with excellent enantioselectivities (up to 99.9% ee) and achieve high turnover numbers (TON of up to 11,800). Moreover, the obtained hydrogenation products were also successfully transformed into other derivatives including the important intermediate of plasmepsin inhibitors with maintained enantiopurity.- Published
- 2023
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17. Overcoming the Heat Transfer Paradox: Nano Ridges Induce "Pistol Bubbles" and Reverse the Boiling Curve.
- Author
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Xu J, Ye W, Yu X, and Zhang B
- Abstract
To increase the boiling heat transfer limit, we disrupted the previously nonevaporating region and increased the vaporization activity of "inert" liquid molecules by introducing nano ridges on the boiling surface. This solved the paradox of no heat transfer occurring through the thinnest liquid film in boiling bubbles; thus, the internal heat transfer limit of the bubbles was exceeded. We found that vigorous boiling occurred immediately once the nonevaporating region was activated, and the bubble frequency increased by an order of magnitude, reaching 1186 Hz, which has not been previously reported. With an increase in heat flux, the boiling curve exhibited a "return". We achieved an extremely high bubble frequency by experimentally quantifying the major influence of nonevaporating region disruption on boiling heat transfer. The mechanism behind the generation of the ultrahigh-frequency bubbles was discovered. This study also reveals a new mechanism for the reversed boiling curve.
- Published
- 2023
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18. Correction to "Nonlocal Optical Response of Particle Plasmons in Single Gold Nanorods".
- Author
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Ye W
- Published
- 2023
- Full Text
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19. Convergent Biocatalytic Mediated Synthesis of siRNA.
- Author
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Paul S, Gray D, Caswell J, Brooks J, Ye W, Moody TS, Radinov R, and Nechev L
- Subjects
- Humans, RNA, Small Interfering genetics, Biocatalysis, Phosphorylation, Oligonucleotides chemistry
- Abstract
New technologies are required to combat the challenges faced with manufacturing commercial quantities of oligonucleotide drug substances which are required for treating large patient populations. Herein we report a convergent biocatalytic synthesis strategy for an Alnylam model siRNA. The siRNA chemical structure includes several of the unnatural modifications and conjugations typical of siRNA drug substances. Using Almac's 3-2-3-2 hybrid RNA ligase enzyme strategy that sequentially ligates short oligonucleotide fragments (blockmers), the target siRNA was produced to high purity at 1 mM concentration. Additional strategies were investigated including the use of polynucleotide kinase phosphorylation and the use of crude blockmer starting materials without chromatographic purification. These findings highlight a path toward a convergent synthesis of siRNAs for large-scale manufacture marrying both enzymatic liquid and classical solid-phase synthesis.
- Published
- 2023
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20. Rh-Catalyzed Asymmetric Hydrogenation of α-Substituted Alkenyl Sulfones: Highly Chemo- and Enantioselective Access to Chiral Sulfones.
- Author
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Wu X, Su Y, Zi G, Ye W, and Hou G
- Abstract
Rh-( R , R )-f-spiroPhos complex-catalyzed asymmetric hydrogenation of α-substituted alkenyl sulfones has been achieved, affording the chiral γ-keto sulfones and simple α-alkyl-substituted sulfones in high yields (96-99%) with excellent chemo-/enantioselectivities (86-96% ee) and high turnover numbers (TONs) of up to 4000. The method provides an efficient and high-enantioselectivity strategy for chiral γ-keto sulfones and simple α-substituted sulfones under mild conditions. Moreover, the obtained hydrogenation product was transformed into other important chiral α-substituted sulfones.
- Published
- 2023
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21. Intrinsically Disordered Flanking Regions Increase the Affinity of a Transcriptional Coactivator Interaction across Vertebrates.
- Author
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Karlsson E, Ottoson C, Ye W, Andersson E, and Jemth P
- Subjects
- Animals, Humans, Amino Acid Sequence, Cell Membrane, Zebrafish
- Abstract
Interactions between two proteins are often mediated by a disordered region in one protein binding to a groove in a folded interaction domain in the other one. While the main determinants of a certain interaction are typically found within a well-defined binding interface involving the groove, recent studies show that nonspecific contacts by flanking regions may increase the affinity. One example is the coupled binding and folding underlying the interaction between the two transcriptional coactivators NCOA3 (ACTR) and CBP, where the flanking regions of an intrinsically disordered region in human NCOA3 increases the affinity for CBP. However, it is not clear whether this flanking region-mediated effect is a peculiarity of this single protein interaction or if it is of functional relevance in a broader context. To further assess the role of flanking regions in the interaction between NCOA3 and CBP, we analyzed the interaction across orthologs and paralogs (NCOA1, 2, and 3) in human, zebra fish, and ghost shark. We found that flanking regions increased the affinity 2- to 9-fold in the six interactions tested. Conservation of the amino acid sequence is a strong indicator of function. Analogously, the observed conservation of increased affinity provided by flanking regions, accompanied by moderate sequence conservation, suggests that flanking regions may be under selection to promote the affinity between NCOA transcriptional coregulators and CBP.
- Published
- 2023
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22. Dimethyl Ferrocene-Induced Ambient-Processed High-Quality Films toward Efficient Perovskite Solar Cells for Industrial Application.
- Author
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Ou D, Ye W, Shang MH, Tu J, Zheng J, Wang L, Yang W, Du Z, and Yang Z
- Abstract
Metal halide perovskite solar cells (PSCs) have recently made significant progress with power conversion efficiencies (PCEs) boosted from 3.8% to a certified one over 26.1%, partially benefiting from the high-quality perovskite film enabled by the effective one-step spin-coating route. However, an extra antisolvent step with poor controllability and producibility is often involved in such a process, and some intrinsic defects are generated inevitably, especially in ambient atmospheric conditions, thus fundamentally limiting the commercialization of PSCs. Here, we introduce 1,1'dimethyl ferrocene into methylammonium lead halide precursor, which could not only recover the defects within perovskite film but also simplify the process without the extra antisolvent step. Accordingly, a dense and uniform perovskite film with large grains has been obtained under ambient conditions, which has much lower defect density, better stability against moisture penetration, and enhanced thermal tolerance than the control one, delivering a champion PCE of 16.92%. Current work sheds light on the simplified air-processed strategy for high-quality perovskite films, which might pave the way for exploring efficient and stable PSCs toward industrial applications.
