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Quantitative defect regulation of heterostructures for sulfur catalysis toward fast and long lifespan lithium-sulfur batteries

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Nano Research 2022年第9期15卷 7925-7932页

作者： Saisai Qiu Xinqi Liang shuwen niu Qingguo Chen Gongming Wang Minghua Chen Key Laboratory of Engineering Dielectric and Applications(Ministry of Education) School of Electrical and Electronic EngineeringHarbin University of Science and TechnologyHarbin 150080China Hefei National Laboratory for Physical Science at the Microscale Department of ChemistryUniversity of Science&Technology of ChinaHefei 230026China

The advancement of lithium-sulfur(Li-S)batteries is severely retarded by lithium polysulfides(LiPSs)shuttling behavior and sluggish redox ***,the heterogeneous composite with defective Bi_(2)Se_(3−x)nanosheets and porous nitrogen-doped carbon(Bi_(2)Se_(3−x)/NC)is prepared by selenizing bismuth metal-organic frameworks as a multifunctional sulfur *** highly efficient immobilization-conversion on LiPSs is realized by the synergistic effect of structure construction strategy and defect *** is found that Bi_(2)Se_(3−x)with the suitable amount of selenium vacancies achieves the best electrochemical performance due to the advantages of its structure and *** results confirm the intrinsic correlation between defects and catalysis,which are revealed by computational and experimental *** to these superiorities,the developed sulfur electrodes exhibited admirable stability and a fairly lower capacity decay rate of approximately 0.0278%per cycle over 1,000 cycles at a 3 C *** at the high sulfur loading of 6.2 mg·cm^(−2),the cathode still demonstrates a high discharge capacity of 455 mAh·g^(−1)at 1 *** work may enlighten the development of mechanism investigation and design principles regarding sulfur catalysis toward high-performance Li-S batteries.

关键词： lithium-sulfur(Li-S)batteries lithium polysulfides(LiPSs) shuttle effect redox kinetics selenium vacancy sulfur catalysis

Two-dimensional MOS2 for hydrogen evolution reaction catalysis: The electronic structure regulation

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Nano Research 2021年第6期14卷 1985-2002页

作者： shuwen niu Jinyan Cai Gongming Wang Hefei National Laboratory for Physical Science at Microscale and Department of Chemistry University of Science and Technology of ChinaHefei230026China

Molybdenum disulfide (MoS2) has been recognized as one of the most promising candidates to replace precious Pt for hydrogen evolution reaction (HER) catalysis, due to the natural abundance, low cost, tunable electronic properties, and excellent chemical stability. Although notable processes have been achieved in the past decades, their performance is still far less than that of Pt. Searching effective strategies to boosting their HER performance is still the primary goal. In this review, the recent process of the electronic regulation of MoS2 for HER is summarized, including band structure engineering, electronic state modulation, orbital orientation regulation, interface engineering. Last, the key challenges and opportunities in the development of MoS2-based materials for electrochemical HER are also discussed.

关键词： hydrogen evolution reaction(HER) electronic structure modulation molybdenum disulfide density functional theory phase and interfacial engineering

Cu_(2+1)O/CuO_(x)heterostructures promote the electrosynthesis of C^(2+)products from CO_(2)

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Nano Research 2023年第4期16卷 4698-4705页

作者： Rongbo Sun Cong Wei Zixiang Huang shuwen niu Xiao Han Cai Chen Haoran Wang Jia Song Jun-Dong Yi Geng Wu Dewei Rao Xusheng Zheng Yuen Wu Gongming Wang Xun Hong Center of Advanced Nanocatalysis(CAN) Department of Applied ChemistryUniversity of Science and Technology of ChinaHefei 230026China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China National Synchrotron Radiation Laboratory(NSRL) University of Science and Technology of ChinaHefei 230026China

Manipulating the oxidation state of Cu catalysts can significantly affect the selectivity and activity of electrocatalytic carbon dioxide reduction(CO_(2)RR).However,the thermodynamically favorable cathodic reduction to metallic states typically leads to catalytic ***,a defect construction strategy is employed to prepare crystalline/amorphous Cu_(2+1)O/CuO_(x)heterostructures(c/a-CuO_(x))with abundant Cu0 and Cuδ+(0<δ<1)sites for CO_(2)*** C^(2+)Faradaic efficiency of the heterostructured Cu catalyst is up to 81.3%,with partial current densities of 406.7 mA·cm−***,real-time monitoring of the Cu oxidation state evolution by in-situ Raman spectroscopy confirms the stability of Cuδ+species under long-term high current density *** functional theory(DFT)calculations further reveal that the adjacent Cu0 and Cuδ+sites in heterostructured c/a-CuO_(x)can efficiently reduce the energy barrier of CO coupling for C^(2+)products.

