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Manipulating d-d orbital hybridization induced by Mo-doped Co_(9)S_(8) nanorod arrays for high-efficiency water electrolysis

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Journal of Energy Chemistry 2024年第6期93卷 592-600,I0015页

作者： Xue Zhou Jing Li Guangyao Zhou Weiran Huang Yucan Zhang Jun Yang Huan Pang Mingyi Zhang Dongmei Sun Yawen Tang Lin Xu Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023JiangsuChina 'College of science Jinling Institute of TechnologyNanjing 211169JiangsuChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Nanjing IPE institute of Green Manufacturing Industry Nanjing 211100JiangsuChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009JiangsuChina Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina

Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic ***,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water *** has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)*** to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,*** impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) *** innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.

关键词： d-d orbital hybridization Transition metal sulfides Nanorods arrays Water electrolysis

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Unraveling the catalytic redox mechanism of lithium–sulfur batteries through advanced in-situ/operando characterizations

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science China Chemistry 2024年

作者： Pan Zeng Cheng Yuan Bin Su Genlin Liu Jiechang Gao Kun Yang Qingyuan Wang Liang Zhang institute for advanced Study School of Mechanical Engineering Chengdu University institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Dyson School of Design Engineering Imperial College London

Accelerating the redox conversion of lithium polysulfides(LiPSs) with electrocatalysts has been regarded as an effective avenue to surmount the shuttle effect and realize high-performance lithium–sulfur(Li–S) batteries. However, the complicated reaction process, especially the real-time evolution of sulfur-containing species and electrocatalysts under working conditions, has brought great difficulties in the explicit understanding of reaction mechanism of Li–S batteries, thereby severely hampering the design of highly efficient electrocatalysts. Therefore, a crucial prerequisite for correctly identifying the reaction mechanism is an in-depth analysis of the dynamic evolution of reaction intermediates and their structure-performance relationships. In this review,we comprehensively summarized the most recent progress in the dynamic behaviors of LiPSs and electrocatalysts of Li–S batteries under working conditions in conjunction with closely related in-situ/operando characterizations to recognize the realtime evolution of phase, composition, and atomic/electronic structure, thereby unraveling the corresponding catalytic mechanism. In addition, the major challenges and unexplored issues of catalytic conversion of LiPSs were summarized and discussed, aiming to provide perspectives into the development of highly efficient electrocatalysts in Li–S chemistry. Based on this review, we believe that reasonable regulation of reconstruction behaviors can achieve satisfactory electrocatalysts with high catalytic activity, accelerating the development of green energy.

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Electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species

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SusMat 2024年第2期4卷 51-74页

作者： Zheng Zhang Danyang Li Yunchuan Tu Jiao Deng Huiting Bi Yongchao Yao Yan Wang Tingshuai Li Yongsong Luo Shengjun Sun Dongdong Zheng Sónia A.C.Carabineiro Zhou Chen Junjiang Zhu Xuping Sun Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhanHubeiChina School of Chemistry and Chemical Engineering Chongqing UniversityChongqingChina i-Lab Vacuum Interconnected NanotechWorkstation(Nano-X)Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhouJiangsuChina institute of Fundamental and Frontier sciences University of Electronic Science and Technology of ChinaChengduSichuanChina College of Chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJinanShandongChina LAQV-REQUIMTE Department of ChemistryNOVA School of Science and TechnologyUniversidade NOVA de Lisboa2829-516 CaparicaPortugal College of Materials Xiamen UniversityXiamenFujianChina

The electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species not only offers an effective avenue to achieve carbon neutral-ity and reduce environmental pollution,but also establishes a route to synthesize valuable chemicals,such as urea,amide,and *** innovative approach expands the application range and product categories beyond simple carbona-ceous species in electrocatalytic CO_(2) reduction,which is becoming a rapidly advancing *** review summarizes the research progress in electrocatalytic urea synthesis,using N_(2),NO_(2)^(-),and NO_(3)^(-)as nitrogenous species,and explores emerging trends in the electrosynthesis of amide and amine from CO_(2) and nitro-gen ***,the future opportunities in this field are highlighted,including electrosynthesis of amino acids and other compounds containing C-N bonds,anodic C-N coupling reactions beyond water oxidation,and the catalytic mechanism of corresponding *** critical review also captures the insights aimed at accelerating the development of electrochemical C-N coupling reactions,confirming the superiority of this electrochemical method over the traditional techniques.