- Published
- 2023
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23. Nonlocal Optical Response of Particle Plasmons in Single Gold Nanorods.
- Author
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Ye W
- Abstract
The investigation of particle plasmons in metal nanoparticles has predominantly relied on local optical response approximations. However, as the nanoparticle size approaches the average distance of electrons to the metal surface, mesoscopic effects such as size-dependent plasmon line width broadening and resonance energy blue shifts are expected to become observable. In this work, we compared the experimental spectral characteristics with simulated values obtained by using a generalized nonlocal optical response theory-based local analogue model. Our results show that the nonlocal plasmon damping effects in single nanoparticles are less pronounced than those observed in plasmon-coupled systems. Furthermore, our research demonstrates that single-particle dark-field spectroscopy is an effective tool for investigating the nonlocal optical response of particle plasmons in single nanoparticles. These results have important implications for the rational design of novel nanophotonic devices.
- Published
- 2023
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24. Mechanistic Insights into the Biodegradation of Carbon Dots by Fungal Laccase.
- Author
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Feng Y, He Y, Ye W, Lao J, Guan DX, Dong S, Liu G, and Mao L
- Subjects
- Biodegradation, Environmental, Mass Spectrometry, Biotransformation, Trametes metabolism, Laccase chemistry, Laccase metabolism, Carbon
- Abstract
While carbon dots (CDs) have the potential to support the agricultural revolution, it remains obscure about their environmental fate and bioavailability by plants. Fungal laccase-mediated biotransformation of carbon nanomaterials has received little attention despite its known capacity to eliminate recalcitrant contaminants. Herein, we presented the initial investigation into the transformation of CDs by fungal laccase. The degradation rates of CDs were determined to be first-order in both substrate and enzyme. Computational docking studies showed that CDs preferentially bonded to the pocket of laccase on the basal plane rather than the edge through hydrogen bonds and hydrophobic interactions. Electrospray ionization-Fourier transform-ion cyclotron resonance mass spectrometry (ESI-FT-ICR MS) and other characterizations revealed that the phenolic/amino lignins and tannins portions in CDs are susceptible to laccase transformation, resulting in graphitic structure damage and smaller-sized fragments. By using the
13 C stable isotope labeling technique, we quantified the uptake and translocation of13 C-CDs by mung bean plants.13 C-CDs (10 mg L-1 ) accumulated in the root, stem, and leaf were estimated to be 291, 239, and 152 μg g-1 at day 5. We also evidenced that laccase treatment alters the particle size and surface chemistry of CDs, which could facilitate the uptake of CDs by plants and reduce their nanotoxicity to plants.- Published
- 2023
- Full Text
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25. Reduction-Active Antisolvent: A Universal and Innovative Strategy of Further Ameliorating Additive Optimization for High Efficiency Perovskite Solar Cells.
- Author
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Chen WH, Chen W, Zhang P, Li Y, Ye W, Ning L, Du P, Song L, Xiong J, and Lu W
- Abstract
To further ameliorate current additive engineering of perovskites for viable applications, the inherent limitations should be overcome; these include weakened coordination of the dopants to the [PbI
6 ]4- octahedra during crystallization and ubiquity of ineffective bonding sites. Herein, we introduce a facile strategy for synthesizing a reduction-active antisolvent. Washing with reduction-active PEDOT:PSS-blended antisolvent substantially enhances the intrinsic polarity of the Lewis acid (Pb2+ ) in [PbI6 ]4- octahedra, which causes significant strengthening of the coordinate bonding between additives and perovskite. Thus, coordination of the additive to the perovskite becomes much stable. Additionally, the enhanced coordination ability of Pb2+ can enhance the effective bonding sites and further enhance the efficacy of additive optimization to the perovskite. Here, we demonstrate five different additives as dopant bases and repeatedly verify the universality of this approach. The photovoltaic performance and stability of doped-MAPbI3 devices are further improved, revealing the advanced potential of additive engineering.- Published
- 2023
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26. Iodine-Mediated α-C-H Amination of Carbonyl Compounds via Nitrogen-Directed Oxidative Umpolung.
- Author
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Wang M, Yi X, Ye W, Shi Q, Yu W, and Chang J
- Subjects
- Amination, Oxidation-Reduction, Oxidative Stress, Nitrogen chemistry, Iodine
- Abstract
A new synthetic strategy for direct C( sp
3 )-H amination of carbonyl compounds at their α-carbon has been established employing molecular iodine and nitrogen-directed oxidative umpolung. In this transformation, iodine acts not only as an iodinating reagent but also as a Lewis acid catalyst, and both the nitrogen-containing moiety and the carbonyl group in the substrate play important roles. This synthetic approach is applicable to a broad variety of carbonyl substrates, including esters, ketones, and amides. Its features also include no requirement for transition metals, mild reaction conditions, short reaction times, and gram-scale synthesis.- Published
- 2023
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27. Wound-Healing Material with Antibacterial and Antioxidant Functions, Constructed Using Keratin, Hyperbranched Polymers, and MnO 2 .
- Author
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Lu Y, Ye W, Kang W, Wang S, Zhu Z, Chen X, and Li J
- Subjects
- Animals, Humans, Antioxidants pharmacology, Antioxidants chemistry, Escherichia coli, Staphylococcus aureus, Reactive Oxygen Species, Manganese Compounds pharmacology, Oxides pharmacology, Hydrogels pharmacology, Hydrogels chemistry, Wound Healing, Anti-Bacterial Agents pharmacology, Anti-Bacterial Agents chemistry, Keratins, Polymers pharmacology, Polymers chemistry
- Abstract
Wound healing, a global medical issue, poses a substantial financial burden. Therefore, developing low-cost and highly efficacious wound-healing materials is essential. In this study, we prepared keratin-hyperbranched polymer hydrogel-M (KHBP-M), a multifunctional composite gel, by mixing reduced keratin containing free sulfhydryl groups extracted from human hair waste, hyperbranched polymer (HBP) with double bonds at the end, and MnO
2 nanoparticles prepared using the biological template method. Keratin has intrinsic wound-healing properties, and MnO2 is a wound-healing material with both photothermal antibacterial and reactive oxygen species (ROS)-scavenging abilities. KHBP-M showed antibacterial effects against both Gram-positive ( Staphylococcus aureus ) and Gram-negative ( Escherichia coli ) bacteria. When exposed to irradiation (808 nm), the killing ratio for S. aureus reached 99.99%, which is especially suitable for wound environments. A similar trend was noted for E. coli . The composite hydrogel also showed excellent ROS-scavenging ability and could resist oxidative stress in L929 cells. Furthermore, in an animal model of infected wounds, the KHBP-M hydrogel treated with near-infrared light had the fastest wound-healing rate, reaching 82.98% on day 15. Our study provides a promising wound-healing material, with simple preparation methods, easy access to sources, and low cost involved.- Published
- 2023
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28. Metabolic Footprinting-Based DNA-AuNP Encoders for Extracellular Metabolic Response Profiling.