关键词： CO_(2)electroreduction C-C coupling heterostructures in-situ Raman manipulation of oxidation states

Identifying the Geography and Determinants of O2O Online Retailers in Megacity in Central China:A Case Study of Zhengzhou City

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Chinese Geographical Science 2021年第5期31卷 931-950页

作者： QI Jinghui niu shuwen YE Chenxi WANG Luojia WEl Yongna WEN Yuzhao ZHAO Shuling College of Civil Engineering and ArchitecturelCollaborative Imnovation Center for Aviation Economy Development Zhengzhou University of AeronauticsZhengzhou 450046China College of Earth and Environmental Sciences Lanzhou UniversityLanzhou 730000China School of Business Zhengzhou University of AeronauticsZhengzhou 450046China School of Economics Lanzhou University of Finance and EconomicsLanzhou 730101China College of Environment and Planning Henan UniversityKaifeng 475004China College of Resource and Environment Henan University of Economics and LawZhengzhou 450046China

In recent years,O2O e-commerce,represented by online group-buying,has developed vigorously,which had significant impacts on urban commercial *** City is a rising national central city in China,and its e-commerce development level is ahead,but relevant researches are ***,the data of online retailers of *** was collected and combined with Baidu map and Baidu heat map ***,we adopted the methods such as spatial statistics and geodetector to explore the geography and determinants of O2O online retailers in Zhengzhou urban *** main conclusions are 1)The spatial development of O2O online retailers is characterized by significant global high-value agglomeration.2)The agglomeration areas of different types of O2O online retailers are *** of them are concentrated in the old urban area within the Third Ring Road of Zhengzhou City,forming five comprehensive agglomeration areas.3)The areas with the high e-commerce development level are mainly concentrated in the northeast and southwest of the x-shaped region formed by the intersection of Lianyungang-Lanzhou and Beijing-Guangzhou *** Square and Guomao 360 Plaza are at the highest development level,followed by Zhongyuan Wanda Plaza and Daxue Middle *** development level at other areas is relatively low.4)Zhengzhou’s O2O commercial pattern is highly dependent on physical *** population distribution,especially the population distribution during the nightlife period,plays a vital role in its spatial development,followed by *** influences of physical distance are slightly larger than that of time cost,but the difference between them is *** addition,travelling costs have the least *** paper could provide certain references for urban commercial planning.

关键词： O2O online retailers geodetector kernel density spatial development Zhengzhou City China

Accelerating water dissociation kinetics of Ni3N by tuning interfacial orbital coupling

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Nano Research 2021年第10期14卷 3458-3465页

作者： Yishang Wu Yufang Xie shuwen niu Yipeng Zang Jinyan Cai Zenan Bian Xuanwei Yin Yanyan Fang Da Sun Di niu Zheng Lu Amirabbas Mosallanezhad Huijuan Wang Dewei Rao Hongge Pan Gongming Wang Hefei National Laboratory for Physical Science at the Microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei 230026China Experimental Center of Engineering and Material Science University of Science and Technology of ChinaHefei 230026China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China Institute of Science and Technology for New Energy Xi’an Technological UniversityXi’an 710021China School of Materials Science and Engineering State Key Laboratory of Silicon MaterialsZhejiang UniversityHangzhou 310027China

The high unoccupied d band energy of Ni_(3)N basically results in weak orbital coupling with water molecule,consequently leading to slow water dissociation ***,we demonstrate Cr doping can downshift the unoccupied d orbitals and strengthen the interfacial orbital coupling to boost the water dissociation *** prepared Cr-Ni_(3)N/Ni displays an impressive overpotential of 37 mV at 10 mA·cmgeo-2,close to the benchmark Pt/C in 1.0 M KOH *** structural analysis reveals the Cr dopant exists as the Cr-N_(6)states and the average d band energy of Ni_(3)N is also *** functional theory calculation further confirms the downshifted d band energy can strengthen the orbital coupling between the unpaired electrons in O 2p and the unoccupied state of Ni 3d,which thus facilitates the water adsorption and *** work provides a new concept to achieve on-demand functions for hydrogen evolution catalysis and beyond,by regulating the interfacial orbital coupling.

关键词： unoccupied d orbitals Ni_(3)N Cr-N_(6)doping interfacial orbital coupling hydrogen evolution reaction

Orbital-regulated interfacial electronic coupling endows Ni3N with superior catalytic surface for hydrogen evolution reaction

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Science China Chemistry 2020年第11期63卷 1563-1569页

作者： Yanyan Fang Da Sun shuwen niu Jinyan Cai Yipeng Zang Yishang Wu Linqin Zhu Yufang Xie Yun Liu Zixuan Zhu Amirabbas Mosallanezhad Di niu Zheng Lu Junjie Shi Xiaojing Liu Dewei Rao Gongming Wang Yitai Qian Hefei National Laboratory for Physical Science at the Microscale Department of ChemistryUniversity of Science&Technology of ChinaHefei 230026China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China

