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Observation of oxygen evolution over a {Ni12}-cluster-based metal-organic framework

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Science China Chemistry 2022年第6期65卷 1088-1093页

作者： Zongsu Han Zheng Yan Kunyu Wang Xinchen Kang Kai Lv Xiaoping Zhang Zhen Zhou Sihai Yang Wei Shi Peng Cheng department of Chemistry Key Laboratory of Advanced Energy Materials Chemistry(MOE)Renewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin300071China College of biological Chemical Sciences and EngineeringJiaxing UniversityJiaxing314001China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing100190China department of Chemistry University of ManchesterManchesterM139PLUK School of Materials Science and engineering Institute of New Energy Material ChemistryNankai UniversityTianjin300350China

The development of efficient electrocatalysts based on non-noble metals for oxygen evolution reaction(OER) remains an important and challenging task. Multinuclear transition-metal clusters with high structural stability are promising OER catalysts but their catalytic role is poorly understood. Here we report the crystallographic observation of OER activity over robust {Ni12}-clusters immobilised in a porous metal-organic framework, NKU-100, by single-crystal X-ray diffraction as a function of external applied potential. We observed the aggregation of confined oxygen species around the {Ni12}-cluster as a function of applied potential during the electrocatalytic process. The refined occupancy of these oxygen species shows a strong correlation with the variation of current density. This study demonstrates that the enrichment of oxygen species in the secondary coordination sphere of multinuclear transition-metal clusters can promote the OER activity.

关键词： metal-organic framework oxygen evolution reaction secondary coordination sphere X-ray diffraction binding site

Oxygen-deficient titanium dioxide supported cobalt nano-dots as efficient cathode material for lithium-sulfur batteries

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Journal of energy Chemistry 2020年第9期29卷 390-397,I0012页

作者： You Li Xiao Zhang Guihua Liu Ashton Gerhardt Katelyn Evans Aizhong Jia Zisheng Zhang Hebei Provincial Key Laboratory of Green chemical Technology and High Efficient energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China department of chemical and biological engineering University of OttawaOttawaOntario K1N 6N5Canada

Lithium sulfur(Li-S)batteries demonstrate great promise for efficient energy storage systems once the lithium polysulfide(LPS)shuttling and sluggish redox kinetics can be well ***,we developed a sea urchin-structured oxygen-deficient titanium dioxide semiconductor anchored with cobalt nano-dots(Co@TiO2-x)as a high-performance multifunctional sulfur host material for Li-S *** sea urchin-structured Co@TiO2-x offers strong structural stability and strengthened chemical interaction towards ***,the incorporation of Co nano-dots into TiO2 leads to increased oxygen vacancies,which augments the electrical conduction and benefits LPS conversion acceleration as *** a result,the oxygen vacancy-rich Co@TiO2-x composite exhibits excellent conductivity,strong LPS confinement and promoted sulfur electrochemical kinetics,rendering enhanced LPS shuttling inhibition and rapid redox *** to these features,the Co@TiO2-x/S cathode exhibits a discharge capacity of 803 mAh g-1at 1 C and a good cyclic stability upon 500 cycles with a low capacity fading rate of 0.07%per *** synergistic design of conductive multifunctional LPS barrier is also promising to enlighten the material engineering in other energy storage applications.

关键词： Titanium dioxide Oxygen vacancy Cobalt nano-dots Lithium-sulfur battery conversion kinetics

Rational design of Co nano-dots embedded three-dimensional graphene gel as multifunctional sulfur cathode for fast sulfur conversion kinetics

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Journal of energy Chemistry 2021年第5期30卷 132-140页

作者： Tongtao Wan Shuming Liu Changcheng Wu Zhaoyang Tan Shuanglong Lin Xiaojie Zhang Zisheng Zhang Guihua Liu Hebei Provincial Key Laboratory of Green chemical Technology and High Efficient energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China College of chemical Technology Shijiazhuang UniversityShijiazhuang 050035HebeiChina department of chemical and biological engineering University of OttawaOttawa KIN 6N5ONCanada