- Author
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Qi G, Zou H, Peng X, He S, Zhang Q, Ye W, Jiang Y, Wang W, Ren G, and Qu X
- Subjects
- DNA, Metabolomics, Cell Culture Techniques
- Abstract
Metabolic footprinting as a convenient and non-invasive cell metabolomics strategy relies on monitoring the whole extracellular metabolic process. It covers nutrient consumption and metabolite secretion of in vitro cell culture, which is hindered by low universality owing to pre-treatment of the cell medium and special equipment. Here, we report the design and a variety of applicability, for quantifying extracellular metabolism, of fluorescently labeled single-stranded DNA (ssDNA)-AuNP encoders, whose multi-modal signal response is triggered by extracellular metabolites. We constructed metabolic response profiling of cells by detecting extracellular metabolites in different tumor cells and drug-induced extracellular metabolites. We further assessed the extracellular metabolism differences using a machine learning algorithm. This metabolic response profiling based on the DNA-AuNP encoder strategy is a powerful complement to metabolic footprinting, which significantly applies potential non-invasive identification of tumor cell heterogeneity.
- Published
- 2023
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29. Robust Acute Pancreatitis Identification and Diagnosis: RAPIDx.
- Author
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Zhu Q, Luo J, Li HP, Ye W, Pan R, Shi KQ, Yang R, Xu H, Li H, Lee LP, and Liu F
- Subjects
- Humans, Acute Disease, Serum Amyloid A Protein genetics, Serum Amyloid A Protein metabolism, Proteomics, Pancreatitis diagnosis
- Abstract
The occurrence of acute pancreatitis (AP) is increasing significantly worldwide. However, current diagnostic methods of AP do not provide a clear clinical stratification of severity, and the prediction of complications in AP is still limited. Here, we present a robust AP identification and diagnosis (RAPIDx) method by the proteomic fingerprinting of intact nanoscale extracellular vesicles (EVs) from clinical samples. By tracking analysis of circulating biological nanoparticles released by cells ( i.e. , EVs) via bottom-up proteomics, we obtain close phenotype connections between EVs, cell types, and multiple tissues based on their specific proteomes and identify the serum amyloid A (SAA) proteins on EVs as potential biomarkers that are differentially expressed from AP patients significantly. We accomplish the quantitative analysis of EVs fingerprints using MALDI-TOF MS and find the SAA proteins (SAA1-1, desR-SAA1-2, SAA2, SAA1-2) with areas under the curve (AUCs) from 0.92 to 0.97, which allows us to detect AP within 30 min. We further realize that SAA1-1 and SAA2, combined with two protein peaks (5290.19, 14032.33 m / z ), can achieve an AUC of 0.83 for classifying the severity of AP. The RAPIDx platform will facilitate timely diagnosis and treatment of AP before severity development and persistent organ failure and promote precision diagnostics and the early diagnosis of pancreatic cancer.
- Published
- 2023
- Full Text
- View/download PDF
30. Integrated Transcriptomic and Metabolomic Analyses Reveal the Molecular and Metabolic Basis of Flavonoids in Areca catechu L.
- Author
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Lai J, Li C, Zhang Y, Wu Z, Li W, Zhang Z, Ye W, Guo H, Wang C, Long T, Wang S, and Yang J
- Subjects
- Areca chemistry, Flavonoids metabolism, Gene Expression Profiling, Gene Expression Regulation, Plant, Transcriptome, Catechin metabolism
- Abstract
Areca catechu L., of the Arecaceae family, is widely distributed in tropical Asia. In A. catechu , the extracts and compounds, including flavonoids, have various pharmacological activities. Although there are many studies of flavonoids, the molecular mechanism of their biosynthesis and regulation remains unclear in A. catechu . In this study, 331 metabolites were identified from the root, stem, and leaf of A. catechu using untargeted metabolomics, including 107 flavonoids, 71 lipids, 44 amino acids and derivatives, and 33 alkaloids. The transcriptome analysis identified 6119 differentially expressed genes, and some were enriched in the flavonoid pathway. To analyze the biosynthetic mechanism of the metabolic differences in A. catechu tissues, 36 genes were identified through combined transcriptomic and metabolomic analysis, in which glycosyltransferase genes Acat_15g017010 and Acat_16g013670 were annotated as being involved in the glycosylation of kaempferol and chrysin by their expression and in vitro activities. Flavonoid biosynthesis could be regulated by the transcription factors, AcMYB5 and AcMYB194 . This study laid a foundation for further research on the flavonoid biosynthetic pathway of A. catechu .
- Published
- 2023
- Full Text
- View/download PDF
31. In Situ Prepared Three-Dimensional Covalent and Hydrogen Bond Synergistic Binder to Boost the Performance of SiO x Anodes for Lithium-Ion Batteries.
- Author
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Long J, He W, Liao H, Ye W, Dou H, and Zhang X
- Abstract
Polymer binders play an important role in enhancing the electrochemical performance of silicon-based anodes to alleviate the volume expansion for lithium-ion batteries. It is difficult for common one-dimensional (1D) linear binders to limit the volume expansion of a silicon-based electrode when combined with silicon-based particles with scant binding points. Therefore, it is necessary to design a three-dimensional (3D) network structure, which has multiple binding points with the silicon particles to dissipate the mechanical stress in the continuous charge and discharge circulation. Here, a covalent and hydrogen bond synergist 3D network green binder (poly(acrylic acid) (PAA)-dextrin 9 (Dex
9 )) was prepared by the simple in situ thermal condensation of a one-dimensional liner binder PAA and Dex in the electrode fabrication process. The optimized SiOx @PAA-Dex9 electrode exhibits an initial Coulombic efficiency (ICE) of 82.4% at a current density of 0.2 A g-1 . At a high current density of 1 A g-1 , it retains a capacity of 607 mAh g-1 after 300 cycles, which is approximately twice as high as that of the SiOx @PAA electrode. Furthermore, the results of in situ electrochemical dilatometry (ECD) and characterization of electrode structures demonstrate that the PAA-Dex9 binder can effectively buffer the huge volume change and maintain the integrity of the SiOx electrodes. The research overcomes the low electrochemical stability difficulty of the 3D binder and sheds light on developing the simple fabrication procedure of an electrode.- Published
- 2023
- Full Text
- View/download PDF
32. Sm-Doped PIN-PMN-PT Transparent Ceramics with High Curie Temperature, Good Piezoelectricity, and Excellent Electro-Optical Properties.
