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Apically guiding electron/mass transfer reaction induced by Ag/FeN_(x)Mott-Schottky effect within a hollow star reactor toward high performance zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 106-116,I0004页

作者： Kaixiang Shi Kaixin Wang Tong Li Junhao Li Jie Ren Xu Li Yonggang Min Zhouguang Lu Wei Tan Quanbing Liu Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center(Rongjiang Laboratory) Guangdong University of TechnologyJieyang 515200GuangdongChina Guangzhou Key Laboratory of Clean Transportation Energy Chemistry Guangdong Provincial Key Laboratory of Plant Resources BiorefinerySchool of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006GuangdongChina Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province School of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou 571158HainanChina School of Materials and Energy Guangdong University of TechnologyGuangzhou 510006GuangdongChina Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055GuangdongChina

The disparity in the transfer of carriers(electrons/mass)during the reaction in zinc-air batteries(ZABs)results in sluggish kinetics of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),along with elevated overpotentials,thereby imposing additional constraints on its ***,the pre-design and target-development of inexpensive,high-performance,and long-term stable bifunctional catalysts are urgently *** this work,an apically guiding dual-functional electrocatalyst(Ag-FeN_(x)-N-C)was prepared,in which a hierarchical porous nitrogen-doped carbon with three-dimensional(3D)hollow star-shaped structure is used as a substrate and high-conductivity Ag nanoparticles are coupled with iron nitride(FeN_(x))*** calculations indicate that the Mott-Schottky heterojunction as an inherent electric field comes from the two-phase bound of Ag and FeN_(x),of which electron accumulation in the FeN_(x)phase region and electron depletion in the Ag phase region promote orientated-guiding charge *** effective modulation of local electronic structures felicitously reforms the d-band electron-group distribution,and intellectually tunes the masstransfer reaction energy barriers for both ORR/***,the hollow star-s haped hierarchical porous structure provides an apical region for fast mass *** results show that the halfwave potential for ORR is 0.914 V,and the overpotential for OER is only 327 mV at 10 mA cm^(-2).A rechargeable ZAB with Ag-FeN_(x)-N-C as the air cathode demonstrates long-term cycling performance exceeding 1500 cycles(500 h),with a power density of 180 mW cm^(-2).Moreover,when employing AgFeN_(x)-N-C as the air cathode,flexible ZABs demonstrate a notable open-circuit voltage of 1.42 V and achieve a maximum power density of 65.6 mW cm^(-2).Ag-FeN_(x)-N-C shows guiding electron/mass transfer route and apical reaction microenvironment for the electrocatalyst architecture in the explo

关键词： Hollow star structure Mott-Schottky effect Apically guiding effect Bifunctional catalysis Zinc-air batteries

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Heat preservation,antifouling,hemostatic and antibacterial aerogel wound dressings for emergency treatment

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Frontiers of Materials Science 2023年第2期17卷 93-103页

作者： Fangling Li Xiaoman Han Dongdong Cao Junxia Yin Li Chen Dongmei Li Lin Cui Zhiyong Liu Xuhong Guo School of Chemistry and Chemical Engineering Shihezi UniversityShihezi 832003China Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan Shihezi 832003China School of Biomedical Engineering Faculty of Electronic Information and Electrical EngineeringDalian University of TechnologyDalian 116024China School of Medicine Shihezi UniversityShihezi 832003China State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China

Hemostatic dressings with multiple functions are superior to current hemostatic dressings for use in the complex situation of emergency *** particular,the existing dressings lack consideration for the prevention of hypothermic shock after massive *** this study,gelatin(GN)and oxidized pectin(OP)were used for Schiff base cross-linking,and then polyvinyl alcohol(PVA)solution mixed with hemostatic caffeic acid(CA)was introduced to obtain aerogel substrate material(CB)after ***(PDMS)and silver nanowires(Ag NWs)were used to construct a hydrophobic layer,an antibacterial layer and an infrared reflective layer on both sides of CB to prepare a multifunctional aerogel wound dressing with heat preservation,antifouling,hemostasis and antibacterial properties(PDMS-Ag NW-CB).The results showed that the infrared transmittance of PDMS-Ag NW-CB is almost 0,so that thermal energy loss from the body is *** contact angles with water and blood are 129°and 120°,respectively,which have the effect of *** dressing can absorb blood quickly within 10 min,adhere to and gather platelets,and achieve *** has good antibacterial and ***,PDMS-Ag NW-CB has great potential in application to emergency treatment.