关键词： C-N coupling CO_(2) reduction electrocatalysis nitrogenous species reaction mechanism

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Bifunctional noble-metal-free cocatalyst coating enabling better coupling of photocatalytic CO_(2)reduction and H_(2)O oxidation on direct Z-scheme heterojunction

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Nano Research 2024年第6期17卷 5022-5030页

作者： Wei Zhao Weihao Mo Yan Zhang Lingxuan Hu Yiyi Zheng Zhulei Chen Xiangyue Niu Yuling Zhao Lichun Liu Shuxian Zhong Song Bai Key Laboratory of the Ministry of Education for advanced Catalysis Materials College of Chemistry and Materials ScienceZhejiang Normal UniversityJinhua 321004China College of Biological Chemical Sciences and Engineering and Nanotechnology Research InstituteJiaxing UniversityJiaxing 314001China College of Geography and Environmental sciences Zhejiang Normal UniversityJinhua 321004China College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310058China School of Biological and Chemical Engineering Panzhihua UniversityPanzhihua 617000China

Selective loading of spatially separated redox cocatalysts on direct Z-scheme heterojunctions holds great promise for advancing the efficiency of artificial photosynthesis,which however is limited to the photodeposition of noble metal cocatalysts and the fabrication of hollow double-shelled semiconductor ***,the co-exposure of discrete cocatalyst and semiconductor increases the product diversity when both the exposed sites of which participate in CO_(2)***,we present a facile and versatile protocol to overcome these limitations via surface coating of Z-scheme heterojunctions with bifunctional noble-metal-free *** Cu_(2)O/Fe_(2)O_(3)(CF)as a model heterojunction and layered Ni(OH)_(2)as a model cocatalyst,it is found that Ni(OH)_(2)lying on the surfaces of Cu_(2)O and Fe_(2)O_(3)separately co-catalyzes the CO_(2)reduction and H_(2)O *** experimental and theoretical investigation reveals that the Ni(OH)_(2)outer layer:(i)mitigates the charge recombination in CF and balances their transfer and consumption;(ii)reduces the rate-determining barriers for CO_(2)-to-CO and H_(2)O-to-O_(2)conversion,(iii)suppresses the side proton reduction occurring on CF,and(iv)protects the CF from component *** expected,the redox reactions stoichiometrically proceed,and significantly enhanced photocatalytic activity,selectivity,and stability in CO generation are achieved by the stacked Cu_(2)O/Fe_(2)O_(3)@Ni(OH)_(2)in contrast to *** study demonstrates the significance of the synergy between bifunctional cocatalysts and Z-scheme heterojunctions for improving the efficacy of overall redox reactions,opening a fresh avenue for the rational design of artificial photosynthetic systems.

关键词： Z-scheme heterojunction bifunctional cocatalyst CO_(2)reduction H_(2)O oxidation stoichiometric redox reaction

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Unlocking efficient energy storage via regulating ion and electron-active subunits:an(SbS)_(1.15)TiS_(2)superlattice for large and fast Na^(+)storage

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science China Chemistry 2024年第1期67卷 336-342页

作者： Baixin Peng Tianxun Cai Shaoning Zhang Yuqiang Fang Zhuoran Lv Yusha Gao Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of Materials science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China School of Physical science and technology ShanghaiTech UniversityShanghai 200031China Beijing National Laboratory for Molecular sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Alloying-type metal sulfides with high sodiation activity and theoretical capacity are promising anode materials for high energy density sodium ion ***,the large volume change and the migratory and aggregation behavior of metal atoms will cause severe capacity decay during the charge/discharge ***,a robust and conductive TiS_(2)framework is integrated with a high-capacity SbS layer to construct a single phase(SbS)_(1.15)TiS_(2)superlattice for both high-capacity and fast Na^(+)*** metallic TiS_(2)sublayer with high electron activity acts as a robust and conductive skeleton to buffer the volume expansion caused by conversion and alloying reaction between Na+and SbS ***,high capacity and high rate capability can be synergistically realized in a single phase(SbS)_(1.15)TiS_(2)*** novel(SbS)_(1.15)TiS_(2)anode has a high charge capacity of 618 mAh g^(-1)at 0.2 C and superior rate performance and cycling stability(205 mAh g^(-1)at 35 C after 2,000 cycles).Furthermore,in situ and ex situ characterizations are applied to get an insight into the multi-step reaction *** integrity of robust Na-Ti-S skeleton during(dis)charge process can be *** superlattice construction idea to integrate the Na^(+)-active unit and electron-active unit would provide a new avenue for exploring high-performance anode materials for advanced sodium-ion batteries.

