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Fe-N-C core-shell catalysts with single low-spin Fe(Ⅱ)-N_(4)species for oxygen reduction reaction and high-performance proton exchange membrane fuel cells

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Journal of Energy Chemistry 2024年第6期93卷 538-546,I0013页

作者： Yan Wan Linhui Yu Bingxin Yang Caihong Li Chen Fang Wei Guo Fang-Xing xiao Yangming Lin Xiamen Key Laboratory of rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021FujianChina CAS Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021FujianChina Fujian Institute of research on the Structure of Matter Chinese Academy of SciencesFuzhou 350002FujianChina College of Materials Science and Engineering Fuzhou UniversityNew CampusMinhou 350108FujianChina College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117FujianChina

Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(Orr)relative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic contributions of Fe-N_(4)moiety with different chemical/spin states(e.g.D1,D2,D3)to Orr are unclear since various states coexist *** the present work,Fe-N-C core-shell nanocatalyst with single lowspin Fe(Ⅱ)-N_(4)species(D1)is synthesized and identified with ex-situ ultralow temperature Mossbauer spectroscopy(T=1.6 K)that could essentially differentiate various Fe-N_(4)states and invisible Fe-O *** quantifying with CO-pulse chemisorption,site density and turnover frequency of Fe-N-C catalysts reach 2.4×10^(-9)site g^(-1)and 23 e site~(-1)s^(-1)during the Orr,***-wave potential(0.915V_(rHE))of the Fe-N-C catalyst is more positive(approximately 54 mV)than that of Pt/***,we observe that the performance of PEMFCs on Fe-N-C almost achieves the 2025 target of the US Department of Energy by demonstrating a current density of 1.037 A cm^(-2)combined with the peak power density of 0,685 W cm^(-2),suggesting the critical role of Fe(Ⅱ)-N_(4)site(D1).After 500 h of running,PEMFCs still deliver a power density of 1.26 W cm^(-2)at 1.0 bar H_(2)-O_(2),An unexpected rate-determining step is figured out by isotopic labelling experiment and theoretical *** work not only offers valuable insights regarding the intrinsic contribution of Fe-N_(4)with a single spin state to alkaline/acidic Orr,but also provides great opportunities for developing high-performance stable PEMFCs.

关键词： Fuel cells Oxygen reduction reaction Non-platinum group metals(PGMs) Isotopic labelling Active site TOF

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Smart materials for safe lithium-ion batteries against thermal runaway

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Journal of Energy Chemistry 2024年第7期94卷 360-392页

作者： Yu Ou Pan zhou Wenhui Hou xiao Ma Xuan Song Shuaishuai Yan Yang Lu Kai Liu Department of Chemical Engineering Tsinghua UniversityBeijing 100084China

In recent years,the new energy storage system,such as lithium ion batteries(LIBs),has attracted much *** order to meet the demand of industrial progress for longer cycle life,higher energy density and cost efficiency,a quantity of research has been conducted on the commercial application of ***,it is difficult to achieve satisfying safety and cycling performance *** may be thermal runaway(Tr),external impact,overcharge and overdischarge in the process of battery abuse,which makes the safety problem of LIBs more *** this review,we summarize recent progress in the smart safety materials design towards the goal of preventing Tr of LIBs reversibly from different abuse *** from smart responsive materials and novel structural design,the safety of LIBs can be improved a *** expect to provide a comprehensive reference for the development of smart and safe lithium-based battery materials.

关键词： Lithium ion batteries(LIBs) Thermal runaway(Tr) Smart materials Safe batteries Solid electrolyte interface(SEI)

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Transparent micropatterned conductive films based on highlyordered nanowire network

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Nano research 2024年第5期17卷 4288-4297页

作者： Xin-ran zhang Hai-Tao Deng Xu zeng Yi-Lin Wang Peng Huang xiao-Sheng zhang School of Integrated Circuit Science and Engineering University of Electronic Science and Technology of ChinaChengdu 611731China

Transparent conductive films that are based on nanowire networks are essential to construct flexible,wearable,and even stretchable ***,large-scale precise micropatterning,especially with regard to the controllability of the organizing orientation of nanowires,is a critical ***,we proposed a liquid film rupture self-assembly approach for manufacturing transparent conductive films with microstructure arrays based on a highly ordered nanowire *** large-scale microstructure conductive films were fabricated through air-liquid interface self-assembly and liquid film rupture *** typical micropattern morphologies,including square,hexagon,circle,serpentine,etc.,were prepared to reveal the universal applicability of the proposed *** homogeneity and controllability of this approach were verified for multiple *** the assembly cycles increasing,the optical transmittance decreases *** addition,theoretical model analysis is carried out,and the analytical formula of the speed of the film moving with the surface tension and the density of the liquid film is ***,the feasibility of this approach for piezoresistive strain sensors is *** fabrication approach demonstrated a cost-effective and efficient method for precisely arranging nanowires,which is useful in transparent and wearable applications.

