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Boosting cationic and anionic redox activity of Li-rich layered oxide cathodes via Li/Ni disordered regulation

Journal of Energy Chemistry 2025年第1期 533-543页

作者： Zewen Liu Zhen Wu Hao Wang Xudong Zhang Yuanzhen chen Yongning Liu Shengwu Guo shenghua chen Yanli Nan Yan Liu State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University School of Materials Science and Engineering Xi'an University of Architecture and Technology Hefei Advanced Computing Center Operation Management Corp Ltd Network Information Center Xi'an Jiaotong University

Lithium-rich layered oxides （LLOs） are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries （LIBs）.However,they suffer from voltage decay and low initial Coulombic efficiency （ICE） due to severe structural degradation caused by irreversible O ***,we introduce a three-in-one strategy of increasing Ni and Mn content,along with Li/Ni disordering and TM–O covalency regulation to boost cationic and anionic redox activity simultaneously and thus enhance the electrochemical activity of *** target material,Li1.2Ni0.168Mn0.558Co0.074O2（L1）,exhibits an improved ICE of 87.2%and specific capacity of 293.2 mA h g-1and minimal voltage decay of less than 0.53 m V cycle-1over 300 cycles at 1C,compared to Li1.2Ni0.13Mn0.54Co0.13O2（Ls）(274.4 mA h g-1for initial capacity,73.8%for ICE and voltage decay of 0.84 mV/cycle over 300 cycles at 1C).Theoretical calculations reveal that the density of states （DOS） area near the Fermi energy level for L1 is larger than that of Ls,indicating higher anionic and cationic redox reactivity than ***,L1 exhibits increased O-vacancy formation energy due to higher Li/Ni disordering of 4.76%（quantified by X-ray diffraction Rietveld refinement） and enhanced TM–O covalency,making lattice O release more difficult and thus improving electrochemical *** increased Li/Ni disordering also leads to more Ni2+presence in the Li layer,which acts as a pillar during Li+de-embedding,improving structural *** research not only presents a viable approach to designing low-Co LLOs with enhanced capacity and ICE but also contributes significantly to the fundamental understanding of structural regulation in high-performance LIB cathodes.

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Computational study of transition metal single-atom catalysts supported on nitrogenated carbon nanotubes for electrocatalytic nitrogen reduction

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Nano Research 2023年第1期16卷 325-333页

作者： Yanyang Qin Yan Li Wenshan Zhao shenghua chen Tiantian Wu Yaqiong Su School of Chemistry Xi'an Key Laboratory of Sustainable Energy Materials ChemistryState Key Laboratory of Electrical Insulation and Power EquipmentXi'an Jiaotong UniversityXi'an 710049China Department of Chemistry Tsinghua UniversityBeijing 100084China

Developing efficient and stable catalysts for the electrocatalytic N_(2)reduction reaction(NRR)shows promise in nitrogen ***,we proposed active and stable single-atom catalysts(SACs)toward NRR,where transition metals are anchored on nitrogenated carbon nanotubes(NCNTs).Among the screened nine common transition metals(Ti,V,Cr,Mn,Fe,Mo,Ru,Rh,and Ag)on(4,4)NCNTs,we found Mo-NCNT possesses the most excellent NRR catalytic activity and selectivity with a low overpotential of 0.29 ***,the NRR performance of Mo-NCNT was further engineered by controlling the nanotube diameter,where the lowest overpotential is 0.18 V at a diameter of 9.6Å.In addition,we found a linear scaling relation between*NNH and*NH_(2)on the studied catalysts with the exception of(2,2)and(3,3)Mo-NCNTs,owing to their extremely unstable *** attribute the outstanding NRR performance of Mo-NCNT to the moderate adsorption of N_(2)due to the slightly low d-band center of Mo,and the charge donating and accepting capacity of *** work has provided a deeper insight into designing highefficiency and stable NRR SACs supported by NCNTs.

