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Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Zscheme heterojunctions with enhanced photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 5002-5010页

作者： Qingtao Zhu honglei Shen chao han Liu huang Yanting Zhou Yuanxin Du Xi Kang Manzhou Zhu Department of Materials Science and Engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic ***,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 h_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and *** enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional *** work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.

关键词： atomically precise metal nanocluster Z-scheme heterojunction interfacial charge transfer build-in electric field photocatalytic hydrogen production

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Reactive oxygen species:Multidimensional regulators of plant adaptation to abiotic stress and development

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Journal of Integrative Plant Biology 2024年第3期66卷 330-367页

作者： Pengtao Wang Wen-Cheng Liu chao han Situ Wang Ming-Yi Bai Chun-Peng Song State Key Laboratory of Crop Stress Adaptation and Improvement School of Life SciencesHenan UniversityKaifeng 475004China The Key Laboratory of Plant Development and Environmental Adaptation Biology Ministry of EducationSchool of Life SciencesShandong UniversityQingdao 266237China Faculty of Science McGill UniversityMontreal H3B1X8Canada

Reactive oxygen species(ROS)are produced as undesirable by-products of metabolism in various cellular compartments,especially in response to unfavorable environmental conditions,throughout the life cycle of *** ROS production disrupts normal cellular function and leads to oxidative *** cope with excessive ROS,plants are equipped with a sophisticated antioxidative defense system consisting of enzymatic and non-enzymatic components that scavenge ROS or inhibit their harmful effects on ***,when maintained at relatively low levels,ROS act as signaling molecules that regulate plant growth,development,and adaptation to adverse ***,we provide an overview of current approaches for detecting *** also discuss recent advances in understanding ROS signaling,ROS metabolism,and the roles of ROS in plant growth and responses to various abiotic stresses.

关键词： abiotic stress growth and development plant reactive oxygen species

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Accelerating solar driven CO_(2) reduction via sulfur-doping boosted water dissociation and proton transfer

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Nano Research 2024年第3期17卷 1056-1065页

作者： Ke Yan Liang Chen Yangguang hu Ting Wang Cong Chen chao Gao Youju huang Benxia Li School of Chemistry and Chemical Engineering Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang ProvinceZhejiang Sci-Tech UniversityHangzhou 310018China College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhou 311121China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

Exploring efficient photocatalysts for solar driven CO_(2) reduction with water(h_(2)O)as a proton donor is highly imperative but remains a great challenge because the synchronous enhancement of CO_(2) activation,h_(2)O dissociation and proton transfer is hardly achieved on a ***,the sluggish h_(2)O dissociation impedes the photocatalytic CO_(2) reduction reaction involving multiple proton–electron coupling transfer ***,a sulfur-doped BiOCl(S-BiOCl)photocatalyst with abundant oxygen vacancies(OV)is developed,which exhibits broadband-light harvesting across solar spectrum and distinct photothermal effect due to *** photocatalytic CO_(2) reduction with h_(2)O in a gas–solid system,the high CO yield of 49.76μmol·g_(cat)^(-1)·h^(-1) with 100%selectivity is achieved over the S-BiOCl catalyst under a simulated *** h_(2)O-assisted CO_(2) reduction reaction on S-BiOCl catalyst is triggered by photocatalysis and the photothermal heating further enhances the reaction *** kinetic isotope experiments indicate that the sluggish h_(2)O dissociation affects the whole photocatalytic CO_(2) reduction *** presence of oxygen vacancies promotes the adsorption and activation of h_(2)O and CO_(2),and the doped S sites play a crucial role in boosting h_(2)O dissociation and accelerating the dynamic migration of hydrogen *** a result,the ingenious integration of OV defects,S sites and photothermal effect in S-BiOCl catalyst conjointly contributes to the significant improvement in photocatalytic CO_(2) reduction performance.

