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Interface-engineered MoS_(2)/CoS/NF Bifunctional catalysts for highly-efficient water electrolysis

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Journal of Energy Chemistry 2022年第12期75卷 16-25,I0002页

作者： Wenxia Chen Xingwang Zhu Rui Wang Wei Wei Meng Liu Shuai Dong Kostya Ken Ostrikov Shuang-Quan Zang School of Chemistry and Chemical Engineering Henan Key Laboratory of Biomolecular Recognition and SensingHenan D&A Engineering Center of Advanced Battery MaterialsShangqiu Normal UniversityShangqiu 476000HenanChina Henan Key Laboratory of Crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001HenanChina College of Environmental Science and Engineering Yangzhou UniversityYangzhou 225009JiangsuChina School of Chemistry and Physics and Centre for Materials Science Queensland University of Technology(QUT)BrisbaneQLD 4000Australia

The utilization of non-noble metal catalysts with robust and highly efficient electrocatalytic activity for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are extremely important for the large-scale implementation of renewable energy devices.Integration of bifunctional electrocatalysts on both anode and cathode electrodes remains a significant challenge.Herein,we report on a novel and facile strategy to construct the ordered and aligned MoS_(2)nanosheet-encapsulated metal–organic frameworks(MOFs)derived hollow CoS polyhedron,in-situ grown on a nickel foam(NF).The starfish-like MoS_(2)/CoS/NF heterojunctions were formed due to the ordered growth of the material caused by NF substrate.The optimized 2-MoS_(2)/CoS/NF heterojunction exhibits robust bifunctional electrocatalytic activity with a low overpotential of 67 and 207 m V toward the HER and OER at 10 mA cm^(-2),and the long-term stability,which exceeds most of the reported bifunctional electrocatalysts.Such high electrocatalytic performance arises due to the synergistic effect between the MoS_(2)and CoS phases across the interface,the abundant active sites,as well as the hierarchical pore framework,which collectively enhance the mass and electron transfer during the reactions.The work provides a promising approach to fabricating Bifunctional catalysts with custom-designed heterojunctions and remarkable performance for applications in electrochemical energy devices and related areas.

关键词： Heterojunction Bifunctional catalysts HER OER

Efficient conversion of benzene and syngas to toluene and xylene over ZnO-ZrO_(2)&H-ZSM-5 Bifunctional catalysts

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Chinese Journal of Chemical Engineering 2022年第5期35卷 203-210页

作者： Xiao Zhao Xuan Shi Zhongshun Chen Long Xu Chengyi Dai Yazhou Zhang Xinwen Guo Dongyuan Yang Xiaoxun Ma School of Chemical Engineering Northwest UniversityXi’an 710069China International Science&Technology Cooperation Base for Clean Utilization of Hydrocarbon Resources Chemical Engineering Research Center of the Ministry of Education for Advanced Use Technology of Shanbei EnergyCollaborative Innovation Center for Development of Energy and Chemical Industry in Northern ShaanxiNorthwest UniversityXi’an 710069China School of Chemical Engineering Dalian University of TechnologyDalian 116024China Shaanxi Key Laboratory of Energy Chemical Process Intensification School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China Shanxi yanchang Petroleum(Group)Corp.LtdXi’an 710000China

A series of ZnO-ZrO_(2) solid solutions with different Zn contents were synthesized by the urea coprecipitation method,which were coupled with H-ZSM-5 zeolite to form Bifunctional catalysts.As a new benzene alkylation reagent,syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene.A suitable ratio of ZnO-ZrO_(2) led to the significant improvement in the catalytic performance,and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C^(9+) aromatics.The highest benzene conversion of 89.2%and toluene/xylene selectivity of 88.7%were achieved over 10%ZnO-ZrO_(2)&H-ZSM-5(Si/Al=23)at a pressure of 3 MPa and a temperature of 450℃.In addition,the effect of the zeolite framework structure on product distribution was examined.Similar to the molecular dynamics of aromatic hydrocarbons,H-ZSM-5 zeolites comprise 10-membered-ring pores,which are beneficial to the activation of benzene;hence,the conversion of benzene is higher.H-ZSM-35 and HMOR zeolites exhibited small eight-membered-ring channels,which were not conducive to the passage of benzene;hence,the by-product ethylbenzene exhibits a higher selectivity.The distance between the active centers of the Bifunctional catalysts was the main factor affecting the catalytic performance,and the powder mixing method was more conducive to the conversion of syngas and benzene.