- Author
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Zheng F, Tian X, Fang Z, Lin J, Lu Y, Gao W, Xin R, Fu D, Qi Y, Ma Z, Ye W, Qin Y, Wang X, and Zhang Y
- Abstract
Transparent piezoelectric materials are capable of coupling several physical effects such as optics, acoustics, electricity, and mechanical deformation together, which expands applications for mechanical-electro-optical multifunctional devices. However, piezoelectricity, transparency, and Curie temperature restrict each other, so it is difficult to achieve high piezoelectricity with both good transparency and a high Curie point. In this paper, Sm-doped 24Pb(In
1/2 Nb1/2 )O3 -42Pb(Mg1/3 Nb2/3 )O3 -34PbTiO3 (PIN-PMN-PT) transparent ceramic with a high piezoelectric coefficient of 905 pC/N, excellent electro-optical coefficient of 814 pm/V, and high Curie-point of 179 °C is fabricated. Sm doping effect on the phase structures, piezoelectricity, ferroelectricity, optical transparency, electro-optical properties, and thermal stability is systematically investigated. Compared with PMN-PT transparent ceramics, PIN-PMN-PT transparent ceramics exhibit better temperature stability. Electro-optical modulation and energy conversion are achieved using PIN-PMN-PT transparent piezoelectric ceramic, which indicates that it has great potential to develop mechanical-electrical-optical multifunctional coupling devices for optical communication, energy harvesting, photoacoustic imaging, and so on.- Published
- 2023
- Full Text
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33. Synthesis of Quinazolinone-Fused Tetrahydroisoquinolines and Related Polycyclic Scaffolds by Iodine-Mediated sp 3 C-H Amination.
- Author
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Wang M, Ye W, Sun N, Yu W, and Chang J
- Abstract
An iodine-mediated intramolecular sp
3 C-H amination reaction producing quinazolinone-fused polycyclic skeletons from 2-aminobenzamide precursors is reported. This reaction does not use transition metals, has a broad substrate scope, and can be used on a gram scale. Under the optimal reaction conditions, a variety of quinazolinone-fused tetrahydroisoquinolines and derivatives of Rutaecarpine were synthesized from readily accessible compounds. The reaction proceeds well with crude 2-aminobenzamide derivatives, allowing for the synthesis of the products from simple 2-aminobenzoic acids and tetrahydroisoquinolines without purification of the 2-aminobenzamide intermediates. Preliminary biological experiments have identified Cereblon (CRBN) inhibitory activity and relevant anti-myeloma medicinal properties in some of these polycyclic products.- Published
- 2023
- Full Text
- View/download PDF
34. Moisture-Insensitive and Highly Selective Detection of NO 2 by Ion-in-Conjugation Covalent Organic Frameworks.
- Author
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Wang J, Cao Q, Cheng XF, Ye W, He JH, and Lu JM
- Subjects
- Humans, Nitrogen Dioxide, Adsorption, Hydrogen Bonding, Gases, Metal-Organic Frameworks
- Abstract
As a common toxic gas, nitrogen dioxide (NO
2 ) seriously threatens the environment and human respiratory system even at part per billion (ppb) level. Covalent organic frameworks (COFs) have gained widespread attention in sensing applications because of the benefits of designability, environmental stability, and a large number of active sites. However, the competitive adsorption of water molecules and the target gas molecules at room temperature as well as the weak interaction between COFs and gas molecules hinder their practical applications. Here, we introduce ion-in-conjugation (IIC) into a covalent organic framework (COF) by preparing a condensate of squaraine (SA) with 1,3,5-tris(4-aminophenyl)benzene (TAPB) to form a mesoporous macrocyclic material (SA-TAPB). Layers of SA-TAPB, drop cast onto interdigitated Ag-Pd alloy electrodes, show a statistically significant conductivity response to NO2 at concentrations as low as 30 ppb and a theoretical detection limit of 10.9 ppb. The sensor displays a lower sensitivity to variations in humidity when operated at 80 °C compared to room temperature. The density functional theory (DFT) calculations indicated that the main adsorption site of NO2 is dual hydrogen bonds formed between two amide hydrogen atoms of SA-TAPB and the NO2 molecule. Gas adsorption experiments revealed that SA-TAPB has the largest adsorption capacity of NO2 versus other interference gases, which were responsible for the excellent selectivity toward NO2 .- Published
- 2022
- Full Text
- View/download PDF
35. Ultralong Organic Phosphorescence: From Material Design to Applications.
- Author
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Shi H, Yao W, Ye W, Ma H, Huang W, and An Z
- Abstract
Organic phosphorescence is defined as a radiative transition between the different spin multiplicities of an organic molecule after excitation; here, we refer to the photoexcitation. Unlike fluorescence, it shows a long emission lifetime (∼μs), large Stokes shift, and rich excited state properties, attracting considerable attention in organic electronics during the past years. Ultralong organic phosphorescence (UOP), a type of persistent luminescence in organic phosphors, shows an emission lifetime of over 100 ms normally according to the resolution limit of the naked eye. According to the Jablonski energy diagram, two prerequisites are necessary for UOP generation and enhancement. One is to promote intersystem crossing (ISC) of the excitons from the excited singlet to triplet states by enhancing the spin-orbit coupling (SOC); the other is to suppress the nonradiative transitions of the excitons from the excited triplet states.In this Account, we will give a summary of our research on ultralong organic phosphorescence, including the design of materials, manipulation of properties, fabrication of nano/microstructures, and function applications. First, we give a brief introduction to the UOP development. Then, we discuss the constructed methods of UOP materials from the inter/intramolecular interaction types, including π-π interactions, intermolecular hydrogen bonds, halogen bonds, ionic bonds, covalent bonds, and so on. These effective interactions can build a rigid environment to restrain the nonradiative transitions from the molecular motions or external quenching by oxygen, moisture, or heat, and thus enhance the UOP performance. Next, the manipulation of UOP properties, containing excitation wavelength, emission colors, lifetimes, and quantum efficiency (QE), through molecular or crystal engineering will be summarized. Recently, the excitation wavelengths of the materials for UOP can be regulated in different regions, such as UV, visible light, and X-ray; the emission colors of UOP can cover the whole visible-light region, from deep blue to red; the phosphorescence lifetime of UOP materials can reach 2.5 s, and the quantum efficiency can be achieved up to 96.5%. Moreover, we will present the fabrication of micro/nanoscale UOP materials, including the preparation of micro/nanostructure, optical performance, and device fabrication. Afterward, we will review the potential applications of UOP materials in organic/bio-optoelectronics, such as information encryption, bioimaging, sensing, afterglow display, etc . Finally, an outlook on the development of UOP materials and applications will be proposed.