关键词： BiOCl sulfur doping photocatalytic CO_(2)reduction h_(2)O activation proton feeding

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highly selectiveα-C(sp^(3))-h arylation of alkenyl amides via nickel chain-walking catalysis

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Chinese Chemical Letters 2024年第7期35卷 271-275页

作者： haoran Shi Jiaxin Wang Yuqin Zhu hongyang Li Guodong Ju Lanlan Zhang chao Wang Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of ChemistryTianjin Normal UniversityTianjin 300387China

herein,we report the migratory hydroarylation of unactivated alkenes with aryl iodides using native and weakly coordinating amide directors under mild *** coordination of the monodentate directing group and the ligand enable the highly regioselective migratory hydroarylation via a chain walking process to form the thermodynamically stable five-membered nickelacyle *** protocol provides a variety of valuableα-aryl-substituted alkylamine products,and exhibited good functional group *** modification of bioactive compounds such as fenofibrate and indomethacin further highlights the synthetic value of this protocol.

关键词： Alkenes hydroarylation Chain-walking Regioselective Nickel catalysis

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Anchoring heterometallic cluster on P-doped carbon nitride for efficient photocatalytic nitrogen fixation in water and air ambient

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Chinese Chemical Letters 2024年第4期35卷 176-180页

作者： chao-Long Chen Rong Chen La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Light-driven nitrogen fixation to produce ammonia is a green and economical technology of nitrogen reduction but is still quite challenging, especially in an air atmosphere without any sacrificial ***, we demonstrate efficient photocatalytic nitrogen fixation using water and air directly by loading lanthanide–transition metal(4f–3d) cluster NdCo_(3) on two-dimensional P-doped graphitic carbon nitrides(PCN) material surface. Benefiting from the increase in the number of nitrogen vacancies(NVs) and highly matched band gap structure and excellent hole trapping ability of clusters, the NdCo_(3)/PCN photocatalyst exhibits efficient nitrogen reduction activity with 371(in air) and 825 μmol h^(-1)g^(-1)(in pure nitrogen)without any sacrificial reagents. The introduction of potassium sulfate inhibits hydrogen production and promotes nitrogen reduction activation. This work suggests that anchoring precisely structured clusters on 2D materials may enhance photocatalytic nitrogen reduction under normal temperature and pressure.

关键词： Photocatalytic Nitrogen fixation 4f-3d Cluster Air atmosphere

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Interfaces engineering of heterostructured Ni Co P/Ni Fe LDh@CC for attaining high catalytic activity in long-lasting rechargeable Zn–air batteries

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Rare Metals 2024年第10期43卷 4961-4972页

作者： Xiao-Lin hu Ji-Chuan Fan Xiang Li Zhen-Kun Wu Yuan-Yi Li chao-he Xu School of Science Chongqing Key Laboratory of New Energy Storage Materials and DevicesChongqing University of Technology JINShAN Science&Technology (Group) Co. Ltd. National Engineering Research Center for Magnesium Alloys Chongqing University College of Aerospace Engineering Chongqing University

Zinc-air batteries (ZABs) offer tremendous potential in various industries and daily life due to their excellent energy density,safety and ***,the practical application of ZABs has been severely hindered by challenges such as high low round-trip efficiencies and overpotential,primarily attributed to the inherent sluggish kinetics in the oxygen evolution reaction(OER) of air *** address these issues effectively and economically,heterojunction engineering accompanied by interfacial chemistry emerges as an ideal approach to designing efficient OER ***,a novel heterogeneous interfacial chemical structure,namely NiCoP/NiFe LDh (layered double hydroxide),needle-like NiCoP and NiFe LDh nanosheets were assembled from cores and shells,***,the NiCoP/NiFe LDh-based ZABs have an exceptionally long cycle life of 238 h,far superior to Pt/C+Ir/C batteries (～97 h).Theoretical calculations and experimental results demonstrate that NiCoP/NiFe LDh possesses tunable interfacial chemistry,demonstrating significant electronic,coordination,geometric and synergistic *** enhancements dramatically improve the active site density,intrinsic activity and electrochemical durability of the *** summary,this work provides a solid foundation for the development of costeffective OER electrocatalysts for electrochemical energy devices.