Lithium-sulfur(Li-S)batteries hold great promises to serve as next-generation energy storage devices because of their high theoretical energy density and environmental ***,the shuttle effect of the soluble lithium polysulfides(LiPS)and intrinsic insulating nature of sulfur lead to low sulfur utilization and coulombic efficiency,leading to poor cycling *** impeded charge transportation and retard LiPS catalytic conversion also endows the Li-S batteries with sluggish redox reaction,leading to unsatisfied rate *** this study,Co-based MOF material ZIF-67 is used as the precursor to prepare Co nano-dots decorated three-dimensional graphene aerogel as sulfur *** porous architecture establishes a highly conductive interconnected framework for fast charge/mass *** exposed Co nano-dots serve as active sites to strongly trap LiPS,which endows CoNDs@G with low decomposition energy barrier for fast LiPS conversion reaction and promote the completely Li2 S catalytic ***-S cells based on the Co-NDs@G cathode exhibits excellent cyclability and a high capacity retention rate of 91.1%in 100 *** strategy offers a new direction to design sulfur immobilizer for accelerated LiPS conversion kinetics of Li-S batteries.

关键词： Lithium-sulfur batteries Co nano-dots Graphene network Metal-organic framework High-loading cathodes

In situ preparation of Ag@AgCl/Bio-veins composites and their photocatalytic activity and recyclability

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Frontiers of chemical Science and engineering 2023年第7期17卷 906-917页

作者： Min Zou Chao Tan Zhengqiu Yuan Ming Wu Jian Jian Lei Zhang Yan Zhang Zhou Ma Hu Zhou School of Resource&Environment and Safety engineering Hunan University of Science and TechnologyXiangtan 411201China Key Laboratory of Theoretical Organic Chemistry and Functional Molecules Ministry of EducationFunctional Film Materials Engineering Research Center of Hunan ProvinceHunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and ConversionSchool of Chemistry and Chemical EngineeringHunan University of Science and TechnologyXiangtan 411201China School of Information and Electrical engineering Hunan University of Science and TechnologyXiangtan 411201China

The industrial application of nano-photocatalysts in wastewater treatment has been severely restricted for a long time due to their difficult separation,poor reusability,and low *** this work,a facile strategy was proposed to enhance the photocatalytic activity and recovery performance of Ag@AgCl *** veins(Bio-veins)with a unique 3D porous construction were used as carriers for the in-situ growth of Ag@AgCl *** electron microscopy results showed that the Ag@AgCl nanoparticles were uniformly loaded on the surface and interior of the Bio-veins,and the size of the Ag@AgCl nanoparticles immobilized on the Bio-veins(50–300 nm)was significantly smaller than Ag@AgCl obtained by the co-precipitation method(1–3μm).The Bio-veins played a vital role in the photocatalysis reaction *** degradation efficiency of the Ag@AgCl/Bio-veins(CI4)was up to 3.50 times as high as pure Ag@***,the composites also exhibited excellent recyclability and stability under both visible and solar *** work provided a suitable strategy for nano-photocatalysts for practical application and may also offer new possibilities for the high-value utilization of biomass materials.

关键词： Ag@AgCl biological veins photocatalytic activity recyclability

Identification of the starting reaction position in the hydrogenation of (N-ethyl)carbazole over Raney-Ni

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Journal of energy Chemistry 2015年第2期24卷 219-224页

作者： Feifei Sun Yue An Lecheng Lei Fuying Wu Jingke Zhu Xingwang Zhang Key Laboratory of Biomass chemical engineering of Ministry of Education Department of Chemical and Biological EngineeringZhejiang University

Hydrogenation of carbazole and N-ethylcarbazole over Raney-Ni catalyst were realized in the temperature range of 393-503 K. 4[H] adduct dominated the hydrogenation products and the formation of 2[H] adduct was the rate-limiting step during the period, in which the conversion of carbazole was less than 40%. The hydrogenation process followed pseudo-first-order kinetics and the hydrogenation activation energies of carbazole and N-ethylcarbazole were 90 kJ/mol and 115 kJ/mol, respectively. The reaction starting position as well as the pathway of the hydrogenation of （N-ethyl）carbazole were investigated by comparing the kinetic characteristics of hydrogen uptake of carbazole and N- ethylcarbazole. The results showed that the reaction was a stepwise hydrogenation process and the first H_2 was added to the C1 = C10 double bond in the hydrogenation.