- Published
- 2022
- Full Text
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36. Selective C9orf72 G-Quadruplex-Binding Small Molecules Ameliorate Pathological Signatures of ALS/FTD Models.
- Author
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Cheng A, Liu C, Ye W, Huang D, She W, Liu X, Fung CP, Xu N, Suen MC, Ye W, Sung HHY, Williams ID, Zhu G, and Qian PY
- Subjects
- Animals, C9orf72 Protein genetics, C9orf72 Protein metabolism, DNA, Drosophila, Ligands, RNA genetics, Reactive Oxygen Species, Amyotrophic Lateral Sclerosis drug therapy, Amyotrophic Lateral Sclerosis genetics, Amyotrophic Lateral Sclerosis metabolism, Biological Products, Frontotemporal Dementia drug therapy, Frontotemporal Dementia genetics, Frontotemporal Dementia metabolism
- Abstract
The G-quadruplex (G4) forming C9orf72 GGGGCC (G4C2) expanded hexanucleotide repeat (EHR) is the predominant genetic cause of amyotrophic lateral sclerosis (ALS) and frontotemporal dementia (FTD). Developing selective G4-binding ligands is challenging due to the conformational polymorphism and similarity of G4 structures. We identified three first-in-class marine natural products, chrexanthomycin A ( cA ), chrexanthomycin B ( cB ), and chrexanthomycin C ( cC ), with remarkable bioactivities. Thereinto, cA shows the highest permeability and lowest cytotoxicity to live cells. NMR titration experiments and in silico analysis demonstrate that cA , cB , and cC selectively bind to DNA and RNA G4C2 G4s. Notably, cA and cC dramatically reduce G4C2 EHR-caused cell death, diminish G4C2 RNA foci in (G4C2)
29 -expressing Neuro2a cells, and significantly eliminate ROS in HT22 cells. In (G4C2)29 -expressing Drosophila , cA and cC significantly rescue eye degeneration and improve locomotor deficits. Overall, our findings reveal that cA and cC are potential therapeutic agents deserving further clinical study.- Published
- 2022
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37. Regulating Surface Wettability and Charge Density of Porous Carbon Particles by In Situ Growth of Polyaniline for Constructing an Efficient Electrical Percolation Network in Flow-Electrode Capacitive Deionization.
- Author
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Xiong J, Zhu Z, Ye W, Mu L, Lu X, and Zhu J
- Abstract
Both electrical conductivity and surface wettability are required for the selection of active carbon materials in flow-electrode capacitive deionization, while a trade-off exists between these two properties. In this work, a hybrid material with a thin layer of polyaniline (PANI) coating on activated carbon (AC/PANI) was successfully developed to retain excellent electrical conductivity and acquire good surface wettability. By adjusting the dosage of initiator, AC/PANI composites with different loading fractions of PANI were obtained. The electrochemical testing demonstrated that the AC/PANI composites have higher specific capacitance and lower ion diffusion resistance compared to pure AC, resulting in better desalinization performance. Specifically, with a feed concentration of 1600 mg/L, excellent adsorption capacity and high charge efficiency can be simultaneously achieved at 13.51 mg/g and 92.21%, respectively. Benefiting from the formation of a continuous electrical percolation network and reduced solid/liquid interfacial transport resistance, a 39% enhancement of average salt adsorption rate (from 0.54 to 0.75 μmol/min/cm
2 ) was obtained.- Published
- 2022
- Full Text
- View/download PDF
38. Enhanced Cyclability of Lithium Metal Anodes Enabled by Anti-aggregation of Lithiophilic Seeds.
- Author
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Sun J, Cheng Y, Zhang H, Yan X, Sun Z, Ye W, Li W, Zhang M, Gao H, Han J, Peng DL, Yang Y, and Wang MS
- Subjects
- Carbon, Electrodes, Lithium, Seeds
- Abstract
Constructing 3D skeletons modified with lithiophilic seeds has proven effective in achieving dendrite-free lithium metal anodes. However, these lithiophilic seeds are mostly alloy- or conversion-type materials, and they tend to aggregate and redistribute during cycling, resulting in the failure of regulating Li deposition. Herein, we address this crucial but long-neglected issue by using intercalation-type lithiophilic seeds, which enable antiaggregation owing to their negligible volume expansion and high electrochemical stability against Li. To exemplify this, a 3D carbon-based host is built, in which ultrafine TiO
2 seeds are uniformly embedded in nitrogen-doped hollow porous carbon spheres (N-HPCSs). The TiO2 @N-HPCSs electrode exhibits superior Coulombic efficiency, high-rate capability, and long-term stability when evaluated as compertitive anodes for Li metal batteries. Furthermore, the superiority of intercalation-type seeds is comprehensively revealed through controlled experiments by various in situ/ex situ electron and optical microscopies, which highlights the excellent structural stability and lithiophilicity of TiO2 nanoseeds upon repeated cycling.- Published
- 2022
- Full Text
- View/download PDF
39. Microheater Integrated Nanotube Array Gas Sensor for Parts-Per-Trillion Level Gas Detection and Single Sensor-Based Gas Discrimination.