关键词： Coupling effects Interface catalysis Oxygen evolution reaction Theoretical simulation Zinc–air batteries

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Tailored heterostructured Ni_(3)N-NiO nano-frameworks for boosting electrocatalytic oxygen evolution via surface-modulated plasma strategy

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Nano Research 2024年第9期17卷 7909-7917页

作者： Bo Ouyang haonan Qin chao Sun Yilin Deng Ang Li Jipeng Zhu Erjun Kan Rajdeep Singh Rawat MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing School of ScienceNanjing University of Science&TechnologyNanjing 210094China The Laboratory of Road and Bridge Civil EngineeringSchool of ScienceNanjing University of Science&TechnologyNanjing 210094China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China Natural Sciences and Science Education National Institute of EducationNanyang Technological University637616Singapore

The facile reconfiguration of phases plays a pivotal role in enhancing the electrocatalytic production of h2 through heterostructure *** chemical methods have been explored extensively for this purpose,plasma-based techniques offer a promising avenue for achieving heterostructured ***,the conventional plasma approach introduces complexities,leading to a multi-step fabrication process and challenges in precisely controlling partial surface structure modulation due to the intricate interaction *** our pursuit of heterostructures with optimized oxygen evolution reaction(OER)behavior,we have designed a facile auxiliary insulator-confined plasma system to directly attain a Ni_(3)N-NiO heterostructure(hNiNO).By meticulously controlling the surface heating process during plasma processing,such approach allows for the streamlined fabrication of hNiNO *** resulting nano-framework exhibits outstanding catalytic performance,as evidenced by its overpotential of 320 mV at a current density of 10 mA·cm^(-2),in an alkaline *** stands in stark contrast to the performance of NiO-covered Ni_(3)N fabricated using the conventional plasma method(sNiNO).Operando plasma diagnostics,coupled with numerical simulations,further substantiates the influence of surface heating due to auxiliary insulator confinement of the substrate on typical plasma parameters and the formation of the Ni_(3)N-NiO nanostructure,highlighting the pivotal role of controlled surface temperature in creating a high-performance heterostructured electrocatalyst.

关键词： structural modulation auxiliary insulator-confined plasma surface heating control heterostructure electrocatalytic O_(2) evolution

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highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply

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National Science Review 2024年第5期11卷 315-325页

作者： Tong Bao Yamin Xi chaoqi Zhang Peiyang Du Yitong Xiang Jiaxin Li Ling Yuan Chengzhong Yu chao Liu School of Chemistry and Molecular Engineering East China Normal University Australian Institute for Bioengineering and Nanotechnology The University of Queensland

Photocatalytic N2fixation is a promising strategy for ammonia（Nh3） synthesis;however,it suffers from relatively low ammonia yield due to the difficulty in the design of photocatalysts with both high charge transfer efficiency and desirable N2adsorption/activation ***,an S-scheme CoSx/ZnS heterojunction with dual active sites is designed as an efficient N2fixation *** CoSx/ZnS heterojunction exhibits a unique pocket-like nanostructure with small ZnS nanocrystals adhered on a single-hole CoSxhollow *** the heterojunction,the ele ctronic interaction between ZnS and CoSxcreates electron-deficient Zn sites with enhanced N2chemisorption and electron-sufficient Co sites with active hydrogen supply for N2hydrogenation,cooperatively reducing the energy barrier for *** combination with the promoted photogenerated electron-hole separation of the S-scheme heterojunction and facilitated mass transfer by the pocket-like nanostructure,an excellent N2fixation performance with a high Nh3yield of 1175.37 μmol g-1h-1is *** study provides new insights into the design of hetero junction photocatalysts for N2fixation.

关键词： photocatalysis nitrogen fixation S-scheme heterojunction active hydrogen ammonia

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Enhanced Electrochemical Properties and Optimized Li^(+)Transmission Pathways of PEO/LLZTO-Based Composite Electrolytes Modified by Supramolecular Combination

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Energy & Environmental Materials 2024年第1期7卷 238-246页

作者： Zhengyi Lu Lin Peng Yi Rong Enli Wang Ruhua Shi hongxun Yang Yadong Xu Ruizhi Yang chao Jin College of Energy Soochow Institute for Energy and Materials InnovationsSoochow UniversitySuzhou 215006China Jiangsu Runchao Energy Storage Technology Co. LtdZhenjiang 212050China

