433 results on '"Zhong, Z."'
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2. Magnetic field modulated upconversion luminescence in NaYF4:Yb,Er nanoparticles.
- Author
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Chen, P., Jia, H., Zhong, Z., Han, J., Guo, Q., Zhou, J., Liu, X., and Qiu, J.
- Abstract
Upconversion, an anti-Stokes process that converts two or more lower energy photons into a higher energy photon, has been paid growing attention due to its wide range of applications ranging from photonics to bioscience. This process, however, suffers from poor efficiency which strongly hampers its application and commercialization. We show here that the upconversion luminescence of NaYF
4 :Yb,Er nanoparticles can be modulated by the magnetic field and an enhancement of upconversion intensity by a factor of 2.5 is obtained at 20 T. The increased upconversion luminescence is interpreted in terms of enhanced energy transfer from Yb3+ to Er3+ and the enhanced non-radiative transition from4 S3/2 to4 F9/2 and4 I11/2 to4 I13/2 of Er3+ ions. In addition, continuous spectral broadening and shift of f–f transitions with increasing magnetic field intensity are observed, which are ascribed to the Zeeman effect and the difference in the g factor of Zeeman levels. The results demonstrated here may open a new gate towards the modulation of the excited state process by the magnetic field. [ABSTRACT FROM AUTHOR]- Published
- 2015
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3. Synthesis and Diels–Alder Reaction of Acetylenic Sulfonate†.
- Author
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W. M. Lee, Albert, H. Chan, W., P. Zhong, Z., F. Lee, K., and B. W. Yeung, Anissa
- Published
- 1998
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4. Synthetic nanointerfacial bioengineering of Ti implants: on-demand regulation of implant-bone interactions for enhancing osseointegration.
- Author
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Dong Y, Hu Y, Hu X, Wang L, Shen X, Tian H, Li M, Luo Z, and Cai C
- Abstract
Titanium and its alloys are the most commonly used biometals for developing orthopedic implants to treat various forms of bone fractures and defects, but their clinical performance is still challenged by the unfavorable mechanical and biological interactions at the implant-tissue interface, which substantially impede bone healing at the defects and reduce the quality of regenerated bones. Moreover, the impaired osteogenesis capacity of patients under certain pathological conditions such as diabetes and osteoporosis may further impair the osseointegration of Ti-based implants and increase the risk of treatment failure. To address these issues, various modification strategies have been developed to regulate the implant-bone interactions for improving bone growth and remodeling in situ . In this review, we provide a comprehensive analysis on the state-of-the-art synthetic nanointerfacial bioengineering strategies for designing Ti-based biofunctional orthopedic implants, with special emphasis on the contributions to (1) promotion of new bone formation and binding at the implant-bone interface, (2) bacterial elimination for preventing peri-implant infection and (3) overcoming osseointegration resistance induced by degenerative bone diseases. Furthermore, a perspective is included to discuss the challenges and potential opportunities for the interfacial engineering of Ti implants in a translational perspective. Overall, it is envisioned that the insights in this review may guide future research in the area of biometallic orthopedic implants for improving bone repair with enhanced efficacy and safety.
- Published
- 2024
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5. A small library of copper-based metallenes with superior antibacterial activity.
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Miao Z, Lu C, Xu CY, Ma Y, Cao Z, Liu L, Gong D, and Zha Z
- Abstract
We report the preparation of a small library of copper-based metallenes, such as copperene, brassene, bronzene, cupronickelene and AlCuZn trimetallene, via a cryo-pretreatment assisted liquid phase exfoliation method. To the best of our knowledge, these nanosheets may represent a new category of metallenes. Benefiting from mixed-valence copper-induced oxidative stress and cleavage effects of layered structures, the obtained metallenes could efficiently eliminate drug-resistant bacteria even at a concentration as low as 1 μg mL
-1 . Due to the alloy engineering-induced change in the release rate of metal ions, the CuZn metallene exhibited a much better antibacterial ability than the other metallenes and three clinical antibiotics. We believe this work not only expands the category of emerging 2D metallenes, but also proposes a strategy combining 2D and alloy engineering to improve the antibacterial properties of copper-based materials.- Published
- 2024
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6. (Ga 1- x Al x ) 4 B 2 O 9 : controlled surface acid-base properties and catalytic behavior towards the Strecker reaction.
- Author
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Wang W, Fan Z, Tang S, Wu Y, Xu K, Luo B, and Suib SL
- Abstract
Solid bases are valuable catalysts for industrial syntheses. However, controlling the basicity of these catalysts remains a challenge. Ga
4 B2 O9 , due to μ3 -O within its structure, could behave as a special solid base catalyst exhibiting intrinsic Lewis basicity. In this work, a sol-gel method was proposed to obtain continuously adjustable acidity and basicity of the metal borate catalyst (Alx Ga1- x )4 B2 O9 . According to the results of NH3 -TPD, CO2 -TPD, and the systematic experimental design, Lewis basic sites originating from GaO5 groups in (Alx Ga1- x )4 B2 O9 boost the Strecker reaction rather than the Lewis acid sites related to unsaturated Al. This work illustrates the possible application of bulk-type solid solutions with simultaneous Lewis acid and base sites for the first time. A reaction mechanism has also been proposed based on the catalytic reaction results.- Published
- 2024
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7. Dirhodium(II) complex catalyzed dehydrosilylation of styrenes: theoretical investigations on the mechanism, selectivity, and ligand effects.
- Author
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Zhong Z, Li Q, and Li X
- Abstract
The dirhodium(II) complexes with bridging phosphine and OAc ligands showed high reactivity and selectivities in olefin dehydrosilylation. In order to determine the structure of the actual catalyst which cannot be determined experimentally, the geometries of the dirhodium catalyst, the detailed catalytic mechanism, and the stereo- and chemo-selectivities of the title reaction were studied using DFT calculations. The results showed that one OAc group is monodentate and the other is bidentate in the dirhodium catalyst C'. The determined catalytic cycle consists of four processes: Rh-H bond activation in C', Si-H bond activation in alkoxysilane, alkylene insertion into the Rh-Si bond, followed by β-H elimination or σ-metathesis reaction. Among them, the alkylene insertion process is the rate-determining step. The stereoselectivity of the title reaction is controlled by the steric effect and orbital interactions between the alkyene and dirhodium catalysts in the β-H elimination process. The chemoselectivity is regulated by the presence of the axial ligand in the dirhodium catalyst, when there is an axial ligand coordinated to the Rh atom, E -alkene is the main product, whereas alkane would be obtained in the absence of an axial ligand. Our work determines the structure of the actual catalyst, and provides explanations and predictions for the activity, and chemo- and stereo-selectivity control of olefin dehydrosilylation.
- Published
- 2024
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8. Zn-facilitated surface reconstruction of Ni-MOF for an enhanced oxygen evolution reaction.
- Author
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Wu F, Jiao Y, Ge JL, Zhu Y, Feng C, Wu Z, and Li Q
- Abstract
Facilitating the surface reconstruction of pre-catalysts has been considered an effective strategy for constructing low-cost and highly efficient OER electrocatalysts. Metal doping is a feasible way to activate the surface reconstruction, thus enhancing the OER performance. Herein, we report a facile hydrothermal method to synthesize a series of Zn-doped Ni-MOF on nickel foam (NiZn-MOF/NF) as promising pre-catalysts toward the oxygen evolution reaction (OER). The Zn leaching of NiZn-MOF/NF can promote the surface self-reconstruction of NiZn-MOF/NF into oxygen-vacancy-rich NiOOH after electrochemical activation. Benefiting from the optimized electronic structure, abundant defects, more accessible active sites, and enhanced electrical conductivity, the reconstructed metal oxyhydroxide hybrids exhibit better electrocatalytic activity than the catalysts transformed from Ni-MOF/NF without Zn doping. The optimized NiZn-MOF/NF-OH as an OER catalyst has an overpotential of 336 mV at 100 mA cm
-2 , and a Tafel slope of 65.9 mV dec-1 , as well as stability over 12 h. This work reveals that Zn cation-doping/leaching induces the surface reconstruction of pre-catalysts for enhanced oxygen catalytic activity, which provides a new approach for the development of advanced electrocatalysts.- Published
- 2024
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9. Visible-light-driven asymmetric aldol reaction of ketones and glycinates via synergistic Lewis acid/photoredox catalysis.