- Author
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Tang W, Chen Z, Song Z, Wang C, Wan Z, Chan CLJ, Chen Z, Ye W, and Fan Z
- Subjects
- Humans, Limit of Detection, Electronic Nose, Heating, Gases, Nanotubes, Carbon
- Abstract
Real-time monitoring of health threatening gases for chemical safety and human health protection requires detection and discrimination of trace gases with proper gas sensors. In many applications, costly, bulky, and power-hungry devices, normally employing optical gas sensors and electrochemical gas sensors, are used for this purpose. Using a single miniature low-power semiconductor gas sensor to achieve this goal is hardly possible, mostly due to its selectivity issue. Herein, we report a dual-mode microheater integrated nanotube array gas sensor (MINA sensor). The MINA sensor can detect hydrogen, acetone, toluene, and formaldehyde with the lowest measured limits of detection (LODs) as 40 parts-per-trillion (ppt) and the theoretical LODs of ∼7 ppt, under the continuous heating (CH) mode, owing to the nanotubular architecture with large sensing area and excellent surface catalytic activity. Intriguingly, unlike the conventional electronic noses that use arrays of gas sensors for gas discrimination, we discovered that when driven by the pulse heating (PH) mode, a single MINA sensor possesses discrimination capability of multiple gases through a transient feature extraction method. These above features of our MINA sensors make them highly attractive for distributed low-power sensor networks and battery-powered mobile sensing systems for chemical/environmental safety and healthcare applications.
- Published
- 2022
- Full Text
- View/download PDF
40. Extraordinary Antiwear Properties of Graphene-Reinforced Ti Composites Induced by Interfacial Decoration.
- Author
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Yan Q, Chen B, Ye W, Wan J, Zhang T, Kou H, Zhou Q, Lu W, Wang H, Shen J, Wang H, and Li J
- Abstract
The expected excellent lubricant effect of graphene in metals during friction and wear is rarely achieved because of the difficulty in synthesizing suitable interfaces. Particularly, the situation is more challenging in titanium (Ti) matrix composites (TMCs) because of the high chemical-interface-reaction tendency between graphene and Ti during composite fabrication. In this study, few-layered graphene (FLG) decorated with SiC nanoparticles (SiCp) was synthesized as reinforcement in Ti-6Al-4V alloy to improve the interface of the composites. It was found that interfacial SiCp not only strengthened the interface bonding by the Si solid solution but also inhibited the chemical reaction between FLG and the Ti matrix with reduced sp
3 defects. The composite with 30 wt % SiC-decorated FLG showed an 86.8% decrement in wear rate compared to the unreinforced matrix, resulting in exceptionally high antiwear enhancing efficiency, which was around fourfold of the available values of other TMCs in the literature. The antiwear mechanism was investigated by thorough characterization of the interfaces and microstructures of the composites. The idea of interfacial decoration can be potentially applied to other nanocarbon/metal composites with the advantages of retaining the function performance of nanocarbon materials.- Published
- 2022
- Full Text
- View/download PDF
41. Dinuclear Organoruthenium Complex for Mitochondria-Targeted Near-Infrared Imaging and Anticancer Therapy to Overcome Platinum Resistance.
- Author
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Wang J, Zhang Y, Li Y, Li E, Ye W, and Pan J
- Subjects
- Cell Line, Tumor, Cell Proliferation, Cisplatin pharmacology, DNA chemistry, Humans, Ligands, Mitochondria, Molecular Docking Simulation, Platinum pharmacology, Reactive Oxygen Species metabolism, Antineoplastic Agents chemistry, Antineoplastic Agents pharmacology, Coordination Complexes chemistry, Coordination Complexes pharmacology, Lung Neoplasms, Ruthenium chemistry, Ruthenium pharmacology
- Abstract
New mononuclear and dinuclear Ru(II) coordination compounds with the 2,7-bisbenzoimidazolyl-naphthyridine ligand have been synthesized and characterized by UV-vis, NMR, and MALDI-TOF. The molecular structures for Ru(II) compounds were determined by single-crystal X-ray diffraction. With the expansion of ligand π-conjugation and the increase in the complexed Ru number, the maximum emission wavelength red-shifted from 696 to 786 nm. The binding mode between complexes and DNA was predicted by molecular docking, which is intercalations and π-π stacking interactions with the surrounding bases. The intercalation mode of DNA binding was then determined by DNA titration and ethidium bromide (EB) displacement experiments. The antigrowth effects of complexes RuY , RuY1 , and RuY2 were tested in HaCat (normal cells), HeLa (cervical cancer), A549 (lung cancer), and A549/DDP (cisplatin-resistant lung cancer) through the MTT assay. The dinuclear complex RuY2 was superior to mononuclear complexes and cisplatin in the cisplatin-resistant cell line. Confocal imaging proved that the subcellular localization of Ru(II) complexes was mitochondria; moreover, apoptosis was detected by flow cytometry. All three complexes showed a dose-dependent manner in all four cell lines. All Ru(II) complexes were found to have reactive oxygen species (ROS). The finding indicated that these Ru(II) complexes caused cell death by both DNA disruption and ROS. This study helps to explore the potential of the polynuclear Ru(II) complexes for the combination of NIR imaging and Pt-resistant cancer therapy.
- Published
- 2022
- Full Text
- View/download PDF
42. Structural Exploration of Polycationic Nanoparticles for siRNA Delivery.
- Author
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Yan Y, Zhang G, Wu C, Ren Q, Liu X, Huang F, Cao Y, and Ye W
- Subjects
- Cations, Hydrophobic and Hydrophilic Interactions, Polymers, RNA, Small Interfering genetics, Methacrylates chemistry, Nanoparticles chemistry
- Abstract
RNA interference (RNAi) is a promising approach to the treatment of genetic diseases by the specific knockdown of target genes. Functional polymers are potential vehicles for the effective delivery of vulnerable small interfering RNA (siRNA), which is required for the broad application of RNAi-based therapeutics. The development of methods for the facile modulation of chemical structures of polymeric carriers and an elucidation of detailed delivery mechanisms remain important areas of research. In this paper, we synthesized a series of methacrylate-based polymers with controllable structures and narrow distributions by atom transfer radical polymerization using various combinations of cationic monomers (2-dimethylaminoethyl methacrylate, 2-diethylaminoethyl methacrylate, and 2-dibutylaminoethyl methacrylate) and hydrophobic monomers (2-butyl methacrylate (BMA), cyclohexyl methacrylate, and 2-ethylhexyl methacrylate). These polymers exhibited varying hydrophobicities, charge densities, and p K
a values, enabling the discovery of effective carriers for siRNA by in vitro delivery assays. For the polymers with BMA segments, 50% of cationic segments were beneficial to the formation of siRNA nanoparticles (NPs) and the in vitro delivery of siRNA. The optimal ratio varied for different combinations of cationic and hydrophobic segments. In particular, 20k PMB 0.5, PME 0.5, and PEB 1.0 showed >75% luciferase knockdown. Efficacious delivery was dependent on high siRNA binding, the small size of NPs, and balanced hydrophobicity and charge density. Cellular uptake and endosomal escape experiments indicated that carboxybetaine modification of 20k PMB 0.5 did not remarkably affect the internalization of corresponding NPs after incubation for 6 h but significantly reduced the endosomal escape of NPs, which leads to the notable decrease in delivery efficacy of polymers. These results provide insights into the mechanism of polymer-based siRNA delivery and may inspire the development of novel polymeric carriers.- Published
- 2022
- Full Text
- View/download PDF
43. PRMT8 Attenuates Cerebral Ischemia/Reperfusion Injury via Modulating Microglia Activation and Polarization to Suppress Neuroinflammation by Upregulating Lin28a.