关键词： (N-ethyl)carbazole hydrogen storage Raney-Ni catalyst reaction kinetics first reaction position

Carbon-Nitride-Based Materials for Advanced Lithium-Sulfur Batteries

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Nano-Micro Letters 2022年第12期14卷 579-601页

作者： Wenhao Sun Zihao Song Zhenxing Feng Yaqin Huang Zhichuan J.Xu Yi-Chun Lu Qingli Zou State Key Laboratory of chemical Resource engineering Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China Electrochemical energy and Interfaces Laboratory Department of Mechanical and Automation EngineeringThe Chinese University of Hong KongHong Kong Special Administrative Region 999077People’s Republic of China School of Materials Science and engineering Nanyang Technological UniversitySingapore 639798Republic of Singapore School of chemical Biologicaland Environmental EngineeringOregon State UniversityCorvallisOR 97331USA

Lithium-sulfur(Li-S)batteries are promising candidates for next-generation energy storage systems owing to their high energy density and low ***,critical challenges including severe shuttling of lithium polysulfides(LiPSs)and sluggish redox kinetics limit the practical application of Li-S *** nitrides(C_(x)N_(y)),represented by graphitic carbon nitride(g-C_(3)N_(4)),provide new opportunities for overcoming these *** a graphene-like structure and high pyridinic-N content,g-C_(3)N_(4) can effectively immobilize LiPSs and enhance the redox kinetics of S *** addition,its structure and properties including electronic conductivity and catalytic activity can be regulated by simple methods that facilitate its application in Li-S ***,the recent progress of applying C_(x)N_(y)-based materials including the optimized g-C_(3)N_(4),g-C_(3)N_(4)-based composites,and other novel C_(x)N_(y) materials is systematically reviewed in Li-S batteries,with a focus on the structure-activity *** limitations of existing C_(x)N_(y)-based materials are identified,and the perspectives on the rational design of advanced C_(x)N_(y)-based materials are provided for high-performance Li-S batteries.

关键词： Lithium-sulfur batteries Carbon nitride Polysulfide conversion Shuttle effect Anode protection

Porous framework materials for energy&environment relevant applications:A systematic review

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Green energy & Environment 2024年第2期9卷 217-310页

作者： Yutao Liu Liyu Chen Lifeng Yang Tianhao Lan Hui Wang Chenghong Hu Xue Han Qixing Liu Jianfa Chen Zeming Feng Xili Cui Qianrong Fang Hailong Wang Libo Li Yingwei Li Huabin Xing Sihai Yang Dan Zhao Jinping Li College of chemical engineering and Technology Shanxi Key Laboratory of Gas Energy Efficient and Clean UtilizationTaiyuan University of TechnologyTaiyuan030024China School of Chemistry and chemical engineering South China University of TechnologyGuangzhou510640China Key Laboratory of Biomass chemical engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China department of Chemistry The University of ManchesterManchesterM139PLUK department of chemical and Biomolecular engineering National University of SingaporeSingapore 117585Singapore ZJU-Hangzhou Global Scientific and Technological Innovation Center Hangzhou311215China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin UniversityChangchun130012China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of ChemistryUniversity of Science and Technology BeijingBeijing100083China

Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related *** of new technologies for green energy production and storage,industrial energy saving and efficiency reinforcement,carbon capture,and pollutant gas treatment is in highly imperious *** emerging porous framework materials such as metal–organic frameworks(MOFs),covalent organic frameworks(COFs)and hydrogen-bonded organic frameworks(HOFs),owing to the permanent porosity,tremendous specific surface area,designable structure and customizable functionality,have shown great potential in major energy-consuming industrial processes,including sustainable energy gas catalytic conversion,energy-efficient industrial gas separation and ***,this manuscript presents a systematic review of porous framework materials for global and comprehensive energy&environment related applications,from a macroscopic and application perspective.