关键词： ZnO-ZrO_(2) Bifunctional catalysts Aromatics Alkylation of benzene Syngas

Decavanadate-based Transition Metal Hybrids as Bifunctional catalysts for Sulfide Oxidation and C-C Bond Construction

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Chinese Journal of Chemistry 2021年第9期39卷 2495-2503页

作者： Xianqiang Huang Xiaoyu Gu Yuquan Qi Yanru Zhang Guodong Shen Bingchuan Yang Wenzeng Duan Shuwen Gong Zechun Xue Yifa Chen Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry&Chemical EngineeringLiaocheng UniversityLiaochengShandong 252059China Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjingJiangsu 210023China

The development of Bifunctional catalysts has drawn much attention in realizing efficient and feasible catalytic systems to meet the diverse dema nd of pote ntial industrial applications.Desig n of stable and powerful bifun ctional catalysts for various catalysis systems is highly desirable yet largely unmet.Here,three kinds of decavanadate-based transition metal hybrids(DTMH)(i.e.,Co-DTMH,Ni-DTMH and Ag-DTMH)have been successfully synthesized through a pH tuning strategy and further characterized.Specifically,the rare M05N six-coordinated transition metal coordination modes have been detected in Co-DTMH and Ni-DTMH,while Ag atoms in Ag-DTMH exhibited three-and five-coordinated geometries with the tuning of specially selected imidazole ligands.Thus-obtained clusters can serve as powerful Bifunctional catalysts for both sulfide oxidation and C-C bond construction.Remarkably,Ag-DTMH dem on st rated excellent heteroge ne ous bifunctional catalytic properties in the selective oxidati on of sulfides and construction of C-C bond(yields up to 99%),which enable successful recycling for three cycles with remained catalytic activities and structure stability.The newly designed decavanadate-based transition metal hybrids with bifunctional property hold high promise in the practical applications like continuous catalysis or flow bed reactions.

关键词： Polyoxometalates Crystal engineering Bifunctional catalysts Oxidation of sulfides Heterogeneous catalysis

Research progress of transition metal compounds as Bifunctional catalysts for zinc-air batteries

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Nano Research Energy 2024年第1期3卷 78-100页

作者： Yan Ran Changfan Xu Deyang Ji Huaping Zhao Liqiang Li Yong Lei Fachgebiet Angewandte Nanophysik Institut für Physik&IMN MacroNanoTechnische Universität IlmenauIlmenau 98693Germany Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistryInstitute of Molecular Aggregation ScienceTianjin UniversityTianjin 300072China

Zinc-air batteries(ZABs)are widely studied because of their high theoretical energy density,high battery voltage,environmental protection,and low price.However,the slow kinetics of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)on the air electrode limits the further application of ZABs,so that how to develop a cheap,efficient,and stable catalyst with bifunctional catalytic activity is the key to solving the development of ZABs.Transition metal compounds are widely used as cathode materials for ZABs due to their low cost,high electrocatalytic activity,and stable structure.This review summarizes the research progress of transition metal compounds as Bifunctional catalysts for ZABs.The development history,operation principle,and mechanism of ORR and OER reactions are introduced first.The application and development of transition metal compounds as Bifunctional catalysts for ZABs in recent years are systematically introduced,including transition metal oxides(TMOs),transition metal nitrides(TMNs),transition metal sulfides(TMSs),transition metal carbides(TMCs),transition metal phosphates(TMPs),and others.In addition,the shortcomings of transition metal compounds as Bifunctional catalysts for ZABs were summarized and reasonable design strategies and improvement measures were put forward,aiming at providing a reference for the design and construction of high-performance ZABs cathode materials.Finally,the challenges and future in this field are discussed and prospected.

关键词： transition metal compounds zinc-air batteries Bifunctional catalysts electrochemical air electrode

La0.5Sr0.5CoO3-δ/Ti3C2Tx as bifunctional Efficient Hybrid catalysts for Li-O2 battery

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La0.5Sr0.5CoO3-δ/Ti3C2Tx as Bifunctional Efficient Hybrid C...