关键词： flexible electronics transparent conductive network micropatterning nanowires micro electromechanical systems(MEMS)

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AdaPIP: Adaptive picture-in-picture guidance for 360° film watching

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Computational Visual Media 2024年第3期10卷 487-503页

作者： Yi-xiao Li Guan Luo Yi-Ke Xu Yu He Fang-Lue zhang Song-Hai zhang Department of Computer Science and Technology Tsinghua UniversityBeijingChinaand Beijing National Research Center for Information Science and Technology(BNRist)Tsinghua UniversityBeijingChina Key Laboratory of Space Utilization Technology and Engineering Center for Space UtilizationChinese Academy of SciencesBeijingChina Victoria University of Wellington WellingtonNew Zealand

360°videos enable viewers to watch freely from different directions but inevitably prevent them from perceiving all the helpful *** mitigate this problem,picture-in-picture(PIP)guidance was proposed using preview windows to show regions of interest(rOIs)outside the current view *** identify several drawbacks of this representation and propose a new method for 360° film watching called *** enhances traditional PIP by adaptively arranging preview windows with changeable view ranges and *** addition,AdaPIP incorporates the advantage of arrow-based guidance by presenting circular windows with arrows attached to them to help users locate the corresponding rOIs more *** also adapted AdaPIP and Outside-In to HMD-based immersive virtual reality environments to demonstrate the usability of PIP-guided approaches beyond 2D *** user experiments on 2D screens,as well as in Vr environments,indicate that AdaPIP is superior to alternative methods in terms of visual experiences while maintaining a comparable degree of immersion.

关键词： 360°videos picture-in-picture(PIP) virtual reality(Vr) visual guidance

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Photoredox-Catalyzed Metal-Free regio-&Stereoselective C(sp^(2))-H Amination of Enamides with N-Aminopyridium Salts

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Chinese Journal of Chemistry 2024年第18期42卷 2235-2242页

作者： zheng-Bao Qin Kun Ni Li Wang xiao-Di Wu Yu zhang Kai zhao Institute of Advanced Synthesis School of Chemistry and Molecular EngineeringJiangsu National Synergetic Innovation Center for Advanced MaterialsNanjing Tech UniversityNanjingJiangsu211816China college of Chemical Engineering Nanjing Forestry UniversityNanjingJiangsu 210037China

A visible-light-induced photoredox-catalyzed regioselective and stereoselective C(sp')-H amination of enamides with bench-stable and A visible-light-induced photoredox-catalyzed regioselective and stereoselective C(sp)-H amination of enamides with bench-stable and easily accessible N-aminopyridium salts is developed,affording synthetically and biologically prominent vicinal 1,2-diamine scaffolds with broad substrate scope and excellent functional group *** transformation proceeded through a radical pathway involving the Giese addition of the relatively electrophilic N-centered sulfonamidyl radical species to nucleophilicβ-olefinic position of enamides followed by the ensuing single electron oxidation andβ-H elimination,delivering geometrically-defined z-configuredβ-sulfonamidylated *** operational simplicity,environmental friendliness and cost efficiency of this methodology allowed it to pave a new avenue to enrich the arsenal of synthetically crucial functionalized enamides and their related derivatives.

关键词： Enamides Amination Photoredox catalysis regioselective Stereoselective Metal-free

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Genetic analysis and fine mapping of a grain size QTL in the smallgrain sterile rice line zhuo201S

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Journal of Integrative Agriculture 2024年第7期23卷 2155-2163页

作者： Bin Lei Jiale Shao Feng zhang Jian Wang Yunhua xiao zhijun Cheng Wenbang Tang Jianmin Wan College of Agronomy Hunan Agricultural UniversityChangsha 410128China National Key Facility for Crop Gene resources and Genetic Improvement/Institute of Crop Sciences Chinese Academy of Agricultural SciencesBeijing 100081China State Key Laboratory for Crop Genetics and Germplasm Enhancement/Jiangsu Plant Gene Engineering research Center Nanjing Agricultural UniversityNanjing 210095China State Key Laboratory of Hybrid rice Hunan Hybrid Rice Research CenterChangsha 410125China