- Author
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Tan J, Yang L, Su H, Yang Y, Zhong Z, Feng X, and Liu X
- Abstract
Visible-light-driven direct asymmetric α-C(sp
3 )-H bond functionalization of glycinate provides a direct and efficient route for the synthesis of diverse optically enriched α-amino acid derivatives. However, asymmetric coupling between glycinate radical species and ketones faces significant challenges, including competitive pathways, mutable intermediates, as well as congested stereogenic centers. Herein, we disclose the first example for the asymmetric photocatalytic synthesis of a diverse array of β-diaryl-β-hydroxy-α-amino acetate derivatives from glycinates and heteroaryl ketones through the synergistic catalysis of achiral iridium photoredox catalyst and chiral lanthanide Lewis acid catalysts. The enantioselective radical addition pathway is supported by spectroscopic experiments, control experiments and DFT calculations., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)- Published
- 2024
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10. Nanoconfined tandem three-phase photocatalysis for highly selective CO 2 reduction to ethanol.
- Author
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Huo H, Hu T, Zhong Z, Zhan C, Huang C, Ju Q, Zhang L, Wu F, Kan E, and Li A
- Abstract
The conversion of CO
2 and H2 O into ethanol with high selectivity via photocatalysis is greatly desired for effective CO2 resource utilization. However, the sluggish and challenging C-C coupling hinders this goal, with the behavior of *CO holding the key. Here, a nanoconfined and tandem three-phase reaction system is established to simultaneously enhance the *CO concentration and interaction time, achieving an outstanding ethanol selectively of 94.15%. This system utilizes a tandem catalyst comprising an Ag core and a hydrophobic Cu2 O shell. The hydrophobic Cu2 O shell acts as a CO2 reservoir, effectively overcoming the CO2 mass-transfer limitation, while the Ag core facilitates the conversion of CO2 to CO. Subsequently, CO undergoes continuous reduction within the nanoconfined mesoporous channels of Cu2 O. The synergy of enhanced mass transfer, nanoconfinement, and tandem reaction leads to elevated *CO concentrations and prolonged interaction time within the Cu2 O shell, significantly reducing the energy barrier for *CO-*CO coupling compared to the formation of *CHO from *CO, as determined by density functional theory calculations. Consequently, C-C coupling preferentially occurs over *CHO formation, producing excellent ethanol selectivity. These findings provide valuable insights into the efficient production of C2+ compounds., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)- Published
- 2024
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11. Thermal modulation of surface-enhanced Raman scattering and plasmon-induced catalysis in Ag nanoparticle/ZnO microrod composites.
- Author
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Wang Y, Liu R, Zhong Z, Liu J, Feng X, Liu L, and Jiang F
- Abstract
The surface-enhanced Raman scattering (SERS) performance and photocatalytic degradation of dye molecules absorbed on Ag nanoparticle-decorated ZnO microrods are investigated at 20 and 50 °C. The role of temperature in the mechanism is elucidated. This work provides insight into the optimization of temperature-dependent plasmon-induced catalysis using similar materials.
- Published
- 2024
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12. Negative Poisson's ratio of sulfides dominated by strong intralayer electron repulsion.
- Author
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Zhu Y, Cao X, Yang S, Hu J, Li B, and Chen Z
- Abstract
Geometrical variations in a particular structure or other mechanical factors are often cited as the cause of a negative Poisson's ratio (NPR). These factors are independent of the electronic properties of the materials. This work investigates a class of two-dimensional (2D) sulfides with the chemical formula MX
2 (M = Ti, Cr, Mn, Fe, Co, X = S) using first-principles calculations. Among them, monolayered TiS2 , CrS2 , and MnS2 were found to exhibit a structure-independent NPR. The strong strain response of intra-layer interactions is responsible for this unique phenomenon. This can be traced to the lone pair of electrons of the S atoms and the weak electronegativity of the central atoms in multi-orbital hybridization. Our study provides valuable insights and useful guidelines for designing innovative NPR materials.- Published
- 2024
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13. Advanced lightweight lightning strike protection composites based on super-aligned carbon nanotube films and thermal-resistant zirconia fibers.
- Author
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Zhu M, Zhang P, Gao F, Bai Y, Zhang H, Zu M, Liu L, and Zhang Z
- Abstract
Carbon nanotube films have drawn attention in the past decade as promising substitutes for aluminum or copper used in aircraft lightning strike protection (LSP) systems. Throughout this study, advanced lightweight lightning strike protection (LSP) composites are based on highly conductive super-aligned carbon nanotube films (SA-CNTFs) and a new isolation layer of zirconia fiber paper. The internal damage level of the composite laminate was assessed using a microfocus X-ray system and non-destructive ultrasonic techniques. Results show that the composite laminate comprising SA-CNTFs (1000-layer) and zirconia fiber paper (1-layer) effectively shields CFRP from 100 kA lightning strikes. Furthermore, weight reductions of approximately 44.3% and 10.4% can be achieved, respectively, relative to the isolation layer of glass fibers and quartz fibers. Meanwhile, the lightning protection mechanism was further studied., Competing Interests: The authors declare no competing financial interest in this work., (This journal is © The Royal Society of Chemistry.)
- Published
- 2024
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14. Bifidobacterium animalis subsp. lactis LPL-RH improves postoperative gastrointestinal symptoms and nutrition indexes by regulating the gut microbiota in patients with valvular heart disease: a randomized controlled trial.
- Author
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Lan W, Yang H, Zhong Z, Luo C, Huang Q, Liu W, Yang J, Xiang H, Tang Y, and Chen T
- Subjects
- Humans, Male, Female, Middle Aged, Adult, Postoperative Complications microbiology, Aged, Gastrointestinal Diseases, Double-Blind Method, Gastrointestinal Microbiome drug effects, Probiotics therapeutic use, Probiotics administration & dosage, Probiotics pharmacology, Bifidobacterium animalis, Heart Valve Diseases surgery
- Abstract
Gastrointestinal symptoms constitute a frequent complication in postoperative patients with valvular heart disease (VHD), impacting their postoperative recovery. Probiotics contribute to regulating human gut microbiota balance and alleviating postoperative gastrointestinal symptoms. Our objective involved assessing the potential of Bifidobacterium animalis subsp. lactis LPL-RH to alleviate postoperative gastrointestinal symptoms and expedite patient recovery. Adult patients diagnosed with VHD scheduled for valve surgery were enrolled. 110 patients were randomly divided into two groups and received LPL-RH or a placebo for 14 days. Gastrointestinal symptoms were evaluated using the Gastrointestinal Symptoms Questionnaire. An analysis of the time to recovery of bowel function and various postoperative variables was conducted in both study groups. Variations in the intestinal microbiota were detected via 16S rRNA sequencing. The study was completed by 105 participants, with 53 in the probiotic group and 52 in the placebo group. Compared to the placebo group, LPL-RH significantly reduced the total gastrointestinal symptom score after surgery ( p = 0.004). Additionally, LPL-RH was found to significantly reduce abdominal pain ( p = 0.001), bloating ( p = 0.018), and constipation ( p = 0.022) symptom scores. Furthermore, LPL-RH dramatically shortened the time to recovery of bowel function ( p = 0.017). Moreover, LPL-RH administration significantly enhanced patients' postoperative nutrition indexes (red blood cell counts, hemoglobin level, p < 0.05). Microbiome analysis showed that the composition and diversity of the postoperative intestinal microbiota differed between the probiotic and placebo groups. No adverse incidents associated with probiotics were documented, emphasizing their safety. This study initially discovered that oral B. animalis subsp. lactis LPL-RH can assist in regulating intestinal microbiota balance, alleviating gastrointestinal symptoms, promoting intestinal function recovery, and enhancing nutrition indexes in patients with VHD after surgery. Regulating the intestinal microbiota may represent a potential mechanism for LPL-RH to exert clinical benefits.
- Published
- 2024
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15. Laser-induced microbubble as an in vivo valve for optofluidic manipulation in living Mice's microvessels.
- Author
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Shao M, Li C, Meng C, Liu R, Yu P, Lu F, Zhong Z, Wei X, Zhou J, and Zhong MC
- Subjects
- Animals, Mice, Microbubbles, Lasers, Microvessels physiology
- Abstract
Optofluidic regulation of blood microflow in vivo represents a significant method for investigating illnesses linked to abnormal changes in blood circulation. Currently, non-invasive strategies are limited to regulation within capillaries of approximately 10 μm in diameter because the adaption to blood pressure levels in the order of several hundred pascals poses a significant challenge in larger microvessels. In this study, using laser-induced microbubble formation within microvessels of the mouse auricle, we regulate blood microflow in small vessels with diameters in the tens of micrometers. By controlling the laser power, we can control the growth and stability of microbubbles in vivo . This controlled approach enables the achievement of prolonged ischemia and subsequent reperfusion of blood flow, and it can also regulate the microbubbles to function as micro-pumps for reverse blood pumping. Furthermore, by controlling the microbubble, narrow microflow channels can be formed between the microbubbles and microvessels for assessing the apparent viscosity of leukocytes, which is 76.9 ± 11.8 Pa·s in the in vivo blood environment. The proposed design of in vivo microbubble valves opens new avenues for constructing real-time blood regulation and exploring cellular mechanics within living organisms.