关键词： (SbS)_(1.15)TiS_(2) sulfides sodium ion battery superlattice fast-charging

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Epidermal visualized health monitoring system based on stretchable and washable TPU hybrid conductive microtextiles

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Rare Metals 2024年第7期43卷 3185-3193页

作者： Jing-Bo Yuan Zhi-Hong Feng Dong-Chan Li Yang Luo Yun-Lei Zhou School of Chemical Engineering Hebei University of Technology Engineering Research Center of Chemical Technology for Efficient Utilization of Seawater ResourcesMinistry of EducationTianjin 300401China National Key Laboratory of Application Specific Integrated Circuit Shijiazhuang050000China Department of Materials ETH Zürich8093 ZurichSwitzerland Hangzhou institute of technology Xidian UniversityHangzhou 311231China

Electronic textiles,an emerging class of electronic technology,offer exciting opportunities for seamless integration with the human *** applications have been developed based on electronic ***,researches on integrating multiple electronic textilebased devices are still *** this study,we present a system integrated with an electrocardiogram monitoring sensor and an electroluminescence device based on stretchable and washable conductive micro *** signal is acquired by an electrocardiograph amplifier and displayed by a dual-color electroluminescence device based on the processed *** integrated electronic device has excellent moisture permeability and comfort for long-term *** system reported in this study opens a new avenue for the application of electronic textiles in health monitoring,robotic prosthetics,and competitive sports.

关键词： Conductive microtextile Textile composite Electronic textile Electroluminescent displays

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Hyperbranched polyamidoamine protective layer with phosphate and carboxyl groups for dendrite-free Zn metal anodes

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Chinese Chemical Letters 2024年第10期35卷 495-499页

作者： Xinxiu Yan Xizhe Huang Yangyang Liu Weishang Jia Hualin Chen Qi Yao Tao Chen Key Laboratory of General Chemistry of the National Ethnic Afairs Commission School of Chemistry and EnvironmentSouthwest Minzu UniversityChengdu 610041China institute of smart city and inteligent transportation Southwest Jiaotong UniversityChengdu 611756China School of Materials science and Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China

Zinc metal is regarded as one of the most promising anodes for Zn-based batteries in next-generation energy storage ***,the dendrite growth and interfacial corrosion lead to poor reversibility and cycle life of Zn ***,we synthesize a 2-phosphate-1,2,4-butane tricarboxylic acid modified hyperbranched polyamidoamine containing rich terminal groups of phosphate and carboxyl(HPC)as modified layer for the Zn ***,the in situ acid-etching promotes the exposure of(002)Zn plane and the generated salt-polymer complexes could be adhered to the Zn anodes *** greatly favors the uniform deposition of Zn and inhibits interfacial ***,stable HPC@Zn anode plating/stripping for over 1200 h at a high areal capacity of 4 mAh/cm^(2)and a current density of 4 m A/cm^(2)is *** study provides a new avenue of hyperbranched polymer in interfacial design for highly reversible and stable Zn metal anodes.

关键词： Zn anode Znmetal batteries Surface chemistry Functional groups Hyperbranched polyamidoamine

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Dual-functional microneedle with programmatic regulation of macrophage for autoimmune psoriasis treatment

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Nano Research 2024年第8期17卷 7436-7448页

作者： Ze Qiang Zhao Bo Zhi Chen Jia Li Gan Yun Hao Feng Ling Liang Lingyun Yu Zi Yi Wang Samin Abbaszadeh Mohammad-Ali Shahbazi Ruixing Yu Xin Dong Guo State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Beijing Laboratory of Biomedical Materials College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China China-Japan Friendship Hospital Chinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100029China Department of Dermatology China-Japan Friendship HospitalBeijing 100029China Department of Pharmaceutical Biomaterials School of PharmacyZanjan University of Medical SciencesZanjan 45139-56184Iran Department of Biomaterials and Biomedical technology University Medical Center GroningenUniversity of GroningenAntonius Deusinglaan 19713 AV GroningenThe Netherlands W.J.Kolff institute for Biomedical Engineering and Materials science University of GroningenAntonius Deusinglaan 19713 AV GroningenThe Netherlands

Modulating the immune microenvironment to establish sustained positive feedback within immune pathways represents a promising avenue for the treatment of ***,the precise and efficient delivery of therapeutic systems to the subcutaneous basal layer to modulate immune disorders is a major challenge in the treatment of autoimmune *** this project,we introduce a dual-functional microneedle(DF-MN)designed to combine MNs with multiple release kinetics and immunotherapy,the programmed treatment is achieved through segmented design of the MN structure,realizing the unification of rapid and long-lasting treatment of autoimmune *** vivo imaging results showed that GelMA@M-CSF showed fluorescent signals after 5 days of delivery to subcutaneous tissues,whereas HA@IL-13 showed minimal fluorescent signals after 2 *** multistage release behavior of MNs and the diffusion mechanism of drugs were explained at the molecular level,in combination with coarse-grained molecular ***,DF-MN can successfully induce macrophage reprogramming in vitro and ameliorate overall symptoms in a psoriasis mice model,suggesting that it has the potential to be an effective strategy for the treatment of psoriasis and portends to be a transformative platform for the treatment of other autoimmune diseases.