关键词： nitrogen reduction single-atom catalysts density functional theory(DFT) carbon nanotubes nitrogen doping

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Volume-complementary bipolar layered oxide enables stable symmetric sodium-ion batteries

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Nano Research 2024年第5期17卷 4125-4133页

作者： Bo Peng Feng Wang Nazir Ahmad Lai Yu shenghua chen Genqiang Zhang School of Materials Science and Engineering Key Laboratory of Efficient Conversion and Solid-state Storage of Hydrogen and Electricity of Anhui ProvinceAnhui University of TechnologyMa’anshan 243002China Hefei National Research Center for Physical Sciences at the Microscale Chinese Academy of Sciences(CAS)Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China National Innovation Platform(Center)for Industry-Education Integration of Energy Storage Technology School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China

The commercialization of sodium-ion batteries is based on developing low-cost,highly stable,and safe cathode and anode ***,the promising hard carbon anode and layered oxide cathode suffer from low sodium-embedded potential near 0.1 V and severe phase transitions,which cause safe problem and short lifespan,***,we design a low-strain bipolar P2-Na_(0.7)Ni_(0.25)Fe_(0.2)Ti_(0.55)O_(2) to solve the mentioned obstacles,whereas(Ni,Fe)and Ti provide charge compensation when it is used as cathode and anode,*** is revealed that the bipolar layered oxide undergoes solid-solution reaction when used as cathode or anode,and exhibits volume-complementary feature in a sodium-ion full-cell,as identified by in-situ X-ray ***,the safe symmetric sodium-ion full-cell exhibits excellent cyclic stability with 91.7%capacity retention after 200 *** work will provide a new horizon for designing safe and stable sodium-ion batteries.

关键词： sodium-ion batteries bipolar layered oxides solid-solution reaction volume complementation symmetric battery

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Low‐dimensional material supported single‐atom catalysts for electrochemical CO_(2) reduction

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SmartMat 2022年第1期3卷 84-110页

作者： Bingqing Wang shenghua chen Zedong Zhang Dingsheng Wang Department of Chemistry Tsinghua UniversityBeijingChina

Converting CO_(2) emissions to valuable carbonaceous chemicals/fuels under mild conditions provides a sustainable way to maintain carbon balance and alleviate the energy ***‐dimensional material(LDM)supported single‐atom catalysts(SACs)have been attracted significant attention for electrochemical CO_(2) reduction reaction(ECR)in recent *** is mainly because integrating the single‐atoms and LDMs can inherit the advantages of themselves and the synergy effects between them are potential to enhance the ECR *** this review,we summarized the strategies for synthesizing LDM supported SACs for ECR,and different LDM supported SACs for ECR have been briefly ***,some optimization strategies for LDM supported SACs towards CO_(2) electroreduction are *** the end of this review,the perspectives and challenges of LDM supported SACs for ECR are provided.

关键词： ECR electrochemical CO_(2)reduction low‐dimensional material single‐atom catalysts

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Efficiently coupled glucose oxidation for high-value D-glucaric acid with ultradurable hydrogen via Mn(III)in acidic solution

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Nano Research 2023年第8期16卷 10748-10755页

作者： Junhua Li Yi Jiang Xu Zhang Yidan Huo Fanglin Du Yongxiao Tuo Zhiyan Guo Dawei chen shenghua chen College of Material Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China National Innovation Platform(Center)for Industry-Education Integration of Energy Storage Technology Xi’an Jiaotong UniversityXi’an 710049China State Key Laboratory of Heavy Oil Processing College of New EnergyChina University of Petroleum(East China)Qingdao 266580China

The electrooxidation of the alcohol and aldehyde molecules instead of water coupled with H2 production has been proven to be effective for producing high-value fine chemicals under alkaline *** is also noteworthy that under acidic conditions,the stability of non-noble metal water oxidation catalysts remains a great challenge due to the lattice oxygen ***,we coupled the biomass-derived glucose oxidation for high-value D-glucaric acid(GRA)with ultra-durable hydrogen in acid solution over a Yb-MnO_(2)*** Mn^(3+)regulated by Yb atoms doped in MnO_(2)can effectively optimize the adsorption and desorption processes of the alcohol and aldehyde group and improve the intrinsic activity but cannot for *** catalyst exhibited extremely high activity and stability after 50 h for glucose oxidation,inhibiting the lattice oxygen process and MnO4−formation,while the activity was quickly lost within 0.5 h for water *** functional theory(DFT)calculations further demonstrated that glucose oxidation reaction proceeds preferentially due to the oxidation of aldehyde group with lower adsorption-free energy(−0.4 eV)than water(ΔG>0 eV),avoiding the lattice oxygen *** work suggests that biomass-derived glucose oxidation not only provides a cost-effective approach for high-value chemicals,but also shows an extremely potential as an alternative to acidic oxygen evolution reaction(OER)for ultradurable H2 production.

