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Molecular simulation study on the evolution process of hydrate residual structures into hydrate

Chinese Journal of Chemical Engineering 2024年第5期69卷 79-91页

作者： liwei cheng Yunfei Li Jinlong Cui Huibo Qin Fulong Ning Bei Liu Guangjin chen Faculty of Engineering China University of GeosciencesWuhan 430074China State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China College of Science Nanchang Institute of TechnologyNanchang 330099China School of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China National Center for International Research on Deep Earth Drilling and Resource Development China University of Geosciences(Wuhan)Wuhan 430074China

The clathrate hydrate memory effect is a fascinating phenomenon with potential applications in carbon capture,utilization and storage(CCUS),gas separation,and gas storage as it can accelerate the secondary formation of clathrate hydrate.However,the underlying mechanism of this effect remains unclear.To gain a better understanding of the mechanism,we conducted molecular dynamic simulations to simulate the initial formation and reformation processes of methane hydrate.In this work,we showed the evolution process of hydrate residual structures into hydrate cages.The simulation results indicate that the residual structures are closely related to the existence of hydrate memory effect,and the higher the contribution of hydrate dissociated water to the hydrate nucleation process,the faster the hydrate nucleation.After hydrate dissociation,the locally ordered structures still exist after hydrate dissociation and can promote the formation of cluster structures,thus accelerating hydrate nucleation.Additionally,the nucleation process of hydrate and the formation process of clusters are inseparable.The size of clusters composed of cup-cage structures is critical for hydrate nucleation.The residence time at high temperature after hydrate decomposition will affect the strength of the hydrate memory effect.Our simulation results provide microscopic insights into the occurrence of the hydrate memory effect and shed light on the hydrate reformation process at the molecular scale.

关键词： Memory effect Molecular simulation Hydrate reformation Residual structures

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Advanced Strategies for Overcoming Endosomal/Lysosomal Barrier in Nanodrug Delivery

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Research 2024年第1期2023卷 315-337页

作者： Chong Qiu Fei Xia Junzhe Zhang Qiaoli Shi Yuqing Meng chen Wang Huanhuan Pang liwei Gu chengchao Xu Qiuyan Guo Jigang Wang Artemisinin Research Center and Institute of Chinese Materia MedicaChina Academy of Chinese Medical SciencesBeijing 100700China Department of Nephrology and Shenzhen Clinical Research Centre for GeriatricsShenzhen People's HospitalThe First Affiliated HospitalSouthern University of Science and TechnologyShenzhenGuangdong 518020China

Nanocarriers have therapeutic potential to facilitate drug delivery,including biological agents,smallmolecule drugs,and nucleic acids.However,their efficiency is limited by several factors;among which,endosomal/lysosomal degradation after endocytosis is the most important.This review summarizes advanced strategies for overcoming endosomal/lysosomal barriers to efficient nanodrug delivery based on the perspective of cellular uptake and intracellular transport mechanisms.These strategies include promoting endosomal/lysosomal escape,using non-endocytic methods of delivery to directly cross the cell membrane to evade endosomes/lysosomes and making a detour pathway to evade endosomes/lysosomes.On the basis of the findings of this review,we proposed several promising strategies for overcoming endosomal/lysosomal barriers through the smarter and more efficient design of nanodrug delivery systems for future clinical applications.

关键词： somal drugs finding

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Direct observation of oxygen vacancy formation and migration over ceria surface by in situ environmental transmission electron microscopy

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Journal of Rare Earths 2024年第4期42卷 676-682页

作者： Dawei Pang Wei Li Ningqiang Zhang Hong He Shengcheng Mao Yanhui chen liwei Cao Chong Li Ang Li Xiaodong Han Beijing Key Laboratory of Solid Microstructure and Properties Department of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Beijing Key Laboratory for Green Catalysis and Separation The Faculty of Environment and LifeBeijing University of TechnologyBeijing10124China International Joint Research Laboratory for Quantum Functional Materials of Henan School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou450001China