关键词： microneedle psoriasis M2 macrophage immunoregulation

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Large contributions of emission reductions and meteorological conditions to the abatement of PM_(2.5)in Beijing during the 24th Winter Olympic Games in 2022

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Journal of Environmental sciences 2024年第2期136卷 172-188页

作者： Yaping Jiang Shaocai Yu Xue Chen Yibo Zhang Mengying Li Zhen Li Zhe Song Pengfei Li Xiaoye Zhang Eric Lichtfouse Daniel Rosenfeld Key Laboratory of Environmental Remediation and Ecological Health Ministry of EducationResearch Center for Air Pollution and HealthCollege of Environmental and Resource SciencesZhejiang UniversityHangzhou 310058China College of science and technology Hebei Agricultural UniversityBaoding 071000China Chinese Academy of Meteorological sciences China Meteorological AdministrationBeijing 100081China Aix-Marseille Univ CNRSColl FranceCNRSIRDINRAEEuropole Mediterraneen de l’ArboisAvenue Louis Philibert13100 Aix en ProvenceFrance Xi’an Jiaotong University State Key Laboratory of Multiphase Flow in Power EngineeringXi’an 710049China institute of Earth sciences The Hebrew University of JerusalemJerusalemIsrael

To guarantee the blue skies for the 2022 Winter Olympics held in Beijing and Zhangjiakou from February 4 to 20,Beijing and its surrounding areas adopted a series of emission control *** provides an opportunity to determine the impacts of large-scale temporary control measures on the air quality in Beijing during this special ***,we applied the WRF-CMAQ model to quantify the contributions of emission reduction measures and meteorological *** show that meteorological conditions in 2022 decreased PM_(2.5)in Beijing by 6.9 and 11.8μg/m^(3)relative to 2021 under the scenarios with and without emission reductions,*** emission reduction measures implemented in Beijing and seven neighboring provinces resulted in an average decrease of 13.0μg/m^(3)(-41.2%)in PM_(2.5)in *** the entire period,local emission reductions contributed more to good air quality in Beijing than nonlocal emission *** the emission reduction scenario,local,controlled regions,other regions,and boundary conditions contributed 47.7%,42.0%,5.3%,and 5.0%to the PM_(2.5)concentrations in Beijing,*** results indicate that during the cleaning period with the air masses from the northwest,the abatements of PM_(2.5)were mainly caused by local emission ***,during the potential pollution period with the air masses from the east-northeast and west-southwest,the abatements of PM_(2.5)were caused by both local and nonlocal emission reductions almost *** implies that regional coordinated prevention and control strategies need to be arranged scientifically and rationally when heavy pollution events are forecasted.

关键词： PM_(2.5) WRF-CMAQ Meteorological conditions Emission reductions Winter Olympic games

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Metal oxide ion gated transistors based sensors

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science China(Technological sciences) 2024年第4期67卷 1040-1060页

作者： LI Yang YAO Yu WANG LeLe WANG LiWei PANG YunCong LUO ZhongZhong ARUNPRABAHARAN Subramanian LIU ShuJuan ZHAO Qiang College of Electronic and Optical Engineering&College of Flexible Electronics(Future technology) Nanjing University of Posts&Telecommunications(NJUPT)Nanjing 210023China State Key Laboratory of Organic Electronics and Information Displays&Jiangsu Key Laboratory for Biosensors Institute of Advanced Materials(IAM)Nanjing University of Posts&Telecommunications(NJUPT)Nanjing 210023China Department of Chemical Engineering Polytechnique MontréalMontréalQuébec H3C3J7Canada

Metal oxide ion-gated transistors(MOIGTs)have garnered significant attention within the sensing domain due to their potential for achieving heightened sensitivity while consuming minimal energy across diverse *** harnessing the advantageous combination of metal oxides'high carrier mobility and facile surface customization,coupled with the potent signal amplification capabilities of ion-gated transistors,MOIGTs offer a promising avenue for discerning biomolecules,overseeing chemical reactions,p H levels,as well as facilitating gas or light *** the past few decades,the MOIGT field has made remarkable strides in refining device physics,enhancing material properties,showcasing robust sensing capabilities,and broadening its application *** advancements have simultaneously unveiled new challenges and opportunities,necessitating interdisciplinary expertise to fully unlock the commercial potential of *** this comprehensive review,we offer a snapshot of this swiftly evolving technology,delve into its current applications,and provide insightful recommendations for future directions in the coming decade.

关键词： sensors ion gated transistors metal oxide semiconductors biosensors chemosensors pH sensors

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