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Journal of Energy Chemistry 2022年第5期31卷 411-419页

作者： Canfu Zhang Binbin Chen Haoran Cai Renzhi Huang Yingchun Liu Huilin Pan Department of Chemistry Zhejiang UniversityHangzhou 310027ZhejiangChina

Exploring low-cost and effective approaches to extend the potentials of aqueous electrolytes is highly ***,it is found that the activity of H_(2)O in aqueous electrolytes could be intensively manipulated by introducing small urea and long-chain polyethylene glycol(PEG)molecules into Li TFSI-H_(2)O electrolyte systems without super salt *** urea and PEG molecules could exclude partial coordinated H_(2)O out of the inner solvation shell of Li_(4) and reconstruct hydrogen-bonding network between H_(2)O and PEG molecules outside the solvation sheaths with restricted H_(2)O activity and extended electrochemical *** bonding competitions in aqueous electrolytes and their correlation to the electrochemical performance of full cells are *** the occurrence probability of H_(2)O around Li_(4)is lower than 40%,stable cycling of 3.1 V LiMn_(2)O_(4)-Li_(4)Ti_(5)O_(12) full cell is achieved,showing 73%capacity retention after 200 cycles at 1 C rate in optimal *** work provides new avenues to understand the role of H_(2)O and explore low-cost and effective approaches for the development of nextgeneration aqueous lithium-ion batteries.

关键词： Solvation sheath H_(2)O activity Aqueous electrolytes Lithium-ion batteries

A Superaerophobic Bimetallic Selenides Heterostructure for Efficient Industrial-Level Oxygen Evolution at Ultra-High Current Densities

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Nano-Micro Letters 2020年第8期12卷 213-224页

作者： Jiaxin Yuan Xiaodi Cheng Hanqing Wang Chaojun Lei Sameer Pardiwala Bin Yang Zhongjian Li Qinghua Zhang Lecheng Lei Shaobin Wang Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China Institute of zhejiang university-Quzhou Quzhou 324000People’s Republic of China Ningbo Research Institute Zhejiang UniversityNingbo 315100People’s Republic of China zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia

Cost-effective and stable electrocatalysts with ultra-high current densities for electrochemical oxygen evolution reaction(OER)are critical to the energy crisis and environmental ***,we report a superaerophobic three dimensional(3D)heterostructured nanowrinkles of bimetallic selenides consisting of crystalline NiSe2 and NiFe2Se4 grown on NiFe alloy(NiSe2/NiFe2Se4@NiFe)prepared by a thermal selenization *** this unique 3D heterostructure,numerous nanowrinkles of NiSe2/NiFe2Se4 hybrid with a thickness of ~100 nm are grown on NiFe alloy in a uniform *** by the large active surface area and high electronic conductivity,the superaerophobic NiSe2/NiFe2Se4@NiFe heterostructure exhibits excellent electrocatalytic activity and durability towards OER in alkaline media,outputting the low potentials of 1.53 and 1.54 V to achieve ultra-high current densities of 500 and 1000 mA cm^−2,respectively,which is among the most active Ni/Fe-based selenides,and even superior to the benchmark Ir/C *** in-situ derived FeOOH and NiOOH species from NiSe2/NiFe2Se4@NiFe are deemed to be efficient active sites for OER.

关键词： Superaerophobicity Bimetallic selenide Heterostructure electrocatalyst Strong interfacial coupling Oxygen evolution reaction

Nitrogen-Doped Carbon-Encased Bimetallic Selenide for High-Performance Water Electrolysis

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Nano-Micro Letters 2019年第4期11卷 185-195页

作者： Junhui Cao Kexin Wang Jiayi Chen Chaojun Lei Bin Yang Zhongjian Li Lecheng Lei Yang Hou Kostya Ostrikov Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058People’s Republic of China Ningbo Research Institute Zhejiang UniversityNingbo 315100People’s Republic of China Institute of zhejiang university-Quzhou 78 Jiuhua Boulevard NorthQuzhou 324000People’s Republic of China School of Chemistry Physicsand Mechanical EngineeringQueensland University of TechnologyBrisbaneQLD 4000Australia