关键词： heat preservation hemostasis antifouling antibacterial wound dressing

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Theoretical analysis of hydrogen solubility in direct coal liquefaction solvents

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International Journal of Coal Science & technology 2024年第2期11卷 187-197页

作者： Xiaobin Zhang Aoqi Wang Xingbao Wang Wenying Li State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024ShanxiChina College of Chemical Engineering and Technology Taiyuan University of TechnologyTaiyuan 030024China

The cyclic hydrogenation technology in a direct coal liquefaction process relies on the dissolved hydrogen of the solvent or oil participating in the hydrogenation ***,a theoretical basis for process optimization and reactor design can be established by analyzing the solubility of hydrogen in liquefaction *** studies of hydrogen solubility in liquefaction solvents are challenging due to harsh reaction conditions and complex solvent *** this study,the composition and content of liquefied solvents were *** model compounds,hexadecane,toluene,naphthalene,tetrahydronaphthalene,and phenanthrene were chosen to represent the liquefied solvents in chain alkanes and monocyclic,bicyclic,and tricyclic aromatic *** solubility of hydrogen X(mol/mol)in pure solvent components and mixed solvents(alkanes and aromatics mixed in proportion to the chain alkanes+bicyclic aromatic hydrocarbons,bicyclic saturated aromatic hydrocarbons+bicyclic aromatic hydrocarbons,and bicyclic aromatic hydrocarbons+compounds containing het-eroatoms composed of mixed components)are determined using Aspen simulation at temperature and pressure conditions of 373–523 K and 2–10 *** results demonstrated that at high temperatures and pressures,the solubility of hydrogen in the solvent increases with the increase in temperature and pressure,with the pressure having a greater ***-more,the results revealed that hydrogen is more soluble in straight-chain alkanes than in other solvents,and the solubility of eicosanoids reaches a maximum of *** hydrogen solubility in aromatic ring compounds decreased gradually with an increase in the aromatic ring *** influence of chain alkanes on the solubility of hydrogen predominates in a mixture of solvents with different mixing ratios of chain alkanes and aromatic *** solubility of hydrogen in mixed aromatic solvents is less than that in the corresponding single ***

关键词： Direct coal liquefaction Liquefaction solvents Process simulation Hydrogen solubility

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Suppressing high voltage chemo-mechanical degradation in single crystal nickel-rich cathodes for high-performance all-solid-state lithium batteries

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Journal of Energy Chemistry 2025年第3期102卷 377-385页

作者： Yirong Xiao Le Yang Chaoyuan Zeng Ze Hua Shuangquan Qu Niaz Ahmad Ruiwen Shao Wen Yang Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Advanced Innovation Center for Intelligent Robots and Systems School of Medical TechnologyBeijing Institute of TechnologyBeijing 100081China School of Chemistry and Chemical Engineering Key Laboratory of Ministry of Education for Advanced Materials in Tropical Island ResourcesCollaborative Innovation Center of Ecological CivilizationHainan UniversityHaikou 570228HainanChina

Sulfide-based all-solid-state lithium batteries suffer from electrochemo-mechanical damage to Ni-rich oxide-based cathode active materials(CAMs),primarily caused by severe volume changes,results in significant stress and strain,causes micro-cracks and interfacial contact loss at potentials>4.3 V(***/Li^(+)).Quantifying micro-cracks and voids in CAMs can reveal the degradation mechanisms of Ni-rich oxidebased cathodes during electrochemical ***,the origin of electrochemical-mechanical damage remains ***,We have developed a multifunctional PEG-based soft buffer layer(SBL)on the surface of carbon black(CB).This layer functions as a percolation network in the single crystal LiNi_(0.83)Co_(0.07)Mn_(0.1)O_(2)and Li_(6)PS_(5)Cl composite cathode layer,ensuring superior ionic conductivity,reducing void formation and particle cracking,and promoting uniform utilization of the cathode active material in all-solid-state lithium batteries(ASSLBs).High-angle annular dark-field STEM combined with nanoscale X-ray holo-tomography and plasma-focused ion beam scanning electron microscopy confirmed that the PEG-based SBL mitigated strain induced by reaction heterogeneity in the *** strain produces lattice stretches,distortions,and curved transition metal oxide layers near the surface,contributing to structural degradation at elevated ***,ASSLBs with a LiNi_(0.83)Co_(0.07)Mn_(0.1)O_(2)cathode containing LCCB-10(CB/PEG mass ratio:100/10)demonstrate a high areal capacity(2.53 mAh g^(-1)/0.32 mA g^(-1))and remarkable rate capability(0.58 mAh g^(-1)at 1.4 mA g^(-1)),with88%capacity retention over 1000 cycles.