The extremely high structural tolerance of ceria to oxygen vacancies(Ov)has made it a desirable catalytic material for the hydrocarbon oxidation to chemicals and pharmaceuticals and the reduction of gaseous pollutants.It is proposed that the formation and diffusion of Ov originate from its outstanding reduction property.However,the formation and diffusion process of Ov over the surface of ceria at the atomic level is still unknown.Herein,the structural and valence evolution of CeO_(2)(111)surfaces in reductive,oxidative and vacuum environments from room temperature up to 700℃was studied with in situ aberration-corrected environmental transmission electron microscopy(ETEM)experiments.Ov is found to form under a high vacuum at elevated temperatures;however,the surface can recover to the initial state through the adsorption of oxygen atoms in an oxygen-contained environment.Furthermore,in hydrogen environment,the step-CeO_(2)(111)surface is not stable at elevated temperatures;thus,the steps tend to be eliminated with increasing temperature.Combined with first-principles density function calculations(DFT),it is proposed that O-terminated surfaces would develop in a hypoxic environment due to the dynamic diffusion of Ov from the outer surface to the subsurface.Furthermore,in a reductive environment,H2 facilitates the formation and diffusion of Ov while Ce-terminated surfaces develope.These results reveal dynamic atomic-scale interplay between the nanoceria surface and gas,thereby providing fundamental insights into the Ov-dependent reaction of nano-CeO_(2) during catalytic processes.

关键词： Ceria Direct observation In situ ETEM Oxygen vacancy Density function calculations Rareearths

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Aberration correction for deformable-mirror-based remote focusing enables high-accuracy whole-cell super-resolution imaging

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Photonics Research 2024年第4期12卷 821-832页

作者： WEI SHI YINGCHUAN HE JIANLIN WANG LULU ZHOU JIANWEI chen liwei ZHOU ZEYU XI ZHEN WANG KE FANG YIMING LI Department of Biomedical Engineering Southern University of Science and TechnologyShenzhen 518055China

Single-molecule localization microscopy(SMLM)enables three-dimensional(3D)investigation of nanoscale structures in biological samples,offering unique insights into their organization.However,traditional 3D super-resolution microscopy using high numerical aperture(NA)objectives is limited by imaging depth of field(DOF),restricting their practical application to relatively thin biological samples.Here,we developed a unified solution for thick sample super-resolution imaging using a deformable mirror(DM)which served for fast remote focusing,optimized point spread function(PSF)engineering,and accurate aberration correction.By effectively correcting the system aberrations introduced during remote focusing and sample aberrations at different imaging depths,we achieved high-accuracy,large DOF imaging(~8μm)of the whole-cell organelles[i.e.,nuclear pore complex(NPC),microtubules,and mitochondria]with a nearly uniform resolution of approximately 35 nm across the entire cellular volume.

关键词： enable mirror resolution

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Genesis of the Nuri Cu-W-Mo Deposit,Tibet,China:Constraints from in situ Trace Elements and Sr Isotopic Analysis of Scheelite

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Acta Geologica Sinica(English Edition) 2024年第1期98卷 117-131页

作者： WANG Yiyun WU Zhishan chen Wenqing DU Qing’an TANG liwei SHI Hongzhao MA Guotao ZHANG Zhi LIANG Wei WU Bo MIAO Hengyi chengdu Center China Geological Survey(Geoscience Innovation Center of Southwest China)Chengdu 610081China The Second Geological Institute of China’s Metallurgical Geology Bureau Fuzhou 351111China