Demand of highly efficient earth-abundant transition metal-based electrocatalysts to replace noble metal materials for boosting oxygen evolution reaction(OER)is rapidly ***,an electrochemically exfoliated graphite(EG)foil supported bimetallic selenide encased in N-doped carbon(EG/(Co,Ni)Se2-NC)hybrid is developed and synthesized by a vapor-phase hydrothermal strategy and subsequent selenization *** as-prepared EG/(Co,Ni)Se2-NC hybrid exhibits a core-shell structure where the particle diameter of(Co,Ni)Se2 core is about 70 nm and the thickness of N-doped carbon shell is approximately 5 *** from the synergistic effects between the combination of highly active Co species and improved electron transfer from Ni species,and N-doped carbon,the EG/(Co,Ni)Se2-NC hybrid shows remarkable electrocatalytic activity toward OER with a comparatively low overpotential of 258 mV at an current density of 10 mA cm?2 and a small Tafel slope of 73.3 mV dec?*** excellent OER catalysis performance of EG/(Co,Ni)Se2-NC hybrid is much better than that of commercial Ir/C(343 mV at 10 mA cm?2 and 98.1 mV dec?1),and even almost the best among all previously reported binary CoNi selenide-based OER ***,in situ electrochemical Raman spectroscopy combined with ex situ X-ray photoelectron spectroscopy analysis indicates that the superb OER catalysis activity can be attributed to the highly active Co-OOH species and modified electron transfer process from Ni element.

关键词： Core-shell structure Bimetallic selenide N-doped carbon Synergistic effect Oxygen evolution reaction

Self-supported hierarchical porous Li_(4)Ti_(5)O_(12)/carbon arrays for boosted lithium ion storage

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Journal of Energy Chemistry 2021年第3期30卷 754-760页

作者： Jun Liu Aixiang Wei Guoxiang Pan Shenghui Shen Zhiming Xiao Yu Zhao Xinhui Xia Guangdong Provincial Key Laboratory of Functional Soft Condensed Matter School of Materials and EnergyGuangdong University of TechnologyGuangzhou 510006GuangdongChina School of Information Science Xinhua College of Sun Yat-sen UniversityGuangzhou 510520GuangdongChina Department of Materials Chemistry Huzhou UniversityHuzhou 313000ZhejiangChina State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Provinceand Department of Materials Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina

The development of fast rechargeable lithium ion batteries(LIBs)is highly dependent on the innovation of advanced high-power electrode *** this work,for the first time,we report a sacrificial NiO arrays template method for controllable synthesis of self-supported hierarchical porous Li_(4)Ti_(5)O_(12)/C(LTO/C)nanoflakes arrays,for use as fast rechargeable anodes for *** ultrathin(2-3 nm)carbon layer was uniformly coated on the LTO forming arrays *** hierarchical porous LTO/C nanoflakes consisted of primary cross-linked nanoparticles of 50-100 nm and showed large *** of the enhanced electrical conductivity and accelerated ion transfer channels,the well-designed binderfree porous LTO/C nanoflakes arrays exhibited notable high-rate lithium ion storage performance with smaller polarization,better electrochemical reactivity,higher specific capacity(157 mAh g^(-1) at the current density of 20C)and improved long-term cycling life(96.2% after 6000 cycles at 20C),superior to the unmodified porous LTO arrays counterpart(126 mAh g^(-1) at 20C and 88.0%after 6000 cycles at 20C).Our work provides a new template for the construction of high-performance high-rate electrodes for electrochemical energy storage.

关键词： Lithium titanate Carbon Anode High rate Lithium ion batteries

Nitrogen-Doped Sponge Ni Fibers as Highly Effcient Electrocatalysts for Oxygen Evolution Reaction

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Nano-Micro Letters 2019年第2期11卷 37-47页

作者： Kaili Zhang Xinhui Xia Shengjue Deng Yu Zhong Dong Xie Guoxiang Pan Jianbo Wu Qi Liu Xiuli Wang Jiangping Tu State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang ProvinceDepartment of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China Guangdong Engineering and Technology Research Center for Advanced Nanomaterials School of Environment and Civil EngineeringDongguan University of TechnologyDongguan 523808People’s Republic of China Department of Materials Chemistry Huzhou UniversityHuzhou 313000People’s Republic of China zhejiang Provincial Key Laboratory for Cutting Tools Taizhou UniversityTaizhou 318000People’s Republic of China Department of Physics City University of Hong KongKowloon 999077Hong Kong Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China

Controllable synthesis of highly active micro/nanostructured metal electrocatalysts for oxygen evolution reaction(OER) is a particularly significant and challenging ***,we report a 3D porous sponge-like Ni material,prepared by a facile hydrothermal method and consisting of cross-linked micro/nanofibers,as an integrated binder-free OER *** further enhance the electrocatalytic performance,an N-doping strategy is applied to obtain N-doped sponge Ni(N-SN) for the first time,via NH3 *** to the combination of the unique conductive sponge structure and N doping,the as-obtainedN-SN material shows improved conductivity and a higher number of active sites,resulting in enhanced OER performance and excellent ***,N-SN exhibits a low overpotential of 365 mV at 100 mA cm-2 and an extremely small Tafel slope of 33 mV dec-1,as well as superior long-term stability,outperforming unmodified sponge ***,the combination of X-ray photoelectron spectroscopy and near-edge X-ray adsorption fine structure analyses shows that γ-NiOOH is the surface-active phase for ***,the combination of conductive sponge structure and N-doping modification opens a new avenue for fabricating new types of high-performance electrodes with application in electrochemical energy conversion devices.