关键词： Single crystal nickel-rich oxide cathode Lattice stretches and distortions Reaction heterogeneity Percolation network All-solid-state lithium batteries

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Tetraphenylethylene-derived organic cages with persistent photogenic radicaloids and efficient photothermal conversion

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Science China Chemistry 2025年第2期68卷 661-669页

作者： Suqiong Yan Bo Yang Fanda Feng Yuan Zhang Shirong Ban Hui Ma Wei Huang State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China Shenzhen Research Institute of Nanjing University Shenzhen 518057China

Transformation of the electronic spin states has received significant interest in recent years because of its applications in the magnetic information storage materials and optical response ***,it can be formidably challenging to use ultraviolet(UV)light as a contactless stimulus to alter the electronic spin states of the supramolecular *** by the approach on the radical cation mechanism of the Scholl reaction and the photocyclization reactivity of tetraphenylethylene(TPE)derivatives,we report two photochromic cages(cage-TPE-1 and cage-TPE-2)that can be photochemically transformed from electron paramagnetic resonance(EPR)-silent to EPR-active form via UV irradiation due to the photo-induced electron transfer process at the TPE *** provided a strong single-electron signal with a g value of 2.003 in cage-TPE-1 and cage-TPE-2 but no signal was detected for the pristine samples without the *** transformation can be monitored by ultraviolet–visible–near-infrared(UV–vis–NIR)and photoluminescence(PL)*** photogenic radical cage intermediate was unstable in solution resulting in the degradation and intramolecular cyclization of the reactive species,while the radicals were found to be stable and persistent in the solid state due to the spin delocalization,the steric protection of confined cavities,and the oxygen *** theoretical calculations and spectral measurements suggest that the photogenic radical cage-TPE-2(•+)experiences photocyclization on the TPE *** with the close-shell cage,the radical cage-TPE-1(•+)and cage-TPE-2(•+)exhibit better photothermal conversion performance due to the incubated infrared absorption from open-shell electron feature and reduced band gap.

关键词： supramolecular cage photogenic radical photocyclization photothermal conversion

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Bifunctional organocatalyst-catalyzed dynamic kinetic resolution of hemiketals for synthesis of chiral ketals via hydrogen bonding control

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Chinese chemical Letters 2025年第1期36卷 248-252页

作者： Meng Shan Yongmei Yu Mengli Sun Shuping Yang Mengqi Wang Bo Zhu Junbiao Chang State Key Laboratory of Antiviral Drugs Pingyuan LaboratoryNMPA Key Laboratory for Research and Evaluation of Innovative DrugSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China

Herein,we report the dynamic kinetic resolution asymmetric acylation ofγ-hydroxy-γ-perfluoroalkyl butenolides/phthalides catalyzed by amino acid-derived bifunctional organocatalysts,and a series of ketals were obtained in high yields(up to 95%)and excellent enantioselectivities(up to 99%).In terms of synthetic utility,the reaction can be performed on a gram scale,and the product can be converted into potential biological nucleoside analog.

关键词： Bifunctional organocatalyst Dynamic kinetic resolution Hemiketal Chiral ketals Hydrogen bonding

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Elucidating the role of P on Mn-and N-doped graphene catalysts in promoting oxygen reduction:Density functional theory studies

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SusMat 2023年第3期3卷 390-401页

作者： Yaqiang Li Penghui Ren Xiangyu Lu Jinqiu Zhang Peixia Yang Xiaoxuan Yang Guangzhao Wang Anmin Liu Gang Wu Maozhong An State Key Laboratory of UrbanWater Resource and Environment School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbinChina Department of Chemical and Biological Engineering University at BuffaloThe State University of New YorkBuffaloNew YorkUSA Key Laboratory of Extraordinary Bond Engineering and Advanced Materials Technology of Chongqing School of Electronic Information EngineeringYangtze Normal UniversityChongqingChina State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalianChina

The non-noble Mn coordinated N,P co-doping graphene materials were investigated theoretically in this work based on density functional theory *** electronic structure is effectively tuned after the introduction of P *** moderate d band center and density of states at Fermi energy of MnN_(4)-P1-G indicate that it is ofmodest adsorption ability for these O-containing *** rank of adsorption energies ofO-containing intermediates for MnN_(4)-P1-G is OH*>2OH*>OOH*>O*>O2*>H2O*,whereas the MnN_(4)-P1-G favors a four-electron process instead of two-electron *** doping of P on MnN_(4)-P1-G can increase the kinetic activity for the rate-determining step as well as the Ulim for MnN_(4)-P1-G significantly increases from 0.38 to 0.45 V compared with MnN_(4)-*** spin density and magnetic moments of Mn are effectively tuned by d,p hybridization to lower the adsorption energy ofOHintermediates(rate-determining step[RDS])so as to improve the catalytic *** is concluded that the P-doped MnN_(4)catalysts with excellent oxygen reduction reaction activity can be obtained and this study can provide theoretical guidance for the rational design of high-performanceMn-based carbonmaterials catalysts.

关键词： MnN_(4)graphene oxygen reduction reaction P doping

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Self-reporting fluorescence deciphers the antibacterial nature of cationic amphiphiles:Monomer or aggregate?