- Published
- 2024
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16. Brønsted acid catalyzed [4 + 2] cycloaddition for the synthesis of bisbenzannulated spiroketals with antifungal activities.
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Hu T, Zhao Y, Luo X, Li Z, and Yang WL
- Abstract
The intermolecular [4 + 2] cycloaddition of o -hydroxy benzyl alcohols with isochroman ketals was realized by CF
3 CO2 H catalysis. A broad range of bisbenzannulated [6,6]-spiroketals were formed under the metal-free mild conditions in moderate to excellent yields (45-98%) with mostly excellent diastereoselectivities (up to >20 : 1 dr). Furthermore, the enantioselective version was also preliminarily investigated and the bisbenzannulated [6,6]-spiroketal was obtained with 61% ee in the presence of Sc(OTf)3 /Feng's chiral N , N '-dioxide ligand. Some of the bisbenzannulated [6,6]-spiroketal products showed good in vitro antifungal activities against Sclerotinia sclerotiorum and Rhizoctonia solani .- Published
- 2024
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17. Synthesis of organic-inorganic hybrid nanocomposites modified by catalase-like catalytic sites for the controlling of kiwifruit bacterial canker.
- Author
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Ding Z, Song Q, Wang G, Zhong Z, Zhong G, Li H, Chen Y, Zhou X, Liu L, and Yang S
- Abstract
Kiwifruit bacterial canker, caused by Pseudomonas syringae pv. Actinidiae ( Psa ), is one of the most important diseases in kiwifruit, creating huge economic losses to kiwifruit-growing countries around the world. Metal-based nanomaterials offer a promising alternative strategy to combat plant diseases induced by bacterial infection. However, it is still challenging to design highly active nanomaterials for controlling kiwifruit bacterial canker. Here, a novel multifunctional nanocomposite (ZnO@PDA-Mn) is designed that integrates the antibacterial activity of zinc oxide nanoparticles (ZnO NPs) with the plant reactive oxygen species scavenging ability of catalase (CAT) enzyme-like active sites through introducing manganese modified polydopamine (PDA) coating. The results reveal that ZnO@PDA-Mn nanocomposites can efficiently catalyze the conversion of H
2 O2 to O2 and H2 O to achieve excellent CAT-like activity. In vitro experiments demonstrate that ZnO@PDA-Mn nanocomposites maintain the antibacterial activity of ZnO NPs and induce significant damage to bacterial cell membranes. Importantly, ZnO@PDA-Mn nanocomposites display outstanding curative and protective efficiencies of 47.7% and 53.8% at a dose of 200 μg mL-1 against Psa in vivo , which are superior to those of zinc thiozole (20.6% and 8.8%) and ZnO (38.7% and 33.8%). The nanocomposites offer improved in vivo control efficacy through direct bactericidal effects and decreasing oxidative damage in plants induced by bacterial infection. Our research underscores the potential of nanocomposites containing CAT-like active sites in plant protection, offering a promising strategy for sustainable disease management in agriculture., Competing Interests: The authors confirm that they have no known competing financial interests or personal relationships that could have influenced the findings presented in this paper., (This journal is © The Royal Society of Chemistry.)- Published
- 2024
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18. Revealing the ACE receptor binding properties and interaction mechanisms of salty oligopeptides from Stropharia rugosoannulata mushroom by molecular simulation and antihypertensive evaluation.
- Author
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Li W, Chen W, Wang J, Zhang Z, Wu D, Liu P, Li Z, Ma H, and Yang Y
- Subjects
- Animals, Rats, Male, Peptidyl-Dipeptidase A metabolism, Peptidyl-Dipeptidase A chemistry, Agaricales chemistry, Agaricales metabolism, Mice, Hypertension drug therapy, Hypertension metabolism, Angiotensin-Converting Enzyme Inhibitors pharmacology, Angiotensin-Converting Enzyme Inhibitors chemistry, Angiotensin-Converting Enzyme Inhibitors metabolism, Protein Binding, Blood Pressure drug effects, Rats, Inbred SHR, Oligopeptides pharmacology, Oligopeptides chemistry, Oligopeptides metabolism, Antihypertensive Agents pharmacology, Antihypertensive Agents chemistry, Molecular Dynamics Simulation
- Abstract
The salty oligopeptides from Stropharia rugosoannulata have been proven to be potential ACE inhibitors. To investigate the ACE receptor binding properties and interaction mechanisms of salty oligopeptides, the molecular interaction, dynamics simulation, and antihypertensive evaluation cross-validation strategy were employed to reveal the oligopeptides' binding reactions and modes with the ACE receptor. Single oligopeptide (ESPERPFL, KSWDDFFTR) had exothermic and specific binding reactions with the ACE receptor, driven by hydrogen bonds and van der Waals forces. The coexistence of the multiple oligopeptide molecules did not produce the apparent ACE receptor competition binding reactions. The molecular dynamics simulation verified that the two oligopeptides disturbed the ACE receptor's different residue regions. Both oligopeptides could form stable complexes with the ACE receptor. Based on the classification of 50 oligopeptides' binding modes, ESPERPFL and KSWDDFFTR belonged to different classes, and their receptor binding modes and sites complemented, resulting in a potential synergistic effect on ACE inhibition. The antihypertensive effect of KSWDDFFTR and its distribution in the body were evaluated using SHR rats orally and ICR mice by tail vein injection, and KSWDDFFTR had antihypertensive effects within 8 h. The study provides a theoretical basis for understanding salty oligopeptides' ACE receptor binding mechanism and their antihypertensive effects.
- Published
- 2024
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19. A liquid metal-embedded 3D interconnected-porous TPU/MXene composite with improved capacitive sensitivity and pressure detection range.
- Author
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Zheng Z, Fang X, Pan Y, Song S, Xue H, Li J, Li Y, and Li J
- Abstract
Flexible capacitive sensors are widely deployed in wearable smart electronics. Substantial studies have been devoted to constructing characteristic material architectures to improve their electromechanical sensing performance by facilitating the change of the electrode layer spacing. However, the air gaps introduced by the designed material architectures are easily squeezed when subjected to high-pressure loads, resulting in a limited increase in sensitivity over a wide range. To overcome this limitation, in this work, we embed the liquid metal (LM) in the internally interconnected porous structure of a flexible composite foam to fabricate a flexible and high-performance capacitive sensor. Different from the conventional conductive elements filled composite, the incompressible feature of the embedded fluidic LM leads to significantly improved mechanical stability of the composite foam to withstand high pressure loadings, resulting in a wider pressure sensing range from 10 Pa to 260 kPa for our capacitive composite sensor. Simultaneously, the metal conductivity and liquid ductility of the embedded LM endow the as-fabricated capacitive sensor with outstanding mechanical flexibility and pressure sensitivity (up to 1.91 kPa
-1 ). Meanwhile, the LM-embedded interconnected-porous thermoplastic polyurethane/MXene composite sensor also shows excellent reliability over 4000 long-period load cycles, and the response times are merely 60 ms and 110 ms for the loading and unloading processes, respectively. To highlight their advantages in various applications, the as-proposed capacitive sensors are demonstrated to detect human movements and monitor biophysical heart-rate signals. It is believed that our finding could extend the material framework of flexible capacitive sensors and offer new possibilities and solutions in the development of the next-generation wearable electronics., Competing Interests: The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (This journal is © The Royal Society of Chemistry.)- Published
- 2024
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20. Dehydrative alkynylation of 3-hydroxyisoindolinones with terminal alkynes for the synthesis of 3-alkynylated 3,3-disubstituted isoindolinones.
- Author
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Yang KC, Zheng SL, Wen Z, Zhang YS, Ni HL, and Chen L
- Abstract
A brand-new procedure for the synthesis of 3-alkynylated 3,3-disubstituted isoindolinones has been disclosed via a HOTf or Fe(OTf)
3 -catalyzed dehydrative alkynylation of 3-hydroxyisoindolinones with terminal alkynes. Aryl, alkenyl and alkyl terminal alkynes are suitable to couple with a broad range of 3-hydroxyisoindolinones to afford the desired products in moderate to good yields. This protocol features the use of an inexpensive catalyst, mild reaction conditions, broad substrate scope and easy elaboration of the products.- Published
- 2024
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21. Surface hopping simulations on charge photogeneration in conjugated polymers.