The Nuri deposit is the only Cu-W-Mo polymetallic deposit with large-scale WO3 resources in the eastern section of the Gangdese metallogenic belt,Tibet,China.However,the genetic type of this deposit has been controversial since its discovery.Based on a study of the geological characteristics of the deposit,this study presents mineralization stages,focusing on the oxide stage and the quartz-sulfide stage where scheelite is mainly formed,referred to as Sch-A and Sch-B,respectively.Through LA-ICP-MS trace element and Sr isotope analyses,the origin,evolutionary process of the oreforming fluid and genesis of the ore deposit are investigated.Scanning Electron Microscope-Cathodoluminescence(SEMCL)observations reveal that Sch-A consists of three generations,with dark gray homogenous Sch-A1 being replaced by relatively lighter and homogeneous Sch-A2 and Sch-A3,with Sch-A2 displaying a gray CL image color with vague and uneven growth bands and Sch-A3 has a light gray CL image color with hardly any growth band.In contrast,Sch-B exhibits a‘core-rim’structure,with the core part(Sch-B1)being dark gray and displaying a uniform growth band,while the rim part(Sch-B2)is light gray and homogeneous.The normalized distribution pattern of rare earth elements in scheelite and Sr isotope data suggest that the early ore-forming fluid in the Nuri deposit originated from granodiorite porphyry and,later on,some country rock material was mixed in,due to strong water-rock interaction.Combining the O-H isotope data further indicates that the ore-forming fluid in the Nuri deposit originated from magmatic-hydrothermal sources,with contributions from metamorphic water caused by water-rock interaction during the mineralization process,as well as later meteoric water.The intense water-rock interaction likely played a crucial role in the precipitation of scheelite,leading to varying Eu anomalies in different generations of scheelite from the oxide stage to the quartz-sulfide stage,while also causing a gradual decrease in oxygen fugacity(fO2)and a sl

关键词： trace elements in situ Sr isotopes tungsten mineralization Gangdese metallogenic belt Tibet

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CO_(2)electrolysis:Advances and challenges in electrocatalyst engineering and reactor design

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Materials Reports(Energy) 2023年第2期3卷 82-102,I0003页

作者： Jiayi Lin Yixiao Zhang Pengtao Xu liwei chen School of Chemistry and Chemical Engineering In-Situ Center for Physical SciencesShanghai Electrochemical Energy Device Research Center(SEED)Shanghai Jiao Tong UniversityShanghai200240China Frontiers Science Center for Transformative Molecules Shanghai Jiao Tong UniversityShanghai200240China

Electrochemical reduction of CO_(2)(CO_(2)RR)coupled with renewable electrical energy is an attractive way of upgrading CO_(2)to value-added chemicals and closing the carbon cycle.However,CO_(2)RR electrocatalysts still suffer from high overpotential,and the complex reaction pathways of CO_(2)RR often lead to mixed products.Early research focuses on tuning the binding of reaction intermediates on electrocatalysts,and recent efforts have revealed that the design of electrolysis reactors is equally important for efficient and selective CO_(2)RR.In this review,we present an overview of recent advances and challenges toward achieving high activity and high selectivity in CO_(2)RR at ambient conditions,with a particular focus on the progress of CO_(2)RR electrocatalyst engineering and reactor design.Our discussion begins with three types of electrocatalysts for CO_(2)RR(noble metalbased,none-noble metal-based,and metal-free electrocatalysts),and then we examine systems-level strategies toward engineering specific components of the electrolyzer,including gas diffusion electrodes,electrolytes,and polymer electrolyte membranes.We close with future perspectives on catalyst development,in-situ/operando characterization,and electrolyzer performance evaluation in CO_(2)RR studies.

