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In-situ electrochemical activation designed hybrid electrocatalysts for water electrolysis

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Science Bulletin 2018年第13期63卷 853-876页

作者： Xiao Shang Bin Dong yong-ming chai Chen-Guang Liu State Key Laboratory of Heavy Oil Processing China University of Petroleum (East China) College of Science China University of Petroleum (East China)

Developing transition metal-based electrocatalysts with rich active sites for water electrolysis plays important roles in renewable energy fields. So far, some strategies including designing nanostructures, incorporating conductive support or foreign elements have been adopted to develop efficient electrocat- alysts. Herein, we summarize recent progresses and propose in-situ electrochemical activation as a new pretreating technique for enhanced catalytic performances. The activation techniques mainly comprise facile electrochemical processes such as anodic oxidation, cathodic reduction, etching, lithium-assisted tuning and counter electrode electro-dissolution. During these electrochemicaI treatments, the catalyst surfaces are modified from bulk phase, which can tune local electronic structures, create more active spe- cies. enlarge surface area and thus improve the catalytic performances. Meanwhile, this technique can couple the atomic, electronic structures with electrocatalysis mechanisms for water splitting. Compared to traditional chemical treatment, the in-situ electrochemical activation techniques have superior advantages such as facile operation, mild environment, variable control, high efficiency and flex- ibility. This review may provide guidance for improving water electrolysis efficiencies and hold promis- ing for application in many other energy-conversion fields such as supercapacitors, fuel cells and batteries.

关键词： In-situ electrochemical activation Transition metal Hybrid electrocatalyst Water electrolysis

Design and modulation principles of molybdenum carbide-based materials for green hydrogen evolution

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Journal of Energy Chemistry 2020年第9期29卷 398-423,I0012页

作者： Jing-Qi Chi Min Yang yong-ming chai Zhi Yang Lei Wang Bin Dong State Key Laboratory of Heavy Oil Processing College of ScienceChina University of Petroleum(East China)Qingdao 266580ShandongChina Key Laboratory of Thin Film and Microfabrication(Ministry of Education) Department of Micro/Nano ElectronicsSchool of Electronic Information and Electrical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Shandong Key Laboratory of Biochemical Analysis College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina

The green production of hydrogen from electrocatalytic water splitting is an important base and promising direction for the future of the large-scale application of hydrogen *** key of green hydrogen evolution depends on the development of low-cost and highly active *** carbides(MoxC),as a typical of earth-abundant transition-metal material,have accumulated great attention due to their low cost,earth abundance,electrical conductivity,similar d-band state to Pt,and regulated morphology/electronic *** this paper,recent researches focusing on MoxC for efficient HER in a wide pH range are summarized from respects of modulation of unique morphology,electronic structure,and electrode interface step by ***,modulation of morphology influence the apparent activity of catalyst,modulation of electronic structure of active sites by heteroatom doping and designing heterointerface boost intrinsic HER kinetics,and modulation of electrode interface via hybridization of MoxC structures with carbon materials can ensure the fast electron transfer and boost the *** the above methods discussed,perspective and challenges of designing MoxC as the substitute of Pt-based electrocatalyst for practical hydrogen generation in a wide pH range are pointed out.

关键词： Molybdenum carbides Classification Electrocatalyst Modulation strategy Hydrogen evolution

Transition Metal Boride-Based Materials for Electrocatalytic Water Splitting

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Chinese Journal of Structural Chemistry 2022年第9期41卷 8-44页

作者： Feng-Ge Wang Xin Liu Qian-Xi Lv Bin Liu yong-ming chai Bin Dong State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China

Electrocatalytic water splitting to produce hydrogen is an eco-friendly way to achieve sustainable utilization of renewable *** industrial application of water electrolysis, which is severely limited by slow kinetic reactions on electrode surfaces, requires the development of highly reactive, low-cost and stable electrocatalytic materials. Transition metal borides/borates have recently emerged as promising electrocatalytic materials for catalyzing hydrogen/oxygen evolution reactions(HER/OER) in inexpensive electrolyzers. However, so far, there has been little comprehensive summary of transition metal borides/borates. Here, this review provides the latest research progress on transition metal borides/borates for electrocatalytic water splitting. The structural characteristics of transition metal borides/borates and their synthesis methods in recent years are discussed. Then, the theoretical and experimental progress of transition metal borides including single-metal borides, multi-metal borides, borate derived and other nanocomposites containing boron(boron-doped nanocomposites/substrate with boron) in electrocatalytic reaction and the role of boron in regulating electrocatalytic performance are further emphasized. Finally, the potential challenges and future prospects of transition metal borides/borates in electrocatalysis are presented.