- Author
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Sun Z, Li S, Meng Y, and An Z
- Abstract
The mechanism of charge photogeneration in neat conjugated polymers has long been controversial and a unified explanation has not been achieved so far. In this paper, we use a surface hopping method to simulate the excited-state dynamics of a system composed of five π-stacked polymer chains. In this system, polaron pairs (PPs) with large electron-hole distance can be seen as free charges. The surface hopping method is based on the Pariser-Parr-Pople (PPP) Hamiltonian and the excited states of the system are calculated with configuration interaction singles (CIS) formalism. During the simulations, the yields of PPs and free charges are calculated using a statistical method. By comparison, it is found that impurity and excess energy have significant effects on the yields of PPs and free charges. Free charges are difficult to be generated in neat systems with small excess energy. Free charges come from direct dissociation of high-energy excitons.
- Published
- 2024
- Full Text
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22. Flexible, transparent, and sustainable cellulose-based films for organic solar cell substrates.
- Author
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Huang L, Li Y, Zheng Z, Bai Y, Russell TP, and He C
- Abstract
Cellulose, often considered a highly promising substitute for petroleum-based plastics, offers several compelling advantages, including abundant availability, cost-effectiveness, environmental friendliness, and biodegradability. However, its inherent highly crystalline structure and extensive hydrogen-bonded network pose challenges for processing and recycling. In this study, we introduce the concept of cellulose vitrimers (CVs), wherein dynamic bonds are incorporated to reconfigure the hydrogen-bonded network, resulting in a mechanically robust, highly transparent material. CVs exhibit exceptional malleability, thermal stability, and noteworthy resistance to water and solvents. Due to the dynamic bond disassociation, CVs can be effectively chemically recycled using a well-established "dissolution-and-reforming" process. Moreover, CVs have proven successful as flexible substrate materials for organic solar cells, outperforming traditional petroleum-based polyethylene naphthalate (PEN). Given these advantages, CVs have the potential to replace conventional petroleum-based materials as recyclable and environmentally friendly alternatives, particularly within the realm of electronic devices and displays.
- Published
- 2024
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23. The toxicity response of the electrochemical signal of the cell to the drug metabolized by the S9 system.
- Author
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Zhang J, Fei C, Qi S, Fu J, Zhou S, Wang Z, Li J, Zhao Y, and Wu D
- Subjects
- Fluorenes toxicity, Guanine, Mutagens, Benzo(a)pyrene metabolism, Benzo(a)pyrene toxicity, Biochemical Phenomena
- Abstract
The electrochemical detection method of cytotoxicity using intracellular purines as biomarkers has shown great potential for in vitro drug toxicity evaluation. However, no electrochemical detection system based on an in vitro drug metabolism mechanism has been devised. In this paper, electrochemical voltammetry was used to investigate the effect of the S9 system on the electrochemical behavior of HepG2 cells, and benzo[ a ]pyrene, fluoranthene, and pyrene were employed to investigate the sensitivity of electrochemical signals of cells to the cytotoxicity of drugs metabolized by the S9 system. The results showed that, within 8 h of exposure to the S9 system, the electrochemical signal of HepG2 cells at 0.7 V did not alter noticeably. The levels of xanthine, guanine, hypoxanthine, and adenine in the cells were not significantly altered. Compared with the absence of S9 system metabolism, benzo[ a ]pyrene and fluoranthene processed by the S9 system decreased the electrochemical signal of the cells in a dose-dependent manner, while pyrene did not change it appreciably. HPLC also revealed that benzo[ a ]pyrene and fluoranthene metabolized by the S9 system decreased the intracellular purine levels, whereas pyrene had no effect on them before and after S9 system metabolism. The cytotoxicity results of the three drugs examined by electrochemical voltammetry and MTT assay showed a strong correlation and good agreement. The S9 system had no effect on the intracellular purine levels or the electrochemical signal of cells. When the drug was metabolized by the S9 system, variations in cytotoxicity could be precisely detected by electrochemical voltammetry.
- Published
- 2024
- Full Text
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24. A first-principles study of 2D single-layer SiP as anode materials for lithium-ion batteries and sodium-ion batteries.
- Author
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Xing Y, Cao C, Huang Z, Huang L, Zhang H, and Jia Q
- Abstract
The promotion of lithium-ion batteries and sodium-ion batteries is limited by the deficiency of suitable anode materials with desired electrochemical properties. In this work, the models of 2D single-layer SiP are constructed to explore its potential as an anode material for LIBs and SIBs using density functional theory (DFT). The diffusion of Li in bulk SiP is anisotropic. There is a low diffusion energy barrier of 0.28 eV along the X -axis. The low surface exfoliation energy suggests that there is a high probability of preparing 2D single-layer SiP experimentally. Its structure stability is verified by ab initio molecular dynamics (AIMD) simulations at 300 K and 400 K. The intercalation and diffusion behaviors of Li/Na on 2D single-layer SiP indicate that Li/Na tends to diffuse along the X -axis direction of 2D single-layer SiP. The diffusion energy barrier of Li/Na on 2D single-layer SiP is lower compared to that of bulk SiP. The conductivity of 2D single-layer SiP is improved after lithiation due to the upshift of Fermi levels. 2D single-layer SiP has a lower average open circuit voltage (1.50 V for LIBs and 1.08 V for SIBs) and a high theoretical capacity (520 mA h g
-1 ). Hence, 2D single-layer SiP can be an ideal anode material for LIBs and SIBs.- Published
- 2024
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25. Transition metal small clusters anchored on biphenylene for effective electrocatalytic nitrogen reduction.
- Author
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Gao Y, Li Q, Yin Z, Wang H, Wei Z, and Gao J
- Abstract
The synthesis of ammonia via an electrochemical nitrogen reduction reaction (NRR, N
2 + 6H+ + 6e- → 2NH3 ), which can weaken but not directly break an inert NN bond under mild conditions via multiple progressive protonation steps, has been proposed as one of the most attractive alternatives for the production of NH3 . However, the development of appropriate catalyst materials is a major challenge in the application of NRRs. Recently, single- or multi-metal atoms anchored on two-dimensional (2D) substrates have been demonstrated as ideal candidates for facilitating NRRs. In this work, by applying spin-polarized density functional theory and ab initio molecular dynamic simulations, we systematically explored the performances of nine types of transition metal multi-atoms anchored on a recently developed 2D biphenylene (BPN) sheet in nitrogen reduction. Structural stability and NRR performance catalyzed by TMn (TM = V, Fe, Ni, Mo, Ru, Rh, W, Re, Ir; n = 1-4) clusters anchored on BPN sheets were systematically explored. After a strict six-step screening strategy, it was found that W2 , Ru2 and Mo4 clusters loaded on BPN demonstrate superior potential for nitrogen reduction with extremely low onset potentials of -0.26, -0.36 and -0.17 V, respectively. Electronic structure analysis revealed that the enhanced ability of these multi-atom catalysts to effectively capture and reduce the N2 molecule can be attributed to bidirectional charge transfer between the d orbitals of transition metal atoms and molecular orbitals of the adsorbed N2 through a "donation-back donation" mechanism. Our findings highlight the value of BPN sheets as a substrate for designing multi-atom nitrogen reduction reaction catalysts.- Published
- 2024
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26. A monofunctional Pt(II) complex combats triple negative breast cancer by triggering lysosome-dependent cell death.
- Author
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Shen X, Peng Y, Yang Z, Li R, Zhou H, Ye X, Han Z, and Shi X
- Subjects
- Humans, Cell Death, Cell Line, Tumor, Lysosomes metabolism, Platinum pharmacology, Platinum therapeutic use, Organoplatinum Compounds chemistry, Organoplatinum Compounds pharmacology, Organoplatinum Compounds therapeutic use, Triple Negative Breast Neoplasms drug therapy, Triple Negative Breast Neoplasms metabolism
- Abstract
Monofunctional Pt(II) complexes with potent efficacy to overcome the drawbacks of current platinum drugs represent a promising therapeutic approach for triple negative breast cancer (TNBC). A heterocyclic-ligated monofunctional Pt(II) complex PtL with a unique action of mode was designed and investigated. PtL induced DNA single-strand breaks and caused genomic instability in TNBC cells. Mechanism studies demonstrated that PtL disrupted lysosomal acidity and function, which in turn triggered lysosome-dependent cell death. Furthermore, PtL showed convincing suppression in the tube forming and cell migratory abilities against the metastatic potential of TNBC cells. The synthesis and investigation of PtL revealed its potential value as an anti-TNBC drug and extended the family of monofunctional Pt(II) complexes.