关键词： Carbon dioxide utilization Carbon dioxide electrochemical reduction Electrocatalyst design Electrolyzer design Gas diffusion electrodes Electrolyte effects Polymer electrolyte membranes

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Review—Lithium Carbon Composite Material for Practical Lithium Metal Batteries

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Chinese Journal of Chemistry 2023年第7期41卷 814-824页

作者： Lei Zheng Ruowei Yi Nan Zheng Yanbin Shen liwei chen School of Nano-Tech and Nano-Bionics University of Science and Technology of ChinaHefeiAnhui230026 China i-Lab CAS Center for Excellence in NanoscienceSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhouJiangsu215123 China in-situ Center for Physical Science School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai200240 China

Comprehensive Summary Lithium(Li)metal is considered ideal for high-energy-density batteries due to its extremely high specific capacity and low electrochemical potential.However,uncontrolled Li dendrite growth and interfacial instability during repeated Li plating/stripping have limited the practical applicability of Li metal batteries(LMBs).Over the past decades,substantial efforts have been devoted to solving the challenges associated with Li metal anodes.Our research team has developed several Li-carbon(Li-C)microsphere composites in recent years to suppress the formation of Li dendrites and achieve a decent cycle life.In this account,we summarize our advances in the design and application of Li-C composites,which include the developments in the structure and chemical composition of high-specific-capacity Li-C composites,strategies for surface passivation of the micro-spherical Li-C composites,and applications of the Li-C composite in next-generation high-energy-density Li-ion,Li-air,and solid-state LMBs.Finally,we discuss future perspectives for developing high-performance Li metal anodes and endeavors to realize the practical applications of LMBs.

关键词： Li anode High-energy-density Li metal batteries Li dendrites Li-carbon composite Artificial coating Interfaces Hierarchical nanostructures

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Dynamic changes in butyrate levels regulate satellite cell homeostasis by preventing spontaneous activation during aging

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Science China(Life Sciences) 2024年第4期67卷 745-764页

作者： Shujie chen Liujing Huang Bingdong Liu Huimin Duan Ze Li Yifan Liu Hu Li Xiang Fu Jingchao Lin Yinlan Xu Li Liu Dan Wan Yulong Yin liwei Xie Department of Endocrinology and Metabolism Zhujiang HospitalSouthern Medical UniversityGuangzhou 510280China State Key Laboratory of Applied Microbiology Southern China Guangdong Provincial Key Laboratory of Microbial Culture Collection and ApplicationGuangdong Open Laboratory of Applied MicrobiologyInstitute of MicrobiologyGuangdong Academy of SciencesGuangzhou 510070China School of Public Health Xinxiang Medical UniversityXinxiang 453003China Department of Infectious Diseases Nanfang HospitalSouthern Medical UniversityGuangzhou 510515China Metabo-Profile Biotechnology(Shanghai)Co.Ltd. Shanghai 201315China Institute of Aging Research Guangdong Provincial Key Laboratory of Medical Molecular DiagnosticsSchool of Medical TechnologyGuangdong Medical UniversityDongguan 524023China Department of Rehabilitation Medicine Nanfang HospitalSouthern Medical UniversityGuangzhou 510000China Laboratory of Animal Nutritional Physiology and Metabolic Process Key Laboratory of Agro-ecological Processes in Subtropical RegionInstitute of Subtropical AgricultureChinese Academy of SciencesChangsha 410125China Bioland Laboratory Guangzhou Regenerative Medicine and Health Guangdong LaboratoryGuangzhou 510005China

The gut microbiota plays a pivotal role in systemic metabolic processes and in particular functions,such as developing and preserving the skeletal muscle system.However,the interplay between gut microbiota/metabolites and the regulation of satellite cell(SC)homeostasis,particularly during aging,remains elusive.We propose that gut microbiota and its metabolites modulate SC physiology and homeostasis throughout skeletal muscle development,regeneration,and aging process.Our investigation reveals that microbial dysbiosis manipulated by either antibiotic treatment or fecal microbiota transplantation from aged to adult mice,leads to the activation of SCs or a significant reduction in the total number.Furthermore,employing multi-omics(e.g.,RNA-seq,16S r RNA gene sequencing,and metabolomics)and bioinformatic analysis,we demonstrate that the reduced butyrate levels,alongside the gut microbial dysbiosis,could be the primary factor contributing to the reduction in the number of SCs and subsequent impairments during skeletal muscle aging.Meanwhile,butyrate supplementation can mitigate the antibiotics-induced SC activation irrespective of gut microbiota,potentially by inhibiting the proliferation and differentiation of SCs/myoblasts.The butyrate effect is likely facilitated through the monocarboxylate transporter 1(Mct1),a lactate transporter enriched on membranes of SCs and myoblasts.As a result,butyrate could serve as an alternative strategy to enhance SC homeostasis and function during skeletal muscle aging.Our findings shed light on the potential application of microbial metabolites in maintaining SC homeostasis and preventing skeletal muscle aging.