The development and application of the small-grain rice sterile line zhuo201S(z201S)has demonstrated its potential for mechanized hybrid rice seed production,leading to significant cost ***,the molecular mechanism responsible for the small-grain size characteristic of z201S remains *** this study,we conducted a genetic analysis using near-isogenic lines constructed from z210S,a small-grain rice sterile line,and r2115,a normal-grain *** results revealed that the small-grain trait in z201S is governed by a single partially dominant gene which also enhances grain *** mapping,we localized the causal gene to the short arm of chromosome 2,within a 113 kb physical region delimited by the molecular markers S2-4-1 and *** analysis and gene expression assays indicated LOC_Os02g14760 as the most likely candidate gene,suggesting that the small-grain size trait of z201S is controlled by a novel locus that has not been previously identified.

关键词： rice grain size map-based cloning

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Tumor initiation and early tumorigenesis:molecular mechanisms and interventional targets

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Signal Transduction and Targeted Therapy 2024年第7期9卷 2900-2935页

作者： Shaosen zhang Xinyi xiao Yonglin Yi Xinyu Wang Lingxuan zhu Yanrong Shen Dongxin Lin Chen Wu Department of Etiology and Carcinogenesis National Cancer Center/National Clinical Research Center/Cancer HospitalChinese Academy of Medical Sciences and Peking Union Medical College100021 BeijingChina Key Laboratory of Cancer Genomic Biology Chinese Academy of Medical Sciences and Peking Union Medical College100021 BeijingChina Changping Laboratory 100021 BeijingChina Collaborative Innovation Center for Cancer Personalized Medicine Nanjing Medical UniversityNanjing 211166China Sun Yat-sen University Cancer Center State Key Laboratory of Oncology in South ChinaGuangzhou 510060China CAMS Oxford Institute Chinese Academy of Medical Sciences100006 BeijingChina

Tumorigenesis is a multistep process,with oncogenic mutations in a normal cell conferring clonal advantage as the initial ***,despite pervasive somatic mutations and clonal expansion in normal tissues,their transformation into cancer remains a rare event,indicating the presence of additional driver events for progression to an irreversible,highly heterogeneous,and invasive ***,researchers are emphasizing the mechanisms of environmental tumor risk factors and epigenetic alterations that are profoundly influencing early clonal expansion and malignant evolution,independently of inducing ***,clonal evolution in tumorigenesis reflects a multifaceted interplay between cell-intrinsic identities and various cell-extrinsic factors that exert selective pressures to either restrain uncontrolled proliferation or allow specific clones to progress into ***,the mechanisms by which driver events induce both intrinsic cellular competency and remodel environmental stress to facilitate malignant transformation are not fully *** this review,we summarize the genetic,epigenetic,and external driver events,and their effects on the co-evolution of the transformed cells and their ecosystem during tumor initiation and early malignant evolution.A deeper understanding of the earliest molecular events holds promise for translational applications,predicting individuals at high-risk of tumor and developing strategies to intercept malignant transformation.

关键词： alterations mechanisms restrain

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Insights into plant salt stress signaling and tolerance

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Journal of Genetics and Genomics 2024年第1期51卷 16-34页

作者： Huapeng zhou Haifan Shi Yongqing Yang Xixian Feng Xi Chen Fei xiao Honghui Lin Yan Guo Key Laboratory of Bio-resource and Eco-Environment of Ministry of Education College of Life SciencesSichuan UniversityChengduSichuan 610064China State Key Laboratory of Plant Environmental resilience China Agricultural UniversityBeijing 100193China College of Grassland Science Nanjing Agricultural UniversityNanjingJiangsu 210095China Xinjiang Key Laboratory of Biological resources and Genetic Engineering College of Life Science and TechnologyXinjiang UniversityUrumqiXinjiang 830046China

Soil salinization is an essential environmental stressor,threatening agricultural yield and ecological security *** soils accumulate excessive soluble salts which are detrimental to most plants by limiting plant growth and *** is of great necessity for plants to efficiently deal with the adverse effects caused by salt stress for survival and successful *** determinants of salt tolerance have been identified in plants,and the cellular and physiological mechanisms of plant salt response and adaption have been intensely *** respond to salt stress signals and rapidly initiate signaling pathways to re-establish cellular homeostasis with adjusted growth and cellular *** review summarizes the advances in salt stress perception,signaling,and response in plants.A better under-standing of plant salt resistance will contribute to improving crop performance under saline conditions using multiple engineering *** rhizosphere microbiome-mediated plant salt tolerance as well as chemical priming for enhanced plant salt resistance are also discussed in this review.