MOF-Derived Co and Fe Species Loaded on N-Doped Carbon Networks as Efficient Oxygen Electrocatalysts for Zn-Air Batteries

中国化学会第十届全国无机化学学术会议

作者： Zemin Sun Mengwei Yuan Genban Sun Huifeng Li Beijing Key Laboratory of Energy Conversion and Storage Materials College of Chemistry Beijing Normal University

Li-oxygen batteries have drawn widespread attention in the past decades.Herein,bifunctional hybrid catalysts based on perovskite LaSrCo Owith TiCT MXene nanosheets are prepared for application as electrocatalysts in Li-oxygen batteries.It is the first time to use high Li ionic diffusion TiCT in Li-oxygen batteries and making it as substrate in-situ growth of high oxygen adsorption and Otransport perovskite LaSrCoO.In this way,the in-situ hybrid catalysts show outstanding catalytic performance to facilitate the reaction kinetics,which display overpotential of only 0.87 V,lower than the TiCT about 540 mV,LaSrCoOabout 430 mV.The Li-oxygen batteries with LaSrCoO/TiCT electrodes run more than 80 cycles at 500 mA g with capacity restriction of 1000 mAh g,much better than TiCT (9 cycles),LaSrCoO(15 cycles) and other reported catalysts based on the perovskite.Moreover,the Li-oxygen batteries with LaSrCoO/TiCT electrode deliver highest initial discharge capacity about 11340 mAh g at 500 mA g,which is about twice than LaSrCoO cathode(6700 m Ah g) and TiCT (5210 m Ah g).All the results suggest that the strategy would be a promising approach to enhance the LOBs performance.

关键词： perovskite LaSrCoO Ti3C2Tx MXene nanosheets Bifunctional catalysts Li-O2 battery insitu hydrothermal synthesis

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Nano-Micro Letters 2022年第10期14卷 136-147页

作者： Yuanyuan Xue Yibo Guo Qinming Zhang Zhaojun Xie Jinping Wei Zhen Zhou School of Materials Science and Engineering Institute of New Energy Material ChemistryKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Renewable Energy Conversion and Storage Center(ReCast)Nankai UniversityTianjin 300350People’s Republic of China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China

Searching for cheap,efficient,and stable oxygen electrocatalysts is vital to promote the practical performance of Zn-air batteries with high theoretic energy density.Herein,a series of Co nanoparticles and highly dispersed Fe loaded on N-doped porous carbon substrates are pre-pared through a“double-solvent”method with in situ doped metal-organic frameworks as pre-cursors.The optimized catalysts exhibit excellent performance for oxygen reduction and evolution reaction.Furthermore,rechargeable Zn-air bat-teries with designed catalysts demonstrate higher peak power density and better cycling stability than those with commercial Pt/C+RuO_(2).According to structure characterizations and electrochemical tests,the interaction of Co nanoparticles and highly dispersed Fe contributes to the superior performance for oxygen electrocatalysis.In addition,large specific surface areas,porous struc-tures and interconnected three-dimensional carbon networks also play important roles in improving oxygen electrocatalysis.This work provides inspiration for rational design of advanced oxygen electrocatalysts and paves a way for the practical application of rechargeable Zn-air batteries.

关键词： Oxygen reduction reaction Oxygen evolution reaction Zn-air batteries Bifunctional catalysts Metal-organic frameworks

Dual-Confined Bead-Like CoSe_(2)@NC@NCNFs bifunctional Catalyst Boosting Rechargeable Zinc-Air Batteries

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Chinese Journal of Chemistry 2024年第4期42卷 397-405页

作者： Kuixing Ding Jiugang Hu Liming Zhao Huanan Yu Shan Cai Yi Yang Jun Tan Hongshuai Hou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangshaHunan410083 China College of Materials and Chemistry China Jiliang UniversityHangzhouZhejiang310018 China College of Standardization China Jiliang UniversityHangzhouZhejiang310018 China