- Published
- 2024
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27. Lactobacillus plantarum 24-7 improves postoperative bloating and hard stools by modulating intestinal microbiota in patients with congenital heart disease: a randomized controlled trial.
- Author
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Yang H, Lan W, Luo C, Huang Q, Zhong Z, Yang J, Xiang H, Chen T, and Tang Y
- Subjects
- Adult, Humans, RNA, Ribosomal, 16S, Lactobacillus plantarum, Gastrointestinal Microbiome, Probiotics therapeutic use, Heart Defects, Congenital surgery
- Abstract
Gastrointestinal symptoms are a common postoperative complication in patients with congenital heart disease (CHD), affecting their postoperative recovery. Probiotic intervention may be a promising therapeutic approach to alleviate postoperative gastrointestinal symptoms. This study aimed to evaluate the potential of Lactobacillus plantarum 24-7 ( L. plantarum 24-7 ) in mitigating postoperative gastrointestinal symptoms and promoting patient recovery. Adult CHD patients scheduled for surgical intervention were recruited. One hundred and twenty patients were randomized and received L. plantarum or placebo intervention twice daily for ten days. Gastrointestinal symptoms were assessed utilizing the Gastrointestinal Symptom Rating Scale (GSRS). Various postoperative variables were analyzed across both groups. Alterations in gut microbiota were evaluated through 16S rRNA sequencing. 112 patients completed the study, with 55 in the probiotic group and 57 in the placebo group. While the disparity in overall postoperative GSRS scores between the two groups did not reach statistical significance ( P = 0.067), marked differences were observed in bloating ( P = 0.004) and hard stool ( P = 0.030) scores. Furthermore, individuals within the probiotic group exhibited lower postoperative neutrophil counts ( P = 0.007) and concurrently higher lymphocyte counts ( P = 0.001). Variations in the diversity and composition of postoperative gut microbiota were discerned between the probiotic and placebo groups. Remarkably, no probiotic-related adverse events were documented. Supplementation with L. plantarum was well-tolerated and demonstrated partial efficacy in ameliorating gastrointestinal symptoms in postoperative CHD patients. Modulating the gut microbiota may be a potential mechanism by which L. plantarum exerts clinical benefits.
- Published
- 2024
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28. n-Type boron β-diketone-containing conjugated polymers for high-performance room temperature ammonia sensors.
- Author
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Song W, Sun J, Wang Q, Wu H, Zheng K, Wang B, Wang Z, and Long X
- Abstract
Organic semiconductor (OSC) gas sensors with good mechanical flexibility have received considerable attention as commercial and wearable devices. However, due to poor resistance to moisture and low conductivity, the improvement in the sensing capability of individual OSCs is limited. Reported here is a promising pathway to construct a series of conjugated organic polymers (COPs) with well-defined pyrimidine (Py-COP) or boron β-diketone (BF-COP) units. Unlike traditional metal- or carbon-based hybrid materials, the developed COPs can provide abundant absorption sites for gaseous analytes. As a result, the as-prepared BF-COP results in an excellent sensing response of over 1500 ( R
a / Rg ) toward 40 ppm of NH3 at room temperature, which is the highest value among those of pristine COPs as n-type sensing materials. Notably, they can maintain their initial sensing responses for two months and 90% relative humidity resistance. Combining the results of in situ Fourier transform infrared spectroscopy and theoretical calculations, the β-diketone skeleton is found to activate the surface electronic environment, verifying that the electron-deficient B ← O groups are adsorption centers. The B/N-heterocyclic decoration effectively modulates the redox properties and electronic interactions, as well as perturbs charge transfer in typical π-conjugated COPs. These results offer insight into developing highly efficient OSC gas sensors, which potentially have broadened sensing applications in the areas of organoboron chemistry.- Published
- 2024
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29. Narrowband TADF emitters with high utilization of triplet excitons: theoretical insights and molecular design.
- Author
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Zhang Q, Liu T, Shi Z, Zheng Z, Lv C, Wang X, and Zhang Y
- Abstract
Narrowband emitters with thermally activated delayed fluorescence (TADF) features, known as multi-resonant TADF (MR-TADF) emitters, are drawing increasing research interest owing to their properties of high efficiency and excellent color purity. However, MR-TADF-based devices often face serious efficiency roll-off at high luminance intensity, which could be attributed to undesired triplet-triplet annihilation (TTA) caused by the structural planarity and relatively small reverse intersystem crossing rate constants ( k
risc ) of MR-TADF emitters. Herein, combining a sp3 -C inserted strategy to suppress harmful bimolecular interactions and chalcogens to improve the krisc , a series of asymmetric narrowband emitters, namely, DMAC-O, DMAC-S, and DMAC-Se, have been theoretically designed to break the slow rate-limiting step of krisc of experimental BN-DMAC. For comparison, both O and Se atoms were doped into the MR skeleton to substitute two sp3 -inserted units, yielding BN-O-Se. The combination of TD-DFT and the wavefunction-based STEOM-DLPNO-CCSD approach exhibits that those asymmetric molecules are promising for simultaneously exhibiting narrow emission spectral full-width at half-maximums (FWHMs) and high luminous efficiencies. The contributions of chalcogens to hole distributions result in red-shifted fluorescent peaks, and the asymmetric strategy also helps with twisted molecular configuration, which is beneficial for suppressing unfavorable TTA. Furthermore, the incorporation of chalcogens is sufficient to promote the intersystem crossing and reverse intersystem crossing channels of asymmetric emitters. More importantly, the doped heavy Se atom results in a significantly increased krisc of 2.32 × 106 s-1 for DMAC-Se, which is more than 200 times larger than 1.09 × 104 s-1 of pristine BN-DMAC. These results suggest that the combination of the heavy Se atom and an sp3 -inserted unit is a feasible strategy for achieving poor planarity and significantly enhancing krisc , which will help in harvesting triplet excitons, thereby inhibiting efficiency roll-off in corresponding narrowband devices.- Published
- 2024
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30. Rational design of a polypropylene composite foam with open-cell structure via graphite conductive network for sound absorption.
- Author
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Li Z, Yang C, Yan K, Xia M, Yan Z, Wang D, and Wang W
- Abstract
An exciting result is reported in this study where a polypropylene (PP) foam with a high open-cell content was achieved by constructing a thermally conductive network for the first time. PP and nano-graphite particles were used as substrate and filler, respectively, to prepare the PP-graphite (PP-G) composite foam by twin-screw blending, hot pressing, and supercritical CO
2 foaming. The nano-graphite particles can effectively adjust the microstructure of the PP-G foam and achieve a high porosity. When the amount of nano-graphite is 10.0 wt%, the PP-G foam exhibits optimal sound absorption performance, compression resistance, heat insulation, and hydrophobic properties. In the human-sensitive frequency range of 1000-6000 Hz, the corresponding average SAC is above 0.9, and the internal tortuosity is 5.27. After 50 cycles of compression, the compressive stress is 980 kPa and the SAC loss is only 7.8%. This study also innovatively proposed a new strategy to achieve the simple and rapid preparation of open-cell PP foams by increasing the thermal conductivity of the foaming substrate.- Published
- 2024
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31. Study on the preparation of ascorbic acid reduced ultrafine copper powders in the presence of different protectants and the properties of copper powders based on methionine protection.
- Author
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Ke X, Xie B, Zhang J, Wang J, Li W, Ban L, Hu Q, He H, Wang L, and Wang Z
- Abstract
High-purity, monodisperse, and low-oxygen submicron copper powder particles with particle sizes in the range of 100-600 nm were synthesized under alkaline conditions using ascorbic acid (C
6 H8 O6 ) as a reductant and copper chloride (CuCl2 ·2H2 O) as a copper source. The redox potential of the Cu-Cl-H2 O system was obtained by calculations and plotted on pH- E diagrams, and a one-step secondary reduction process (Cu(ii) → CuCl(i) → Cu2 O(i) → Cu(0)) was proposed to slow down the reaction rate. The commonalities and differences in the nucleation and growth process of copper powders under methionine (Met), hexadecyl trimethyl ammonium bromide (CTAB), and sodium citrate dihydrate (SSC) as protectants and without the addition of protectants are compared, and the reaction mechanism is discussed. Among them, methionine (Met) showed excellent properties and the Cu2 O(i) → Cu(0) process was further observed by in situ XRD. The synthesized copper powder particles have higher particle size controllability, dispersibility, antioxidant properties, and stability, and can be decomposed at lower temperatures (<280 °C). The resistivity can reach 21.4 μΩ cm when sintered at a temperature of 325 °C for 30 min. This green and simple synthesis process facilitates industrialization and storage, and the performance meets the requirements of electronic pastes., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)- Published
- 2024
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32. Covalent organic frameworks with flexible side chains in hybrid PEMs enable highly efficient proton conductivity.