关键词： Oxygen evolution reaction Electrocatalysis Nickel Sponge Structure Electrochemical energy conversion

Bi/Bi2O3 nanoparticles supported on N-doped reduced graphene oxide for highly efficient CO2 electroreduction to formate

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Chinese Chemical Letters 2020年第6期31卷 1415-1421,F0002页

作者： Junjie Sun Wanzhen Zheng Siliu Lyu Feng He Bin Yang Zhongjian Li Lecheng Lei Yang Hou College of Environment Zhejiang University of TechnologyHangzhou 310014China Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Ningbo Research Institute Zhejiang UniversityNingbo 315100China

Electrocatalytic CO2 reduction(CO2 ER)into formate is a desirable route to achieve efficient transformation of CO2 to value-added chemicals,however,it still suffers from limited catalytic activity and poor ***,we develop a hybrid electrocatalyst composed of bismuth and bismuth oxide nanoparticles(NPs)supported on nitrogen-doped reduced graphene oxide(Bi/Bi2 O3/NrGO)nanosheets prepared by a combined hydrothermal with calcination *** to the combination of undercoordinated sites and strong synergistic effect between Bi and Bi2 O3,Bi/Bi2 O3/NrGO-700 hybrid displays a promoted CO2 ER catalytic performance and selectivity for formate production,as featured by a small onset potential of-0.5 V,a high current density of-18 mA/cm2,the maximum Faradaic efficiency of85%at-0.9 V,and a low Tafel slope of 166 mV/*** results reveal that the higher CO2 ER performance of Bi/Bi2 O3/NrGO-700 than that of Bi NPs supported on NrGO(Bi/NrGO)can be due to the partial reduction of Bi2 O3 NPs into Bi,which significantly increases undercoordinated active sites on Bi NPs surface,thus boosting its CO2 ER ***,a two-electrode device with Ir/C anode and Bi/Bi2 O3/NrGO-700 cathode could be integrated with two alkaline batteries or a planar solar cell to achieve highly active water splitting and CO2 ER.

关键词： NrGO Bi/Bi2O3 CO2 electroreduction Formate Hybrid catalysts

Nanostructured Ternary Metal Tungstate-Based Photocatalysts for Environmental Purification and Solar Water Splitting:A Review

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Nano-Micro Letters 2018年第4期10卷 201-227页

作者： Jun Ke M.Adnan Younis Yan Kong Hongru Zhou Jie Liu Lecheng Lei Yang Hou School of Chemistry and Environmental Engineering Wuhan Institute of Technology Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University Department of Environmental Science and Engineering North China Electric Power University

Visible-light-responsive ternary metal tungstate(MWO_4) photocatalysts are being increasingly investigated for energy conversion and environmental purification applications owing to their striking features, including low cost,eco-friendliness, and high stability under acidic and oxidative conditions. However, rapid recombination of photoinduced electron–hole pairs and a narrow light response range to the solar spectrum lead to low photocatalytic activity of MWO_4-based materials, thus significantly hampering their wide usage in practice. To enable their widespread practical usage, significant efforts have been devoted, by developing new concepts and innovative strategies. In this review, we aim to provide an integrated overview of the fundamentals and recent progress of MWO_4-based photocatalysts. Furthermore, different strategies, including morphological control, surface modification, heteroatom doping, and heterojunction fabrication, which are employed to promote the photocatalyticactivities of MWO_4-based materials, are systematically summarized and discussed. Finally, existing challenges and a future perspective are also provided to shed light on the development of highly efficient MWO_4-based photocatalysts.

关键词： Ternary metal tungstates Micro- and nanostructures Photocatalysis Environmental purification Water splitting

N-doped carbon nanofibers arrays as advanced electrodes for supercapacitors

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Journal of Materials Science & Technology 2020年第20期52卷 144-151页

作者： Guoxiang Pan Feng Cao Yujian Zhang Xinhui Xia Department of Materials Chemistry Huzhou UniversityHuzhou 313000China State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Provinceand Department of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China

The advancement of supe rcapacitors largely relies on the innovation of electrode materials with high-rate performance and ultra-long cycling *** this work,unique N-doped nanofibers on carbon cloth(NCNFs/CC) are prepared by an electrodepositio n-annealing method for application in *** as-prepared N-doped nanofibers(N-CNFs) show diameters of 100-150 nm and cross-link with each other fo rming porous conductive *** to enhanced conductivity and reinforced structural stability,the N-CNFs/CC arrays are demonstrated with better electrochemical performance than CNFs/CC counterpart,including higher specific capacitance(195.2 F g^-1 at a current density of 2.5 A g^-1),excellent rate capability(80.5.% capacity retention as the rate increases from 2.5-20 A g^-1) and good cycling stability(99.5.%retention after 10,000 cycles).These reinforced electrochemical properties are attributed to N-doped conductive architecture with faster ion/electron transfer paths and more active *** findings may offe r a new way for construction of advanced high-rate electrodes for energy storage.