Aggregate

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Aggregate 2023年第5期4卷 214-223页

作者： Chengcheng Zhou Zeyu Ding Weijiang Guan Ben Zhong Tang School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhouChina State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijingChina School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhenChina

Cationic amphiphile aggregates exhibit superior antibacterial activity than ***,the antimicrobial mechanism of aggregates has not been well understood because it is difficult to distinguish and monitor aggregate and monomer in antimicrobial ***,three bola-type cationic amphiphiles with aggregation-induced emission property have been developed to show distinguishable fluorescence in their monomer and *** hydrophilicity of monomer and the stability of aggregate are finely tuned by tailoring the linkers between two quaternary ammonium end groups and tetraphenylethylene *** sensitive fluorescence switching of monomer and aggregate achieves the quantitative monitoring of dynamic interaction of three amphiphiles with *** aggregates with cationic charges first attach to bacterial surface,and the monomers subsequently dissociate from aggregates to penetrate bacterial ***,our results reveal the vital role of stability of aggregates during antimicrobial process,shedding light on the rational design of high-efficient antimicrobials.

关键词： aggregation-induced emission antibacterial nature cationic amphiphiles self-assembly stability

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Interfacial Ru nanoclusters in tandem with single atoms on oxygen-vacancy regulated CeO_(2)for anion exchange membrane seawater-splitting

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Journal of Energy Chemistry 2025年第3期102卷 618-627页

作者： Yue Wang Jing Li Pengfei Yang Hongdong Li Guangrui Xu Yunmei Du Caixia Li Wei Jin Tianyi Ma Zexing Wu Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationInternational Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringCollege of Chemical EngineeringQingdao University of Science&TechnologyQingdao 266042ShandongChina College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Materials Science and Engineering Qingdao University of Science&TechnologyQingdao 266042ShandongChina College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina School of Environmental Science and Engineering Suzhou University of Science and TechnologySuzhou 215009JiangsuChina School of Science STEM CollegeRMIT University 3083VictoriaAustralia

A hydrogen spillover-bridged water dissociation/hydrogen formation could concurrently promote Volmer/Tafel process and improve the efficiency of hydrogen evolution reaction(HER)under alkaline ***,it is still challenging to promote occurrence of hydrogen spillover for the large interfacial transport barriers of H_(2)O and hydrogen on active ***,the strategy of energy barrier gradient to induce hydrogen spillover was proposed by constructing Ru nanoclusters coupled with single atom onto oxygen vacancy cerium dioxide(Ru/CeO_(2)-Ov-2).Density functional theory(DFT)calculations uncover that the adsorption/desorption of H2O occurs at the Ru clusters sites and then the dissociated H*spontaneously overflows from Ru clusters with high binding energy into the adjacent Ru single atom sites with low binding energy,which facilitate the hydrogen ***,the synthesized Ru/CeO_(2)-Ov-2 exhibits a small overpotential of 41 mV at 10 mA cm^(-2)and good stability at 500 mA cm^(-2)for 100 h in alkaline seawater,which could be ascribed to the rapid hydrogen spillover and strong coupling interaction between Ru and CeO_(2)-O_(v).This work provides a novel insight that synthesizing cooperative sites with energy barrier gradient helps to promote hydrogen spillover and accelerate the Volmer/Tafel process of HER.

关键词： Electrocatalyst CeO_(2) Ru Oxygen vacancy Hydrogen evolution reaction

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Micro-nano-fabrication of green functional materials by multiphase microfluidics for environmental and energy applications

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Green Energy & Environment 2024年第8期9卷 1199-1219页

作者： Cheng Qi Tao Zhou Xingjiang Wu Kailang Liu Lei Li Zhou Liu Zhuo Chen Jianhong Xu Tiantian Kong Guangdong Provincial Key Laboratory of Micro/Nano Optomechatronics Engineering College of Mechatronics and Control EngineeringShenzhen UniversityShenzhenGuangdong518000China The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdong518000China Department of Biomedical Engineering School of MedicineShenzhen UniversityShenzhenGuangdong518000China

Multiphase microfluidic has emerged as a powerful platform to produce novel materials with tailor-designed functionalities,as microfluidic fabrication provides precise controls over the size,component,and structure of resultant ***,functional materials with well-defined micro-/nanostructures fabricated by microfluidics find important applications as environmental and energy *** review first illustrated in detail how different structures or shapes of droplet and jet templates are formed by typical configurations of microfluidic channel networks and multiphase flow ***,recent progresses on several representative energy and environmental applications,such as water purification,water collecting and energy storage,were ***,it is envisioned that integrating microfluidics and other novel materials will play increasing important role in contributing environmental remediation and energy storage in near future.

关键词： Microfluidics Multi-phase flow Droplet and microfiber Environmental remediation Energy Storage

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