- Author
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Liu Z, Pang X, Shi B, Xing N, Liu Y, Lyu B, Zhang L, Kong Y, Wang S, Gao Z, Xue R, Jing T, Liu C, Bai Q, Wu H, and Jiang Z
- Abstract
Electrochemical hydrogen compression (EHC) is an emerging energy conversion technology. Proton exchange membranes (PEMs) with high proton conductivity and high mechanical strength are highly required to meet the practical requirements of EHC. Herein, ionic covalent organic frameworks (iCOFs) with tunable side chains were synthesized and introduced into the sulfonated poly (ether ether ketone) (SPEEK) matrix to fabricate hybrid PEMs. In our membranes, the rigid iCOFs afford ordered proton conduction channels, whereas the flexible side chains on iCOFs afford abundant proton conduction sites, adaptive hydrogen bonding networks, and high local density short hydrogen bonds for highly efficient proton transport. Moreover, the hydrogen bond interactions between the side chains on iCOFs and the SPEEK matrix enhance the mechanical stability of membranes. As a result, the hybrid PEM acquires an enhanced proton conductivity of 540.4 mS cm
-1 (80 °C, 100%RH), a high mechanical strength of 120.41 MPa, and a superior performance (2.3 MPa at 30 °C, 100%RH) in EHC applications.- Published
- 2024
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33. Chlorogenic acid releasing microspheres enhanced electrospun conduits to promote peripheral nerve regeneration.
- Author
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Fang J, Jin X, Xu B, Nan L, Liu S, Wang J, Niu N, Wu Z, Chen F, and Liu J
- Subjects
- Rats, Animals, Microspheres, Prostheses and Implants, Nerve Regeneration, Chlorogenic Acid pharmacology, Sciatic Nerve
- Abstract
Chlorogenic acid (CGA) has been confirmed as a polyphenol, and existing research has suggested the high bioactivity of CGA for therapeutic effects on a wide variety of diseases. Despite the existing reports of anti-inflammatory, antioxidant, and neuroprotective effects of CGA, the role and mechanism of CGA in facilitating the regeneration of peripheral nerve defects have been rarely investigated. Herein, a biodegradable polycaprolactone (PCL) conduit with embedded CGA-releasing GelMA microspheres (CGM/PCL) was successfully prepared and used for repairing a rate model with sciatic nerve defects. CGM and CGM/PCL conduits displayed high in vitro biocompatibility and can support the growth of cells for nerve regeneration. Furthermore, CGM/PCL conduits displayed high performance which is close to that of autologous nerve grafts in promoting in vivo PNI regeneration, compared with PCL conduits. The sciatic nerve functional index analysis, electrophysiological examination, and immunological analysis performed to evaluate the functional recovery of the injurious sciatic nerve of rats have indeed proved the favorable effects of CGM/PCL conduits. The result of this study not only aimed to explore CGA's contribution to nerve regeneration but also provided a new strategy for designing and preparing functional NGCs for PNI treatment.
- Published
- 2023
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34. Defective silicotungstic acid-loaded magnetic floral N-doped carbon microspheres for ultra-fast oxidative desulfurization of high sulfur liquid fuels.
- Author
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Liu Y, Yin X, Li C, Xie Z, Zhao F, Li J, Hei J, Han Y, Wang N, and Zuo P
- Abstract
Highly active Keggin-type silicotungstic acid (SiW
12 ) with oxygen vacancy (Ov ) defects was encapsulated into the magnetic floral N-doped carbon microspheres (γ-Fe2 O3 @NC-300) through the facile one-step air pyrolysis of the precursor comprising core-shell Fe3 O4 @polydopamine (Fe3 O4 @PDA) and SiW12 to prepare γ-Fe2 O3 @NC@SiW12 -300. The fabricated catalysts were systematically characterized and subsequently employed for the oxidation desulfurization (ODS) of the model fuel. The magnetic floral γ-Fe2 O3 @NC@SiW12 -300 catalyst exhibited nearly perfect catalytic activity, which under mild conditions could remove 100% amount of 4000 ppm DBT in model fuel within 20 min (0.03 g catalysts and n (H2 O2 )/ n (S) of 2). The catalyst activity is mainly attributed to the high activity SiW12 with the Ov defect and its outstanding dispersibility in γ-Fe2 O3 @NC, along with the high number of exposed active sites. A selected catalyst, γ-Fe2 O3 @NC@SiW12 -300, showed a noticeable turnover frequency (TOF) (110.07 h-1 ) and lower activation energy (38.79 kJ mol-1 ) in oxidative desulfurization (ODS) with good recyclability. HO˙ radical was found to be the active species involved in ODS as confirmed by the EPR and scavenger experiments. Additionally, the fabricated catalyst can be conveniently separated and recycled within an externally applied magnetic field.- Published
- 2023
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35. Tandem phospha -Michael addition/cyclization/dehydration of 2-hydroxychalcones with H -phosphine oxides for the synthesis of 4-phosphorylated 4 H -chromenes.
- Author
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Wen Z, Yang KC, Zheng SL, Zhang YS, Wang SJ, Ni HL, and Chen L
- Abstract
A Hg(OTf)
2 -catalyzed tandem phospha -Michael addition/cyclization/dehydration of 2-hydroxychalcones with H -phosphine oxides is presented. This protocol provides a new and supplementary approach for the preparation of 4-phosphorylated 4 H -chromenes in good yields (up to 99%). In addition, this domino reaction allows the successful construction of two new C-P and C-O bonds in a one-pot operation.- Published
- 2023
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36. Preparation of acid-driven magnetically imprinted micromotors and selective loading of phycocyanin.
- Author
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Yang G, Liu J, Zhang Z, Yuan L, Tian H, and Yang X
- Subjects
- Humans, Motion, Phycocyanin, Proteins
- Abstract
Phycocyanin, a macromolecular protein known for its robust fluorescence, proves to be highly suitable for verifying the successful deposition of imprinted layers. In this study, an acid-propelled magnetic micromotor was successfully fabricated by utilizing surface imprinting and self-propelled nanomotor technology to achieve selective loading and capture of targets such as phycocyanin for future applications in environmental monitoring and precision drug delivery in vivo . This micromotor features a distinct recognition layer achieved through a template electrodeposition method. The outermost imprint layer of the micromotor was meticulously crafted using poly(3,4-ethylenedioxythiophene)/poly(sodium-4-styrenesulfonate) in the presence of a template, while the Pt layer serves as the supportive foundation, the Ni layer acts as the magnetic guidance component, and the innermost layer consists of metal Zn. In acidic environments, the Zn reacts to generate bubbles, which propels the micromotor's motion. The micromotor was comprehensively characterized using techniques such as scanning electron microscopy. Findings highlight the exceptional self-propulsion of the Zn-based micromotor, which is a fusion of molecular imprinting and micromotor technologies. This innovative design achieves an impressive maximum velocity of approximately 100 μm s
-1 , as well as commendable magnetic steering performance. Furthermore, the micromotor demonstrates the ability to imprint target protein through the imprint layer, enabling selective recognition and capture for transport of specific phycocyanin. In vitro cytotoxicity tests have also demonstrated that the micromotors are non-toxic to cells. This breakthrough concept offers a novel avenue for realizing targeted capture and transport of specific nutrients within the human gastric environment.- Published
- 2023
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37. Highly stretchable and self-healing photoswitchable supramolecular fluorescent polymers for underwater anti-counterfeiting.
- Author
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Deng H, Wang H, Tian Y, Lin Z, Cui J, and Chen J
- Abstract
Thanks to the non-destructiveness and spatial-controllability of light, photoswitchable fluorescent polymers (PFPs) have been successfully applied in advanced anti-counterfeiting and information encryption. However, most of them are not suitable for use in harsh underwater environments, including high salinity seawater. In this study, by integrating photochromic molecules into a hydrophobic polymer matrix with the fluorine elastomer, including dipole-dipole interactions, we describe a class of novel photoswitchable supramolecular fluorescent polymers (PSFPs) that can adaptively change their fluorescence between none, green and red by the irradiation of different light. The PSFPs not only exhibited excellent photoswitchable properties, including fast photo-responsibility, prominent photo-reversibility, and photostability, but also exhibited some desired properties, including exceptional stretchability, hydrophobicity, antifouling, self-healing ability, simple preparation process, and processability. We thus demonstrated their applications in underwater data encryption and anti-counterfeiting labels.
- Published
- 2023
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38. Deformability of mouse erythrocytes in different diluents measured using optical tweezers.