关键词： gut microbiota aging satellite cells butyrate Slc16a1(Mct1)

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Insight on metal ions inducing chiral self-assembly of DNA in silica mineralization

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Nano Research 2023年第3期16卷 3998-4003页

作者： Arepati Azhati Lu Han Zhibei Qu Zhouhong Ren Xi Liu liwei chen Shunai Che School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Metal Matrix CompositesShanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240China School of Chemical Science and Engineering Tongji UniversityShanghai 200092China Department of Medicinal Chemistry School of PharmacyFudan UniversityShanghai 201203China School of Chemical Science and Engineering In-situ Center for Physical SciencesFrontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China

The self-assembly of DNA provides an attractive approach to understanding structural formation mechanism in living organisms and to assisting applications in materials chemistry.Herein,we investigated the effect of metal ions on chiral self-assembly of DNA through the synthesis of chiral mesostructured silica via self-assembly of metal ions,DNA,and silica source.31 types of multivalent cationic metal ions were found to induce formation of chiral impeller-like DNA-silica complexes due to the chiral stacking of DNA.The strength of the interaction between the metal ion and phosphate group of DNA was speculated for the chiral stacking of DNA due to close distance of adjacent DNA to assure mutual recognition.Theoretical calculations indicated that chiral packing of DNA depends on the stability of the bridging phosphate-metal ion-phosphate bonds of DNA based on electron delocalization in d-orbital conjugation of metal ions.

关键词： chirality DNA DNA-metal ions interaction silica ultra-small metal-nanoparticle

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Interface-enhanced thermoelectric output power in CrN/SrTiO_(3-x) heterostructure

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Journal of Energy Chemistry 2022年第1期31卷 16-22,I0002页

作者： Xueying Wan Xiaowei Lu Lin Sun Mingyu chen Na Ta Wei Liu Qi chen liwei chen Jian He Peng Jiang Xinhe Bao State Key Laboratory of Catalysis CAS Center for Excellence in NanoscienceDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina i-Lab Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123jiangsuChina Department of Physics and Astronomy Clemson UniversityClemson 29634-0978USA

Thermoelectric devices enable direct conversion between thermal and electrical energy.Recent studies have indicated that the thin film/substrate heterostructure is effective in achieving high thermoelectric performance via decoupling the Seebeck coefficient and electrical conductivity otherwise adversely inter-dependent in homogenous bulk materials.However,the mechanism underlying the thin film/substrate heterostructure thermoelectricity remains unclear.In addition,the power output of the thin film/substrate heterostructure is limited to the nanowatt scale to date,falling short of the practical application requirement.Here,we fabricated the CrN/SrTiO_(3-x) heterostructures with high thermoelectric output power and outstanding thermal stability.By varying the CrN film thickness and the reduction degree of CrN/SrTiO_(3-x) substrate,the optimized power output and the power density have respectively reached 276μWand 10^(8) mW/cm^(2) for the 30 nm CrN film on a highly reduced surface of CrN/SrTiO_(3-x) under a temperature difference of 300 K.The performance enhancement is attributed to the CrN/CrN/SrTiO_(3-x) heterointerface,corroborated by the band bending as revealed by the scanning Kelvin probe microscopy.These results will stimulate further research efforts towards interface thermoelectrics.

关键词： SrTi0_(3-x) CrN Heterostructure Interface thermoelectrics Thin film

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