Poly(ethylene oxide)(PEO)and Li_(6.75)La_(3)Zr_(1.75)Ta_(0.25)O_(12)(LLZTO)-based composite polymer electrolytes(CPEs)are considered one of the most promising solid electrolyte ***,agglomeration of LLZTO within PEO and lack of Li^(+)channels result in poor electrochemical ***,a functional supramolecular combination(CD-TFSI)consisting of activeβ-cyclodextrin(CD)supramolecular with self-assembled LiTFSI salt is selected as an interface modifier to coat LLZTO *** from vast h-bonds formed betweenβ-CD and PEO matrix and/or LLZTO,homogeneous dispersion and tight interface contact are ***,^(6)Li NMR spectra confirm a new Li^(+)transmission pathway from PEO matrix to LLZTO ceramic then to PEO matrix in the as-prepared PEO/LLZTO@CD-TFSI CPEs due to the typical cavity structure ofβ-*** a proof,the conductivity is increased from 5.3×10^(-4)S cm^(-1)to 8.7×10^(-4)S cm^(-1)at 60℃,the Li^(+)transference number is enhanced from 0.38 to 0.48,and the electrochemical stability window is extended to 5.1 V versus Li/Li^(+).Li‖LiFePO_(4)CR2032 coin full cells and pouch cells prove the practical application of the as-prepared PEO/LLZTO@CD-TFSI *** work offers a new strategy of interface modifying LLZTO fillers with functional supramolecular combination to optimize PEO/LLZTO CPEs for solid lithium batteries.

关键词： conductivity interfacial stability LLZTO fillers modification PEO matrix

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Association of daily sitting time and leisure-time physical activity with body fat among ***

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Journal of Sport and health Science 2024年第2期13卷 195-203页

作者： Jingwen Liao Min hu Kellie Imm Clifton J.holmes Jie Zhu chao Cao Lin Yang Guangdong Provincial Key Laboratory of Physical Activity and health Promotion Guangzhou Sport UniversityGuangzhou 510500China Scientific Research Center Guangzhou Sport UniversityGuangzhou 510500China Division of Epidemiology&Genetics Department of Population and Public Health SciencesKeck School of Medicine of the University of Southern CaliforniaLos AngelesCA 90033USA Program in Physical Therapy Washington University School of MedicineSt.LouisMO 63110USA Center for human Nutrition Washington University School of MedicineSt.LouisMO 63110USA Department of Plastic and Reconstructive Surgery Shanghai East HospitalTongji UniversityShanghai 200070China Department of Cancer Epidemiology and Prevention Research Alberta Health ServicesCalgary T2S 3C3Canada Department of Oncology and Community health Sciences University of CalgaryCalgary T2N 1N4Canada

Background:Prolonged sitting and reduced physical activity lead to low energy ***,little is known about the joint impact of daily sitting time and physical activity on body fat *** investigated the independent and joint associations of daily sitting time and physical activity with body fat among ***:This was a cross-sectional analysis of *** representative data from the National health and Nutrition Examination Survey2011-2018 among adults aged 20 years or *** sitting time and leisure-time physical activity(LTPA)were self-reported using the Global Physical Activity *** fat(total and trunk fat percentage)was determined via dual X-ray ***:Among 10,808 adults,about 54.6%spent 6 h/day or more sitting;more than one-half reported no LTPA(inactive)or less than 150 min/week LTPA(insufficiently active)with only 43.3%reported 150 min/week or more LTPA(active)in the past *** fully adjusting for sociodemographic data,lifestyle behaviors,and chronic conditions,prolonged sitting time and low levels of LTPA were associated with higher total and trunk fat percentages in both *** stratifying by LTPA,the association between daily sitting time and body fat appeared to be stronger in those who were inactive/insuufficiently *** the joint analyses,inactive/insuufficiently active adults who reported sitting more than 8 h/day had the highest total(female:3.99%(95%confidence interval(95%CI):3.09%-4.88%);male:3.79%(95%CI:2.75%-4.82%))and trunk body fat percentages(female:4.21%(95%CI:3.09%-5.32%);male:4.07%(95%CI:2.95%-5.19%))when compared with those who were active and sitting less than 4 h/***:Prolonged daily sitting time was associated with increased body fat among *** higher body fat associated with 6 h/day sitting may not be offset by achieving recommended levels of physical activity.

关键词： Adults Body fat distribution Physical activity Sitting time

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