关键词： Salt stress Salt perception Salt response and signaling Plant salt tolerance Chemical priming rhizosphere microbiome

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Therapeutic Effectiveness of Leukocyte-and Platelet-rich Fibrin for Diabetic Foot Ulcers:A retrospective Study

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Current Medical Science 2024年第3期44卷 568-577页

作者： Fen WANG xiao-ling zHANG Jing zHANG Song GONG Jing TAO Hui XIANG xiao-qing FU Xu-na BIAN Xue-feng YU An-hui XU Cheng-la YI Shi-ying SHAO Department of Endocrinology Tongji HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430030China Branch of National Clinical research Center for Metabolic Diseases Wuhan430030China Department of radiology Tongji HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430030China Department of Trauma Surgery Tongji HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430030China

Objective Diabetic foot ulcer(DFU)is one of the most serious complications of ***-and platelet-rich fibrin(L-PrF)is a second-generation autologous platelet-rich *** study aims to investigate the clinical effects of L-PrF in patients with diabetes in real clinical *** Patients with DFU who received L-PrF treatment and standard of care(SOC)from 2018 to 2019 in Tongji Hospital were *** clinical information including patient characteristics,wound evaluation(area,severity,infection,blood supply),SOC of DFU,and images of ulcers was retrospectively extracted and analyzed.L-PrF treatment was performed every 7±2 days until the ulcer exhibited complete epithelialization or an overall percent volume reduction(PVr)greater than 80%.Therapeutic effectiveness,including overall PVr and the overall and weekly healing rates,was *** Totally,26 patients with DFU were enrolled,and they had an ulcer duration of 47.0(35.0,72.3)*** severity and infection of ulcers varied,as indicated by the Site,Ischemia,Neuropathy,Bacterial Infection,and Depth(SINBAD)scores of 2–6,Wagner grades of 1–4,and the Perfusion,Extent,Depth,Infection and Sensation(PEDIS)scores of 2–*** initial ulcer volume before L-PrF treatment was 4.94(1.50,13.83)cm3,and the final ulcer volume was 0.35(0.03,1.76)*** median number of L-PrF doses was 3(2,5).A total of 11 patients achieved complete epithelialization after the fifth week of treatment,and 19 patients achieved at least an 80%volume reduction after the seventh *** overall wound-healing rate was 1.47(0.63,3.29)cm3/week,and the healing rate was faster in the first 2 weeks than in the remaining *** treatment did not change the percentage of complete epithelialization or healing *** Adding L-PrF to SOC significantly improved wound healing in patients with DFU independent of the ankle brachial index,SINBAD score,or Wagner grade,indicating that this method is appropriate for D

关键词： diabetic foot ulcer autologous platelet-rich plasma leukocyte-and platelet-rich fibrin standard of care percentage volume reduction

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Earth-abundant zn-dipyrrin chromophores for efficient CO2 photoreduction

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National Science review 2024年第6期11卷 214-222页

作者： Song Guo Fu-Gui zeng xiao-Di Li Kai-Kai Chen Ping Wang Tong-Bu Lu zhi-Ming zhang Institute for New Energy Materials and Low Carbon Technologies School of Materials Science& Engineering Tianjin University of Technology

The development of strong sensitizing and Earth-abundant antenna molecules is highly desirable for CO2reduction through artificial photosynthesis. Herein, a library of zn–dipyrrin complexes（z-1-z-6） are rationally designed via precisely controlling their molecular configuration to optimize strong sensitizing Earth-abundant photosensitizers. Upon visible-light excitation, their special geometry enables intramolecular charge transfer to induce a charge-transfer state, which was first demonstrated to accept electrons from electron donors. The resulting long-lived reduced photosensitizer was confirmed to trigger consecutive intermolecular electron transfers for boosting CO2-to-CO conversion. remarkably, the Earth-abundant catalytic system with z-6 and Fe-catalyst exhibits outstanding performance with a turnover number of >20 000 and 29.7% quantum yield, representing excellent catalytic performance among the molecular catalytic systems and highly superior to that of noble-metal photosensitizer Ir（ppy）2（bpy）+under similar conditions. Experimental and theoretical investigations comprehensively unveil the structure–activity relationship, opening up a new horizon for the development of Earth-abundant strong sensitizing chromophores for boosting artificial photosynthesis.

关键词： zn complex photocatalysis CO2 reduction charge transfer photosensitizer

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