- Author
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Shao M, Liu R, Li C, Sun Y, Zhong Z, Lu F, Zhou J, and Zhong MC
- Subjects
- Animals, Mice, Erythrocytes physiology, Elasticity, Plasma, Erythrocyte Deformability, Optical Tweezers
- Abstract
Optical tweezers are widely used to measure the mechanical properties of erythrocytes, which is crucial to the study of pathology and clinical diagnosis of disease. During the measurement, the blood sample is diluted and suspended in an exogenous physiological fluid, which may affect the elastic properties of the cells in vitro . Here, we investigate the effect of different diluents on the elastic properties of mouse erythrocytes by quantitatively evaluating their elastic constants using optical tweezers. The diluents are plasma extracted from mouse blood, veterinary blood diluent (V-52D), Dulbecco's modified Eagle's medium (DMEM), phosphate-buffered saline (PBS), and normal saline (NS). To create an environment that closely resembles in vivo conditions, the experiment is performed at 36.5 °C. The results show that the spring constant of mouse erythrocytes in plasma is 6.23 ± 0.41 μN m
-1 . The elasticity of mouse erythrocytes in V-52D and DMEM is 8.21 ± 0.91 and 6.95 ± 0.85 μN m-1 , which are higher than that in plasma extracted from blood, whereas, the elasticity in PBS and NS is 4.23 ± 0.85 and 4.68 ± 0.79 μN m-1 , which are less than that in plasma extracted from blood. At last, we observe the size and circularity of erythrocytes in different diluents, and consider that the erythrocyte diameter and circularity may affect cell deformability. Our results provide a reference of the diluent choice for measuring the mechanical properties of erythrocytes in vitro .- Published
- 2023
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39. Retraction: A novel TMTP1-modified theranostic nanoplatform for targeted in vivo NIR-II fluorescence imaging-guided chemotherapy for cervical cancer.
- Author
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Alifu N, Ma R, Zhu L, Du Z, Chen S, Yan T, Alimu G, Zhang L, and Zhang X
- Abstract
Retraction of 'A novel TMTP1-modified theranostic nanoplatform for targeted in vivo NIR-II fluorescence imaging-guided chemotherapy for cervical cancer' by Nuernisha Alifu et al. , J. Mater. Chem. B , 2022, 10 , 506-517, https://doi.org/10.1039/D1TB02481G.
- Published
- 2023
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40. Surface hopping simulations on charge separation in an organic donor-acceptor system.
- Author
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Sun Z, Li S, Xie S, Meng Y, and An Z
- Abstract
Charge separation in organic solar cells is a long-lasting and heavily debated issue. Here, we use the surface hopping method based on the Pariser-Parr-Pople (PPP) Hamiltonian and configuration interaction singles (CIS) approximation to simulate the charge separation process in an organic donor-acceptor system. The system is composed of one donor polymer chain and four acceptor polymer chains, and they are all stacked face-to-face. We let the system to relax from a photoexcited state, and then we observed that the electron is transferred from the donor chain to different acceptor chains and the hole is left on the donor chain, forming polaron pairs with different electron-hole distances. By performing statistical analysis on a number of trajectories, we found that the electron and the hole are fully separated before the system relaxes to its lowest excited state. The yield of free charges shows a significant dependence on the donor-acceptor band offset which provides the driving force for charge separation, while showing negligible dependence on the photoexcitation energy. The external electric field has a remarkable effect on the yield of free charges.
- Published
- 2023
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41. Tailoring ionomer distribution in the catalyst layer via heteroatom-functionalization toward superior PEMFC performance.
- Author
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Sun D, Zhao Z, Jin M, and Zhang H
- Abstract
We investigate in detail the influence of O, S, and N functionalization of Pt
3 Co/C catalysts on the proton exchange membrane fuel cell (PEMFC). The results demonstrated that N-functionalization is more beneficial for the distribution of the ionomer in the catalyst layer, resulting in a trade-off between oxygen and hydronium ion transport.- Published
- 2023
- Full Text
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42. Electronic properties, skyrmions and bimerons in Janus CrXY (X, Y = S, Se, Te, Cl, Br, I, and X ≠ Y) monolayers.
- Author
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Guan Z, Shen Z, Xue Y, Zhong T, Wu X, and Song C
- Abstract
Using first-principles calculations, we systematically investigate the electronic properties, chiral skyrmions and bimerons in two-dimensional (2D) Janus CrXY (X, Y = S, Se, Te, Cl, Br, I, and X ≠ Y) monolayers. We found that the categories of nonmagnetic atoms (X and Y in CrXY) determine whether CrXY is a ferromagnetic metal or a semiconductor. Unexpectedly, the CrBrS monolayer of these CrXY materials is a room temperature ferromagnetic semiconductor with a Curie temperature of 303 K, and it possesses an off-plane magnetic anisotropy energy of 0.06 meV. Besides, a strong Dzyaloshinskii-Moriya interaction (DMI) of 3.10 meV is found in CrTeI and is mainly induced by the strong spin-orbit coupling of the nonmagnetic atoms Te(I) rather than that of the magnetic Cr atoms. Furthermore, using micromagnetic simulations, skyrmions can be stabilized in CrSeBr without external magnetic fields. More importantly, the bimerons in CrSeCl with in-plane magnetic anisotropy can be transformed into skyrmions or a ferromagnetic state by controlling the direction of external magnetic fields. Our work investigates fourteen kinds of Janus monolayers, serving as guidelines for materials research on DMI, skyrmions and bimerons.
- Published
- 2023
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43. Tuning the magnetic ordering driven by cationic antisite defects in the Li(ZnMn)As system.
- Author
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Wang M, Tang W, Zhang J, Wang S, Xu J, Wang H, Pang G, Zhang Z, and Lan Z
- Abstract
The electronic structure and magnetic properties of Li(ZnMn)As with antisite defects have been investigated by using first-principles calculations within the Perdew-Burke-Ernzerhof generalized gradient approximation. The cation antisite defect induced by Zn substitution for As was considered. Mn-3d, As-4p, Zn-4s, and Zn-4p were involved in the formation of d-sp hybrid orbitals, which enhanced the non-localized properties of Mn-3d electrons and provided a channel of Mn(↑)-As(↓)-Zn
As (↓)-Mn(↑) for indirect exchange of electrons between the magnetic ions. The antisite defect of Zn-substituted As belonged to the acceptor doping, rendering the compound p-type characteristics. The existence of the extra free hole carriers regulated the magnetic ordering transition. The ferromagnetic coupling between the Mn magnetic dopants was more favorable in the system with an antisite defect. In this paper, a novel type of dilute magnetic semiconductor with controllable carriers was designed and the mechanism of ferromagnetic coupling was revealed, which provided a theoretical reference for the subsequent studies.- Published
- 2023
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44. Correction: A H 2 O 2 self-sufficient nanoplatform with domino effects for thermal-responsive enhanced chemodynamic therapy.
- Author
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Zhang S, Cao C, Lv X, Dai H, Zhong Z, Liang C, Wang W, Huang W, Song X, and Dong X
- Abstract
[This corrects the article DOI: 10.1039/C9SC05506A.]., (This journal is © The Royal Society of Chemistry.)
- Published
- 2023
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- View/download PDF
45. Biomineral-binding liposomes with dual antibacterial effects for preventing and treating dental caries.
- Author
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Luo Z, Lin Y, Zhou X, Yang L, Zhang Z, Liu Z, Zhou M, Jiang J, Wu J, Liu Z, Jing P, and Zhong Z
- Subjects
- Humans, Animals, Rats, Lipopolysaccharides pharmacology, Biofilms, Anti-Bacterial Agents pharmacology, Candida albicans, Streptococcus mutans, Hydroxyapatites, Liposomes pharmacology, Dental Caries drug therapy, Dental Caries prevention & control
- Abstract
Dental caries is a chronic oral disease that results from the demineralization of dental hard tissues caused by the long-term interaction of various pathogenic factors in the human oral cavity. Although magnolol (Mag) and fluconazole (FLC) have shown promising antibacterial activity against Candida albicans ( C. albicans ) and Streptococcus mutans ( S. mutans ), their clinical application is limited due to hydrophobicity. In this study, we constructed biomineral-binding liposomes co-loaded with Mag and FLC (PPi-Mag/FLC-LPs) to overcome the hydrophobicity and achieve a dual antibacterial activity in the acidic microenvironment of caries. PPi-Mag/FLC-LPs were characterized by laser particle size analysis, transmission electron microscopy, and high-performance liquid chromatography (HPLC). The ability of PPi-Mag/FLC-LPs to bind hydroxyapatite was assessed in vitro using fluorescence microscopy and HPLC, while the antibacterial activity was examined by measuring drug effects on the acidogenicity, acid resistance, biofilm formation and survival of C. albicans and S. mutans . The pharmacodynamics of PPi-Mag/FLC-LPs was also evaluated in vivo in a rat model of dental caries. Mag and FLC were released rapidly from PPi-Mag/FLC-LPs in a pH-sensitive manner, and they bound effectively to hydroxyapatite, leading to a better antibacterial effect on C. albicans and S. mutans compared to free drugs or liposomes loaded with a single drug. PPi-Mag/FLC-LPs improved the medicinal properties of Mag and FLC and provided a rapid, pH-sensitive release of both drugs in vitro . PPi-Mag/FLC-LPs displayed good antibacterial activity in vivo , showing promise as a dual-drug delivery system for the prevention and treatment of caries.