关键词： acidic water oxidation lattice oxygen mechanism(LOM) non-noble metal catalyst stability D-glucaric acid(GRA)

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Highly emissive tribenzotriquinacene-based double-rimed nanocube

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Nano Research 2023年第7期16卷 9584-9590页

作者： Zhilong Jiang Zihao Wu Jun Wang Bangtang chen Min Wang Weiya Liu Wenzhi Lv Rui Miao He Zhao Die Liu shenghua chen Mingzhao chen Pingshan Wang Institute of Environmental Research at Greater Bay Area Key Laboratory for Water Quality and Conservation of the Pearl River DeltaMinistry of EducationGuangzhou UniversityGuangzhou 510006China Department of Organic and Polymer Chemistry College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China Department of Chemistry Tsinghua UniversityBeijing 100084China College of Chemistry and Chemical Engineering Qiannan Normal University for NationalitiesDuyun 558000China

The study of discrete nanosized cages has gone a long way to seek aesthetically appealing structures and to carry out functional *** the construction of supramolecular cages via a bottom-up self-assembly process has been well developed,the sophisticated synthesis still remains a *** we report the design and assembly of a giant double-rimed nanocube Zn_(24)LH_(8),built with 8 tribenzotriquinacene as six-connected vertices and 24(tpy=terpyridine)connectivities serving as the *** the single-crystal structure of tribenzotriquinacene-based ligand LH,the bowl-shaped ligand defines a suitable rigid platform for the spatially well-defined attachment of three sets of parallel vertices,which promotes the quantitative formation of the desired three-dimensional(3D)double-rimed cubic *** formed nanocube Zn_(24)LH_(8)possesses molecular weight up to 25.6 kDa and side length 5.3 ***,the Zn_(24)LH_(8)exhibits strong cyan light emission with high luminescence quantum yields in solution and in the solid state based on the inherent cage-confinement induced emission *** adding orange-emissive Rhodamine B,emission tuning experiments were achieved including white light *** work presents a new system for the imitation of complex assemblies and provides a promising candidate for emissive materials.

关键词： self-assembly double-rimed nanocube terpyridine coordination light-emitting metallacages

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Corrosion formation and phase transformation of nickel-iron hydroxide nanosheets array for efficient water oxidation

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Nano Research 2021年第12期14卷 4528-4533页

作者： Lanqian Gong Huan Yang Hongming Wang Ruijuan Qi Junlei Wang shenghua chen Bo You Zehua Dong Hongfang Liu Bao Yu Xia Key laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureWuhan National Laboratory for OptoelectronicsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan430074China School of Materials Science and Engineering Wuhan Institute of TechnologyWuhan430074China Institute for Advanced Study Nanchang UniversityNanchang330000China Department of Information Science and Technology East China Normal UniversityShanghai200240China

Designing earth-abundant electrocatalysts with high performance towards water oxidation is highly decisive for the sustainable energy technologies. This study develops a facile natural corrosion approach to fabricate nickel-iron hydroxides for water oxidation. The resulted electrode demonstrates an outstanding activity and stability with an overpotential of 275 mV to deliver 10 mA·cm^(−2). Experimental and theoretical results suggest the corrosion-induced formation of hydroxides and their transformation to oxyhydroxides would account for this excellent performance. This work not only provides an interesting corrosion approach for the fabrication of excellent water oxidation electrode, but also bridges traditional corrosion engineering and novel materials fabrication, which would offer some insights in the innovative principles for nanomaterials and energy technologies.

关键词： water oxidation electrocatalyst corrosion hydroxide phase transformation

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5S-Heudelotinone alleviates experimental colitis by shaping the immune system and enhancing the intestinal barrier in a gut microbiota-dependent manner

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Acta Pharmaceutica Sinica B 2024年第5期14卷 2153-2176页

作者： Qing Meng Jianshuang Guo Ke Lv Yang Liu Jin Zhang Mingyue Li Xirui cheng shenghua chen Xiaoguang Huo Quan Zhang Yue chen Jing Li State Key Laboratory of Medicinal Chemical Biology College of PharmacyNankai UniversityTianjin 300353China College of Chemistry and Frontiers Science Center for New Organic Matter Haihe Laboratory of Sustainable Chemical TransformationsNankai UniversityTianjin 300071China Accendatech Company Ltd.Tianjin 300193China