- Author
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Zheng K, Zhang Y, Zhang C, Ye W, Ye C, Tan X, and Xiong Y
- Subjects
- Animals, Infarction, Middle Cerebral Artery metabolism, Mice, Microglia, Neuroinflammatory Diseases, Brain Ischemia metabolism, Protein-Arginine N-Methyltransferases metabolism, Reperfusion Injury metabolism, Stroke
- Abstract
Activation and polarization of microglia are involved in neuroinflammation and regulate ischemic stroke-associated brain injury. Protein arginine methyltransferase 8 functions as a regulatory component of hypoxic stress-induced neuroinflammation. The protective effect of protein arginine methyltransferase 8 (PRMT8) against ischemic stroke-associated brain injury through regulation of microglia activation and polarization was investigated. First, PRMT8 was downregulated in middle cerebral artery occlusion (MCAO)-induced mice and oxygen-glucose deprivation/reoxygenation (OGD/R)-induced SH-SY5Y. Injection with AAV-PRMT8 reduced infarct volumes in MCAO-induced mice. Moreover, injection with AAV-PRMT8 promoted neuronal survival and ameliorated histopathological changes in the brains of MCAO-induced mice. The neuronal apoptosis and neuroinflammation in MCAO-induced mice were suppressed by AAV-PRMT8 injection. Second, PRMT8 overexpression increased cell viability and suppressed the cell apoptosis and inflammation of OGD/R-induced SH-SY5Y. Third, injection with AAV-PRMT8 reduced almost 50% of CD86 + M1 microglia and enhanced about 20% of CD206 + M2 microglia. Furthermore, PRMT8 overexpression attenuated OGD/R-induced M1 phenotype polarization of BV2. Lastly, PRMT8 upregulated Lin28a and loss of Lin28a attenuated PRMT8 overexpression-induced increase in cell viability and decrease in cell apoptosis and inflammation of OGD/R-induced SH-SY5Y. In conclusion, PRMT8 promoted M2 phenotype polarization of microglia and suppressed neuronal apoptosis to ameliorate cerebral ischemia/reperfusion injury through upregulation of Lin28a.
- Published
- 2022
- Full Text
- View/download PDF
44. Cry3Aa*SpyCatcher Fusion Crystals Produced in Bacteria as Scaffolds for Multienzyme Coimmobilization.
- Author
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Sun Q, Heater BS, Li TL, Ye W, Guo Z, and Chan MK
- Subjects
- Bacterial Proteins genetics, Endotoxins, Hemolysin Proteins, Bacillus thuringiensis genetics, Bacillus thuringiensis Toxins
- Abstract
The production of Cry3Aa enzyme fusion crystals in Bacillus thuringiensis provides a direct method to immobilize individual enzymes and thereby improve their stability and recyclability. Nevertheless, many reactions require multiple enzymes to produce a desired product; thus a general strategy was developed to extend our Cry3Aa technology to multienzyme coimmobilization. Here, we report the direct production of particles comprising a modified Cry3Aa (Cry3Aa*) fused to SpyCatcher002 (Cry3Aa*SpyCat2) for coimmobilization of model enzymes MenF, MenD, and MenH associated with the biosynthesis of menaquinone. The resultant coimmobilized particles showed improved reaction rates compared to free enzymes presumably due to the higher local enzyme substrate concentrations and enhanced enzyme coupling made possible by colocalization. Furthermore, coimmobilization of these enzymes on Cry3Aa*SpyCat2 led to increased thermal stability and recyclability of the overall multienzyme system. These characteristics together with its overall simplicity of production highlight the benefits of Cry3Aa*SpyCat2 crystals as a platform for enzyme coimmobilization.
- Published
- 2022
- Full Text
- View/download PDF
45. Discovery of Benzocyclic Sulfone Derivatives as Potent CXCR2 Antagonists for Cancer Immunotherapy.
- Author
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Dong Y, Fu R, Chen J, Zhang K, Ji M, Wang M, Jiang H, Ye W, Hu J, Li Y, Jin J, Chen X, and Xu H
- Subjects
- Antineoplastic Agents chemistry, Humans, Immunosuppressive Agents chemistry, Immunotherapy, Sulfones chemistry, Tumor Microenvironment, Antineoplastic Agents pharmacology, Immunosuppression Therapy, Immunosuppressive Agents pharmacology, Neoplasms drug therapy, Receptors, Interleukin-8B antagonists & inhibitors, Sulfones pharmacology
- Abstract
Increasing evidence shows that the CXC chemokine receptor 2 (CXCR2) signaling pathway is essentially implicated in the recruitment of myeloid-derived suppressor cells (MDSCs) to the tumor microenvironment and leads to MDSC-mediated immune suppression. Therefore, CXCR2 has recently emerged as a promising drug target for cancer immunotherapy. In this paper, benzocyclic sulfone derivatives were designed as potent CXCR2 antagonists. Structure-activity relationship studies resulted in two lead compounds 9b and 11h , which demonstrated double-digit nanomolar potencies against CXCR2 and significantly inhibited neutrophil infiltration into the air pouch in an in vivo setting. More importantly, 9b and 11h dose-dependently inhibited the tumor growth through oral administration in the Pan02 mouse model. Further cytometry and immunohistochemical analyses revealed that 9b and 11h could reduce the infiltration of neutrophils and MDSCs and enhance the infiltration of CD3
+ T lymphocytes into the Pan02 tumor tissues, shedding light on their mechanisms of action in cancer immunotherapy.- Published