关键词： Porous framework materials Catalysis Separation Gas storage Carbon neutrality

Photothermal-photocatalytic thin-layer flow system for synergistic treatment of wastewater

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Chinese Journal of chemical engineering 2023年第11期63卷 120-129页

作者： Zhongjiao Zha Jun Wu Shaoping Tong Xuebo Cao College of chemical engineering State Key Laboratory Breeding Base of Green Chemistry-Synthesis TechnologyZhejiang University of TechnologyHangzhou 310014China College of biological Chemical Sciences and EngineeringJiaxing UniversityJiaxing 314001China College of Advanced Materials engineering Jiaxing Nanhu UniversityJiaxing 314001China

The integration of the photocatalytic effect into solar steam is highly desirable for addressing freshwater shortages and water ***,a ternary film structure for the adsorption and photothermal and photocatalytic treatment of wastewater was designed by combining the technique of self-assembled carbon nano paper with a nitrogen composite titanium dioxide(N-TiO_(2))deposited on the surface of carbon nanotubes(CNT)using polyvinylidene fluoride(PVDF)as a *** photogeneration of reactive oxygen species can be promoted by rapid oxygen diffusion at the three-phase interface,whereas the interfacial photothermal effect promotes subsequent free radical reactions for the degradation of rhodamine B(93%).The freshwater evaporation rate is 1.35 kg·m^(-2)·h^(-1)and the solar-to-water evaporation efficiency is 94%.Importantly,the N-TiO_(2)/CNT/PVDF(N-TCP)film not only effectively resists mechanical damage from the environment and maintains structural integrity,but can also be made into a large film for outdoor experiments in a large solar energy conversion device to collect fresh water from polluted water and degrade organic dyes in source water simultaneously,opening the way for applications in energy conversion and storage.

关键词： Wastewater disposal Solar-driven distill Thin-layer flow Clean water production Ternary film

Carbonitride MXene Ti_(3)CN(OH)_(x)@MoS_(2)hybrids as efficient electrocatalyst for enhanced hydrogen evolution

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Nano Research 2023年第4期16卷 4656-4663页

作者： Jizhou Jiang Fangyi Li Saishuai Bai Yongjing Wang Kun Xiang Haitao Wang Jing Zou Jyh-Ping Hsu School of Environmental Ecology and biological engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China department of chemical engineering “National Taiwan University”Taipei 10617

Renewable energy powered electrocatalytic water splitting is a promising strategy for hydrogen generation,and the design and development of high-efficiency and earth-abundant electrocatalysts for hydrogen evolution reaction(HER)are highly ***,MoS2 nanoflowers decorated two-dimensional carbonitride-based MXene Ti3CN(OH)x hybrids have been constructed by etching and post-hydrothermal *** electrochemical performance of the as-obtained Ti_(3)CN(OH)_(x)@MoS_(2)hybrids having a quasi core-shell structure is fascinating:An overpotential of 120 mV and a Tafel slope of 64 mV∙dec^(−1)can be delivered at a current density of 10 mA∙cm^(−2).And after 3,000 cyclic voltammetry cycles,it can be seen that there is no apparent *** the experimental results and density functional theory(DFT)calculations indicate that the synergetic effects between Ti_(3)CN(OH)x and MoS_(2)are responsible for the robust electrochemical HER *** electrons of-OH group in Ti_(3)CN(OH)x are transferred to MoS_(2),making the adsorption energy of the composite for H almost *** metallic Ti_(3)CN(OH)x is also beneficial to the fast charge transfer *** construction of MXene-based hybrids with optimal electronic structure and unique morphology tailored to the applications can be further used in other promising energy storage and conversion devices.

关键词： Ti_(3)CN(OH)x MoS_(2) hydrogen evolution reaction density functional theory(DFT)calculations