Aberrant changes in the gut microbiota are implicated in many diseases,including inflammatory bowel disease(IBD).Gut microbes produce diverse metabolites that can shape the immune system and impact the intestinal barrier integrity,indicating that microbe-mediated modulation may be a promising strategy for preventing and treating *** fecal microbiota transplantation and probiotic supplementation are well-established IBD therapies,novel chemical agents that are safe and exert strong effects on the gut microbiota are urgently ***,we report the total synthesis of heudelotinone and the discovery of 5S-heudelotinone(an enantiomer)as a potent agent against experimental colitis that acts by modulating the gut microbiota.5S-Heudelotinone alters the diversity and composition of the gut microbiota and increases the concentration of short-chain fatty acids(SCFAs);thus,it regulates the intestinal immune system by reducing proinflammatory immune cell numbers,and maintains intestinal mucosal integrity by modulating tight junctions(TJs).Moreover,5S-heudelotinone(2)ameliorates colitis-associated colorectal cancer(CAC)in an azoxymethane(AOM)/dextran sulfate sodium(DSS)-induced in situ carcinoma ***,these findings reveal the potential of a novel natural product,namely,5S-heudelotinone,to control intestinal inflammation and highlight that this product is a safe and effective candidate for the treatment of IBD and CAC.

关键词： 5S-heudelotinone Total synthesis Inflammatory bowel disease Gut microbiota Short-chain fatty acids Immune system Intestinal barrier Drug discovery

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煤矸石山防自燃隔离层的构建及其效果

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农业工程学报 2014年第2期30卷 235-243页

作者：陈胜华胡振琪陈胜艳太原理工大学阳泉学院阳泉045000 中国矿业大学(北京)土地复垦与生态重建研究所北京100083 山西省阳泉市农业局阳泉045000

露天堆放的煤矸石山极易自燃引发严重的地质灾害和环境污染。为改善传统的土壤覆盖治理方法，结合阳泉自燃煤矸石山综合治理现场，在黄土覆盖前以当地黏土和粉煤灰为原料构建不同设计构型的隔离层，并动态测量隔离层渗透率以及治理1a后... 详细信息

露天堆放的煤矸石山极易自燃引发严重的地质灾害和环境污染。为改善传统的土壤覆盖治理方法，结合阳泉自燃煤矸石山综合治理现场，在黄土覆盖前以当地黏土和粉煤灰为原料构建不同设计构型的隔离层，并动态测量隔离层渗透率以及治理1a后试验区覆盖层的地温、紧实度，探讨在煤矸石与覆盖土壤之间添加隔离层防治白燃的效果。结果表明：利用黏土和粉煤灰构建隔离层，改善了传统的覆盖层结构，土壤紧实度随土层深度增加呈逐渐增大趋势，形成“上松下紧”利于植被生长的理想剖面；隔离层可有效阻隔空气，效果为粉煤灰与黏土混合〉黏土〉粉煤灰，试验以粉煤灰：黏土=1：2（体积比）比例充分混合构成的隔离层效果最佳，监测期间渗透率一直保持在低于50×10^-12m^2的水平，地温从表入深基本平稳，在土层深度10-30cm处温度大致稳定在10-15℃之间。该研究可为自燃煤矸石山综合治理中隔离层的构建提供参考数据及思路。

关键词：土地复垦自燃黏性土粉煤灰隔离层煤矸石山防治

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A hybrid matching method for geospatial services in a composition-oriented environment

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Science China(Technological Sciences) 2010年第S1期53卷 213-220页

作者： LUO An 1,2,WANG YanDong 1,2 & chen shenghua 2 1 State Key Laboratory of Software Engineering,Wuhan University,Wuhan 430072,China 2 State Key Laboratory of Information Engineering in Surveying,Mapping and Remote Sensing,Wuhan University,Wuhan 430079,China 1. State Key Laboratory of Software Engineering Wuhan University Wuhan 430072 China 2. State Key Laboratory of Information Engineering in Surveying Mapping and Remote Sensing Wuhan University Wuhan 430079 China

With the development of Internet and GIS,large volumes of spatial data,powerful computing resources and many spatial data processing functions are published in the form of Web *** suitable geospatial services in the composition-oriented environment is a crucial *** semantic Web provides a kind of technology to find and compose various service resources automatically through the *** paper proposes a hybrid method for the semantic matching of geospatial *** method includes two *** 1 puts forward a multi-level semantic matching approach,which matches single geospatial service at four levels:classification,input/output,precondition/effect and the quality of service(QoS).This multi-level matching approach makes single service matching quicker and more *** 2 puts forward a matching algorithm for a geospatial service chain based on the *** algorithm adopts a trace algorithm,taking account of the effect of the *** restricts the input/output parameters of the current service by the input/output parameters of service chain,pre-service and *** matches the atomic service dynamically in a composition-oriented environment,and accurately converts the abstract model of geospatial services into an executable geospatial service chain.A case study of the flood analysis for the Poyang Lake illustrates the effectiveness of our context-based matching method for geospatial services.

关键词： geospatial services semantic context composition service match

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