- 2021
- Full Text
- View/download PDF
46. Design and Characterization of Self-Lubricating Refractory High Entropy Alloy-Based Multilayered Films.
- Author
-
Luo D, Zhou Q, Ye W, Ren Y, Greiner C, He Y, and Wang H
- Abstract
Refractory high entropy alloys (RHEAs) have been proven to have excellent mechanical properties with a potential use as protective thin films. However, the combination of high hardness with low friction and wear is a major challenge in the design of RHEA films. In this study, we show that NbMoWTa/Ag self-lubricating multilayered films give a remarkable reduction in friction and at same time maintain high hardness. Interestingly, it is found that the bcc superlattice dominates in both NbMoWTa and Ag layers and the interfaces become coherent when the individual layer thickness h is reduced below 10 nm. The film properties are then strongly dependent on h ranging from 100 to 2.5 nm, and the most promising properties are obtained when the interface structure transforms from incoherent to coherent one. Especially, the multilayer with h = 2.5 nm exhibits superior tribological performance over monolithic NbMoWTa due to the significant coherent strengthening along with the self-lubricating ability in the multilayer. This tailored phase transition and coherent structure between the matrix and lubrication phases can also provide an optimal wear rate-coefficient of friction combination, which is higher than most of the Ag-containing self-lubricating films. The current work might open a new route toward the development of innovative self-lubricating RHEA films with excellent tribological properties.
- Published
- 2021
- Full Text
- View/download PDF
47. Circularly Polarized Organic Room Temperature Phosphorescence from Amorphous Copolymers.
- Author
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Gu L, Ye W, Liang X, Lv A, Ma H, Singh M, Jia W, Shen Z, Guo Y, Gao Y, Chen H, Wang D, Wu Y, Liu J, Wang H, Zheng YX, An Z, Huang W, and Zhao Y
- Abstract
Organic optoelectronic functional materials featuring circularly polarized emission and persistent luminescence represent a novel research frontier and show promising applications in data encryption, displays, biological imaging, and so on. Herein, we present a simple and universal approach to achieve circularly polarized organic phosphorescence (CPP) from amorphous copolymers by the incorporation of axial chiral chromophores into polymer chains via radical cross-linked polymerization. Our experimental data reveal that copolymers ( R / S )-PBNA exhibit a maximum CPP efficiency of 30.6% and the largest dissymmetric factor of 9.4 × 10
-3 and copolymers ( R / S )-PNA show the longest lifetime of 0.68 s under ambient conditions. Given the CPP property of these copolymers, their potential applications in multiple information encryption and displays are demonstrated, respectively. These findings not only lay the foundation for the development of amorphous polymers with superior CPP but also expand the outlook of room-temperature phosphorescent materials.- Published
- 2021
- Full Text
- View/download PDF
48. Divergent S- and C-Difluoromethylation of 2-Substituted Benzothiazoles.
- Author
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Wang X, Ye W, Kong T, Wang C, Ni C, and Hu J
- Abstract
Two unprecedented and complementary synthetic strategies for S- and C-difluoromethylation of 2-substituted benzothiazoles have been developed by taking advantage of the remarkably different reactivity of CF
2 H- and 2-PySO2 CF2 - nucleophiles. A variety of structurally diverse difluoromethyl 2-isocyanophenyl sulfides and 2-difluoromethylated benzothiazoles were synthesized with these two new synthetic protocols.- Published
- 2021
- Full Text
- View/download PDF
49. Lead-Free Halide Cs 2 PtI 6 Perovskite Favoring Pt-N Bonding for Trace NO Detection.
- Author
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Chen ZK, Ye W, Lin HZ, Yu C, He JH, and Lu JM
- Subjects
- Oxides, Titanium, Calcium Compounds, Nitric Oxide
- Abstract
In recent years, the performance research of perovskite materials is not only concentrated in the field of solar cells or optics, but the field of gas sensing has gradually entered the public view. However, the detection of nitric oxide (NO) by lead-free halide perovskites has not yet been reported. Herein, we use Cs
2 PtI6 to realize the first example of a halide perovskite applied to NO sensing. Due to favoring Pt-N binding, the material has some excellent properties such as a NO detection limit as low as 100 parts-per-billion (ppb), ultrahigh selectivity to NO, and can work at room temperature for more than 2 months. In situ sum frequency generation (SFG) spectra and crystal orbital Hamilton population (COHP) analysis reveal that the strong bonding interaction between Pt 5s and N 2s ensure the high adsorption energy, and Pt 5d electron back donation to N 2px , N 2pz antibonding causes the conductive change of the sensors. In addition, its flexible wearable technology shows the application potential of the device and promotes the further development of perovskite materials.- Published
- 2021
- Full Text
- View/download PDF
50. pH Changes That Induce an Axial Ligand Effect on Nonheme Iron(IV) Oxo Complexes with an Appended Aminopropyl Functionality.
- Author
-
Latifi R, Palluccio TD, Ye W, Minnick JL, Glinton KS, Rybak-Akimova EV, de Visser SP, and Tahsini L
- Subjects
- Density Functional Theory, Hydrogen-Ion Concentration, Ligands, Molecular Structure, Iron Compounds chemistry, Oxygen chemistry
- Abstract
Nonheme iron enzymes often utilize a high-valent iron(IV) oxo species for the biosynthesis of natural products, but their high reactivity often precludes structural and functional studies of these complexes. In this work, a combined experimental and computational study is presented on a biomimetic nonheme iron(IV) oxo complex bearing an aminopyridine macrocyclic ligand and its reactivity toward olefin epoxidation upon changes in the identity and coordination ability of the axial ligand. Herein, we show a dramatic effect of the pH on the oxygen-atom-transfer (OAT) reaction with substrates. In particular, these changes have occurred because of protonation of the axial-bound pendant amine group, where its coordination to iron is replaced by a solvent molecule or anionic ligand. This axial ligand effect influences the catalysis, and we observe enhanced cyclooctene epoxidation yields and turnover numbers in the presence of the unbound protonated pendant amine group. Density functional theory studies were performed to support the experiments and highlight that replacement of the pendant amine with a neutral or anionic ligand dramatically lowers the rate-determining barriers of cyclooctene epoxidation. The computational work further establishes that the change in OAT is due to electrostatic interactions of the pendant amine cation that favorably affect the barrier heights.
- Published
- 2021
- Full Text
- View/download PDF
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