- Published
- 2023
- Full Text
- View/download PDF
46. Molecular imprinting-based ratiometric fluorescence sensors for environmental and food analysis.
- Author
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Wen Y, Sun D, Zhang Y, Zhang Z, Chen L, and Li J
- Subjects
- Humans, Spectrometry, Fluorescence methods, Food Analysis, Food Safety, Quantum Dots, Molecular Imprinting methods
- Abstract
Environmental protection and food safety are closely related to the healthy development of human society; there is an urgent need for relevant analytical methods to determine environmental pollutants and harmful substances in food. Molecular imprinting-based ratiometric fluorescence (MI-RFL) sensors, constructed by combining molecular imprinting recognition and ratiometric fluorescence detection, possess remarkable advantages such as high selectivity, anti-interference ability, high sensitivity, non-destruction and convenience, and have attracted increasing interest in the field of analytical determination. Herein, recent advances in MI-RFL sensors for environmental and food analysis are reviewed, aiming at new construction strategies and representative determination applications. Firstly, fluorescence sources and possible sensing principles are briefly outlined. Secondly, new imprinting techniques and dual/ternary-emission fluorescence types that improve sensing performances are highlighted. Thirdly, typical analytical applications of MI-RFL sensors in environmental and food samples are summarized. Lastly, the challenges and perspectives of the MI-RFL sensors are proposed, focusing on improving sensitivity/visualization and extending applications.
- Published
- 2023
- Full Text
- View/download PDF
47. The effect of the intramolecular disorder on hot exciton dynamics in polymer solar cells.
- Author
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Zhang M, Lu Q, Liu X, and An Z
- Abstract
In polymer solar cells (PSCs), the contribution of hot excitons to charge generation is strongly limited by their relatively low yield and ultrafast internal conversion (IC) process. In recent years, different strategies have been proposed to modulate the hot exciton dynamics, but a direct correlation between the microscopic properties of the polymer and hot exciton dynamics is still not completely clear. Here, we theoretically investigate the effect of intramolecular disorder, including the diagonal disorder (DD) and off-diagonal disorder (ODD), on the hot exciton dynamics based on the tight-binding model calculations. We find that the effect of ODD on the hot exciton yield is more significant than that of DD. In addition, we find that the IC relaxation time of hot excitons depends nonmonotonically on the intensity of DD and ODD, indicating that the intramolecular disorder can modulate the competitive relationship between the spontaneous dissociation of hot excitons and the IC process. This work provides a guide for promoting charge generation in PSCs dominated by hot exciton dissociation.
- Published
- 2023
- Full Text
- View/download PDF
48. CD38-selective immuno-nano-DM1 conjugates for depleting multiple myeloma.
- Author
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Yuan Q, Fan D, Zhang Y, Yue S, Cheng R, Zhong Z, and Sun H
- Subjects
- Mice, Animals, ADP-ribosyl Cyclase 1, Cell Line, Tumor, Multiple Myeloma drug therapy, Multiple Myeloma pathology, Hematologic Neoplasms
- Abstract
Multiple myeloma (MM) is a neoplasm of aberrant plasma cells and ranks second among hematologic malignancies. Despite a substantial improvement in clinical outcomes with advances in therapeutic modalities over the past two decades, MM remains incurable, necessitating the development of new and potent therapies. Herein, we engineered a daratumumab-polymersome-DM1 conjugate (DPDC) based highly potent and CD38-selective immuno-nano-DM1 toxin for depleting MM cells in vivo . DPDC with controllable daratumumab density and disulfide-linked DM1 is of small size (51-56 nm), with high stability and reduction-triggered DM1 release. D
6.2 PDC potently inhibited the proliferation of CD38-overexpressed LP-1 and MM.1S MM cells with IC50 values of 2.7 and 1.2 ng DM1 equiv. per mL, about 4-fold stronger than non-targeted PDC. Moreover, D6.2 PDC effectively and safely depleted LP-1-Luc MM cells in an orthotopic mouse model at a low DM1 dosage of 0.2 mg kg-1 , thus alleviating osteolytic bone lesion and extending the median survival by 2.8-3.5-fold compared to all controls. This CD38-selective DPDC provides a safe and potent treatment strategy for MM.- Published
- 2023
- Full Text
- View/download PDF
49. Macrocyclization via remote meta -selective C-H olefination using a practical indolyl template.
- Author
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Zhang P, Jiang Z, Fan Z, Li G, Ma Q, Huang J, Tang J, Xu X, Yu JQ, and Jin Z
- Abstract
The synthesis of macrocyclic compounds with different sizes and linkages remains a great challenge via transition metal-catalysed intramolecular C-H activation. Herein, we disclose an efficient macrocyclization strategy via Pd-catalysed remote meta -C-H olefination using a practical indolyl template. This approach was successfully employed to access macrolides and coumarins. In addition, the intermolecular meta -C-H olefination also worked well and was exemplified by the synthesis of antitumor drug belinostat from inexpensive and readily available benzenesulfonyl chloride. Notably, catalytic copper acetate and molecular oxygen were used in place of silver salts as oxidants. Furthermore, for the first time, the formation of a macrocyclophane cyclopalladated intermediate was detected through in situ Fourier-transform infrared monitoring experiments and ESI-MS., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)
- Published
- 2023
- Full Text
- View/download PDF
50. Tumor-homing bacterium-adsorbed liposomes encapsulating perfluorohexane/doxorubicin enhance pulsed-focused ultrasound for tumor therapy.
- Author
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Ou X, Zhang Z, Lin L, Du Y, Tang Y, Wang Y, and Zou J
- Abstract
Objective : To make up for the insufficient ultrasound ablation of tumors, the energy output or synergist is increased but faces the big challenge of normal tissue damage. In this study, we report a tumor-homing bacterium, Bifidobacterium bifidum ( B. bifidum ), adsorbing liposomes that encapsulate perfluorohexane (PFH) and doxorubicin (DOX) to enhance the pulsed-focused ultrasound (PFUS) for tumor therapy, so as to improve the efficacy, safety and controllability of ultrasound treatment. Methods : The PFH and DOX co-loaded cationic liposomal nanoparticles (CL-PFH-DOX-NPs) were prepared for ultrasound (US) imaging, cell-killing, and B. bifidum adsorption for the reactive oxygen species (ROS) testing. The aggregation of B. bifidum and CL-PFH-DOX-NPs is called tumor-homing aggregation ( B. bifidum @CL-PFH-DOX-NPs) in this study, and the synergistic effects of B. bifidum @CL-PFH-DOX-NPs were analyzed in vivo . Results : Comprehensive studies validated that CL-PFH-DOX-NPs can enhance US imaging and cell-killing and B. bifidum can promote ROS, and B. bifidum @CL-PFH-DOX-NPs achieve PFUS synergism in vivo . Importantly, active homing of B. bifidum facilitated the delivery and retention of CL-PFH-DOX-NPs in tumors, reducing dispersion in normal tissues, achieving the targeting ability of B. bifidum @CL-PFH-DOX-NPs. The best sonication time was chosen according to the distribution of CL-PFH-DOX-NPs in vivo to achieve efficient therapy. Especially, B. bifidum @CL-PFH-DOX-NPs amplified cavitation and the immune-boosting effects. Conclusion : Multifunctional B. bifidum @CL-PFH-DOX-NPs were successfully constructed with well targeting, which not only realized US imaging monitoring, strong cavitation and complementary killing during PFUS, but also achieved immunity enhancement after PFUS. The combination of PFUS, B. bifidum and CL-PFH-DOX-NPs provides a new idea for the potential application of ultrasound therapy in solid tumors., Competing Interests: All authors declare that they have no competing interests., (This journal is © The Royal Society of Chemistry.)
- Published
- 2023
- Full Text
- View/download PDF
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