The interstitial structure and weak Ni-N interaction of Ni3N lead to high unoccupied d orbital energy and unsuitable orbital orientation,which consequently results in weak orbital coupling with H2O and slow water dissociation kinetics for alkaline hydrogen evolution ***,we successfully lower the unoccupied d orbital energy of Ni3N to strengthen the interfacial electronic coupling by employing the strong electron pulling capability of oxygen *** prepared O-Ni3N catalyst delivers an overpotential of 55 mV at 10 mA cm−2,very close to the commercial Pt/*** structural characterization indicates the oxygen incorporation can decrease the electron densities around the Ni ***,density functional theory calculation further proves the oxygen incorporation can create more unoccupied orbitals with lower energy and superior orientation for water adsorption and *** concept of orbital-regulated interfacial electronic coupling could offer a unique approach for the rational design of hydrogen evolution catalysts and beyond.

关键词： hydrogen evolution reaction orbital regulation interfacial electronic coupling Ni3N electrocatalysts

Superior surface electron energy level endows WP_(2) nanowire arrays with N_(2) fixation functions

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Journal of Energy Chemistry 2021年第8期30卷 55-62,I0003页

作者： Dongdong Han Xiaojing Liu Jinyan Cai Yufang Xie shuwen niu Yishang Wu Yipeng Zang Yanyan Fang Fengqi Zhao Wengang Qu Minghua Chen Gongming Wang Yitai Qian Key Laboratory of Engineering Dielectric and Applications(Ministry of Education) Harbin University of Science and TechnologyHarbin 150080China Hefei National Laboratory for Physical Science at the Microscale Department of ChemistryUniversity of Science&Technology of ChinaHefei 230026China Xi’an Modern Chemistry Research Institute Xi’an 710065China

Nitrogen reduction reaction(NRR)under ambient conditions is always a long-standing challenge in science,due to the extreme difficulty in breaking the strong N≡N triple *** key to resolving this issue undoubtedly lies in searching superior catalysts to efficiently activate and hydrogenate the stable nitrogen *** herein evaluate the feasibility of WP_(2) for N2 activation and reduction,and first demonstrate WP_(2) with an impressive ammonia yield rate of 7.13 lg h^(-1)cm^(-2),representing a promising W-based catalyst for *** analysis further reveals that the NRR catalysis on WP_(2) proceeds in a distal reaction pathway,and the exceptional NRR activity is originated from superior surface electron energy level matching between WP_(2) and NRR potential which facilitates the interfacial proton-coupled electron transfer *** successfully unraveling the intrinsic catalytic mechanism of WP_(2) for NRR could offer a powerful platform to manipulate the NRR activity by tuning the electron energy levels.

关键词： WP_(2) Electrocatalysis Energy level Nitrogen reduction Nanowire arrays

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人文发展的多维测度及其政策启示

中国软科学 2021年第5期 99-110页

作者：牛叔文李真梁曼兰州大学资源环境学院甘肃兰州730000 江西师范大学地理与环境学院江西南昌330022

人文发展的多维测度有助于识别制约发展的短板、提高政策的针对性。用多维指标评价65个国家的人文发展水平,结果表明,大多数国家的发展水平明显改善,特别是以中国为代表的一些新兴工业化国家成效显著,但发展不平衡的现象依然突出。中国... 详细信息

人文发展的多维测度有助于识别制约发展的短板、提高政策的针对性。用多维指标评价65个国家的人文发展水平,结果表明,大多数国家的发展水平明显改善,特别是以中国为代表的一些新兴工业化国家成效显著,但发展不平衡的现象依然突出。中国可在本世纪中达到中等发达国家的水平,但需要缩小收入差距、提高可持续发展能力等。

关键词：人文发展多维测度复合评价国际比较政策启示

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甘肃省人口与资源环境耦合的演进分析

中国人口科学 2006年第2期 81-86页

作者：吴文恒牛叔文兰州大学资源环境学院

甘肃省生态环境脆弱,经济欠发达,人口与资源环境的矛盾突出。作者建立评价指标体系,用协调度模型研究1990～2004年甘肃省人口与资源环境耦合的演进态势。研究结果表明,甘肃省人口综合发展水平呈线性增长,资源环境综合状况波动下降;人口... 详细信息

甘肃省生态环境脆弱,经济欠发达,人口与资源环境的矛盾突出。作者建立评价指标体系,用协调度模型研究1990～2004年甘肃省人口与资源环境耦合的演进态势。研究结果表明,甘肃省人口综合发展水平呈线性增长,资源环境综合状况波动下降;人口和资源环境的耦合关系由轻度失调趋向中级协调,后又转向初级协调;资源环境容量空间有限,可持续发展面临巨大压力。因此,应选择人口与资源环境良性互动的协调发展模式。

关键词：人口资源环境耦合协调度甘肃省