Rationally developing efficient and durable Bifunctional catalysts toward oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is critical for rechargeable zinc-air batteries(ZABs).Herein,a bead-like CoSe_(2)@NC@NCNFs bifunctional catalyst was designed and fabricated by confining cubic CoSe_(2)nanoparticles to three-dimensional(3D)porous MOFs-derived nitrogen-doped carbon(NC)and one-dimensional(1D)N-doped carbon nanofibers(NCNFs)through a facile encapsulate strategy.The 1D/3D continuous network structure contributes to the improvement of specific surface area and electronic conductivity,while the strong synergistic effect between CoSe_(2)sites and Co-Nx-C sites can effectively enhance electron/mass transfer and reduce the diffusion resistance.The as-constructed CoSe_(2)@NC@NCNFs catalyst exhibits high catalytic activity and stability toward ORR/OER with a high half-wave potential of 0.80 V(vs.RHE)in ORR and a low overpotential of 280 mV at 10 mA·cm^(−2)in OER.More encouragingly,the rechargeable ZABs with CoSe_(2)@NC@NCNFs cathode deliver high peak power densities(126.8 mW·cm^(−2)),large specific capacities(763.1 mA·h·g^(−1)),and robust charge-discharge cycling stability over 240 cycles.This study provides a facile strategy for designing efficient Bifunctional catalysts for rechargeable energy conversion applications.

关键词： Dual-confined Electrospinning Cobalt selenide Bifunctional catalysts Rechargeable zinc-air batteries

Surface/Interface Engineering of Hierarchical MoO_(2)/MoNi_(4)@Ru/RuO_(2)Heterogeneous Nanosheet Arrays for Alkaline Water Electrolysis with Fast Kinetics

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Chinese Journal of Chemistry 2024年第2期42卷 119-128页

作者： Qiong Zhang Ruixue Zhang Yingxiu Zhao Tiantian Sun Jianyang Gao Guang-Rui Xu Zexing Wu Yu Yang Lei Wang Key Laboratory of Eco-chemical Engineering Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life ScienceTaishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and TechnologyCollege of Chemistry and Molecular EngineeringSchool of Materials Science and EngineeringQingdao University of Science and TechnologyQingdaoShandong 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdaoShandong 266042China

Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable Bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water splitting.Here,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of Ru.Benefiting from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performances.The synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water electrolysis.Moreover,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline media.When building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity.

关键词： Hierarchical heterostructure Surface engineering Bifunctional catalysts Hydrogen evolution reaction Oxygen evolution reaction Watersplitting Catalytic activity Electrocatalysis Heterogeneous catalysis

Simultaneous acceleration of sulfur reduction and oxidation on bifunctional electrocatalytic electrodes for quasi-solid-state Zn–S batteries

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Science China Chemistry 2024年第5期67卷 1531-1538页

作者： Mingli Wang Hong Zhang Tianhang Ding Fangjun Wu Lin Fu Bin Song Pengfei Cao Ke Lu Institutes of Physical Science and Information Technology School of Materials Science and EngineeringKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei 230601China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001China School of Chemistry and Chemical Engineering Guizhou UniversityGuiyang 550025China Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123China State Key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China

The incomplete sulfur reduction and high ZnS re-oxidation energy barrier along with severe side reactions during the battery cycling compromise the practical application of Zn–S electrochemistry. Herein, a bifunctional electrocatalytic sulfur matrix that simultaneously accelerates the sulfur reduction and ZnS oxidation is proposed to realize a highly-efficient Zn–S cell. It is revealed that the N-heteroatom hotspots are more favorable for facilitating the conversion of S to ZnS while the CoO nanocrystal substantially lowers the ZnS activation energy barrier thereby suppressing the formation of disproportionation species(e.g.,SO_(4)^(2-)) and accumulation of inactive ZnS. Accordingly, the Co O anchored on the N-doped carbon-supported sulfur cathode delivers a high Zn^(2+)storage capacity of 1,172 m Ahg^(-1)and outstanding cycling stability with a capacity retention of 71.6% after500 cycles with a high average Coulombic efficiency of 97.8%. Simultaneously, the stable cycling of solid-state Zn–S pouch cells with an energy density of 585 Whkg^(-1)sulfuris also demonstrated. Moreover, the postmortem analysis reveals that the degradation of Zn–S cells is mainly attributed to the limited reversibility of Zn anodes rather than the ZnS decomposition and/or accumulation. The approach to the bidirectional catalysis manipulated the sulfur redox provides a new perspective to realize the theoretical potentials of Zn–S cells.

关键词： Zn–S battery Bifunctional catalysts solid-state battery sulfur redox degradation mechanism