关键词： Supercapacitors Carbon fibers Electrode Porous materials Electrodeposition

A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N_4 Sites for CO_2 Electroreduction

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Nano-Micro Letters 2020年第9期12卷 14-25页

作者： Wanzhen Zheng Feng Chen Qi Zeng Zhongjian Li Bin Yang Lecheng Lei Qinghua Zhang Feng He Xilin Wu Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China College of Geography and Environmental Science Zhejiang Normal UniversityJinhua 321004People’s Republic of China College of Environment Zhejiang University of TechnologyHangzhou 310014People’s Republic of China Institute of zhejiang university-Quzhou Quzhou 324000People’s Republic of China Ningbo Research Institute Zhejiang UniversityNingbo 315100People’s Republic of China zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China

Atomically dispersed metal-nitrogen sites-anchored carbon materials have been developed as effective catalysts for CO2 electroreduction(CO2 ER),but they still suffer from the imprecisely control of type and coordination number of N atoms bonded with central ***,we develop a family of single metal atom bonded by N atoms anchored on carbons(SAs-M-N-C,M=Fe,Co,Ni,Cu)for CO2 ER,which composed of accurate pyrrole-type M-N4 structures with isolated metal atom coordinated by four pyrrolic N *** from atomically coordinated environment and specific selectivity of M-N4 centers,SAs-Ni-N-C exhibits superior CO2 ER performance with onset potential of-0.3 V,CO Faradaic efficiency(F.E.) of 98.5%at-0.7 V,along with low Tafel slope of 115 mV dec-1 and superior stability of 50 h,exceeding all the previously reported M-N-C electrocatalysts for CO2-to-CO *** results manifest that the different intrinsic activities of M-N4 structures in SAs-M-N-C result in the corresponding sequence of Ni> Fe> Cu> Co for CO2 ER *** integrated Zn-CO2 battery with Zn foil and SAs-Ni-N-C is constructed to simultaneously achieve CO2-to-CO conversion and electric energy output,which delivers a peak power density of 1.4 mW cm-2 and maximum CO *** 93.3%.

关键词： Atomic dispersion Pyrrole-type metal–N4 structure Catalytic site CO2 electroreduction Zn–CO2 battery

N-doped CoO nanowire arrays as efficient electrocatalysts for oxygen evolution reaction

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Journal of Energy Chemistry 2019年第10期28卷 13-17页

作者： Kaili Zhang Xinhui Xia Shengjue Deng Dong Xie Yangfan Lu Yadong Wang Jianbo Wu Xiuli Wang Jiangping Tu State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Provinceand School of Materials Science & EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Guangdong Engineering and Technology Research Center for Advanced Nanomaterials School of Environment and Civil EngineeringDongguan University of TechnologyDongguan 523808GuangdongChina School of Engineering Nanyang Polytechnic569830Singapore zhejiang Provincial Key Laboratory for Cutting Tools Taizhou UniversityTaizhou 318000ZhejiangChina

Rational design of cost-effective high-performance electrocatalysts for oxygen evolution reaction (OER) is of great significance for electrochemical water splitting. Herein, we adopt a nitrogen doping method to fabricate self-supported N-doped CoO nanowire arrays (N-CoO) as active electrocatalysts via a facile hydrothermal combined doping method. The N-CoO nanowires are strongly composited with the carbon cloth substrate forming free-standing electrode with reinforced stability and high electronic conductivity. Owing to the increased accessible and electroactive areas, rich/short pathways for charge transfer and enhanced electronic conductivity, the N-CoO electrode exhibits excellent electrocatalytic performance for OER with a low overpotential (319 mV at 10 mA cm^-2 and 410 mV at 100 mA cm^-2) and a low Tafel slope of 74 mV dec^-1 as well as superior long-term stability with no decay in 24 h continuous test in alkaline solution. Our reported design and optimization strategy provide a promising way to construct interesting well-aligned arrays for application in energy storage and conversion.

关键词： Oxygen evolution reaction Nanowires Electrocatalysis Porous structure Cobalt Oxides