关键词： transition metal borides/borates electrocatalysts hydrogen evolution reaction(HER) oxygen evolution reaction(OER) overall water splitting

High-pressure microwave-assisted synthesis of WS_(x)/Ni_(9)S_(8)/NF hetero-catalyst for efficient oxygen evolution reaction

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Rare Metals 2021年第5期40卷 1048-1055页

作者： Xue Ma Xin-Yu Zhang Min Yang Jing-Yi Xie Ren-Qing Lv yong-ming chai Bin Dong College of Science China University of Petroleum(East China)Qingdao 266580China State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266580China

Designing the specific crystal phase with better intrinsic activity and more active sites is a very promising strategy for earth-abundant electrocatalysts for oxygen evolution reaction(OER).Herein,a facile two-step method including the high-pressure microwave and the hydrothermal sulfurization is adopted to prepare the WS_(x)/Ni_(9)S_(8) hetero-catalyst on nickel foam(WS_(x)/Ni_(9)S_(8)/NF).Firstly,WO3 polyhedrons homogeneously cover the surface of NF through the high-pressure microwave hydrothermal ***,WS_(x)/Ni_(9)S_(8) nanoparticles on the surface of NF can be synthesized after a hydrothermal sulfurization,which has been confirmed by scanning electron microscopy(SEM) elemental mapping and high-resolution transmission electron microscopy(HRTEM).The amorphous WSx and Ni9 S8 phase may provide the dual active sites for *** electrochemical measurements show that WS_(x)/Ni_(9)S_(8)/NF has superior OER activity with a low overpotential of 320 mV at the current density of 100 mA·cm^(-2),better than those of other *** enhanced OER performance may be due to the synergistic catalysis from Ni9 S8 phase and high valence of *** to the stable structure of Ni9 S8,the long-term stability of WS_(x)/Ni_(9)S_(8)/NF for at least 10 h can be *** work may provide a new approach for the doped nickel sulfides crystal phase through high-pressure microwave hydrothermal assistance for OER.

关键词： Amorphous WS_(x) Ni_(9)S_(8) High-pressure microwave hydrothermal Electrocatalyst Oxygen evolution reaction

0D-2D Schottky heterostructure coupling of FeS nanosheets and Co_(9)S_(8)nanoparticles for long-term industrial-level water oxidation

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Nano Research 2023年第4期16卷 5929-5937页

作者： Hai-Jun Liu Ning Yu Xiao-Qing Yuan Hui-Ying Zhao Xin-Yu Zhang yong-ming chai Bin Dong State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China

The effective electron and interface/structural coupling for heterostructure electrocatalyst is the key to regulating the intrinsic activity and stability for oxygen evolution reaction(OER).Herein,a facile strategy is developed to fabricate well-dispersed zerodimensional(0D)metallic Co_(9)S_(8)nanoparticles on two-dimensional(2D)FeS nanosheets,forming FeS-Co_(9)S_(8)Schottky heterostructures with abundant heterointerfaces as OER *** strong electronic coupling between FeS and Co_(9)S_(8)expedites electrons flow from Fe atoms in FeS nanosheets to Co atoms in tetrahedron sites(CoTd),thereby leading to the structural integrity of the heterostructure and the constant exposure of active *** Raman spectroscopy also indicates the Co sites in the FeS-Co_(9)S_(8)Schottky heterostructure are OER active ***,FeS-Co_(9)S_(8)heterostructure supported by iron foam(FeS-Co_(9)S_(8)/IF)shows the remarkable activity and durability,achieving an industrial-level 500 mA·cm^(−2)current density at an overpotential of only 332 mV and maintaining for 100 *** work demonstrates that constructing Schottky heterostructure interface with strong coupling effect may be a good strategy for excellent catalytic performances.

关键词： Schottky heterostructure strong electronic coupling electron rearrangement operando Raman oxygen evolution reaction

Hollow Fe_(4)C/FeP Nanoboxes with Heterostructure and Carbon Armor for Efficient and Stable Hydrogen Evolution

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Chinese Journal of Structural Chemistry 2022年第7期41卷 53-58页

作者： Jing-Yi Xie Hui-Ying Zhao Yi-Wen Dong Yang Wu Da-Peng Liu yong-ming chai Bin Dong State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China

The heterojunction interfacial modulation of FeP is an effective strategy to regulate the intrinsic activity and stability, which is a major challenge to promote the industrial application of FeP-based electrocatalysts. Herein, hollow Fe_(4)C/FeP box with heterojunction interface and carbon armor is successfully synthesized, which can expose numerous active sites and protect catalyst from corrosion. Electrochemical measurements show that Fe_(4)C/FeP exhibits excellent hydrogen evolution activity and stability. It only needs 180 mV to achieve the current density of 10 mA cm^(-2). The high-activity may be due to the synergistic effects of porous framework, graphitic carbon coating and heterojunction structure of FeC and FeP, which optimize the electronic structure and accelerates electron transfer. In addition, the target catalyst can withstand 5000 cycles of CV testing without significant change in properties. The excellent stability may be attributed to the graphitic carbon coating as the armor that can prevent the catalyst from corrosion of electrolyte. This work may provide a synthetic approach to produce a series of carbon-coated and heterojunction structure of transition metal phosphides for water splitting.

关键词： carbon armor hollow box heterostructured electrocatalysts hydrogen evolution reaction

Crystal facet engineering of perovskite cobaltite with optimized electronic regulation for water splitting

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Science China Materials 2022年第10期65卷 2665-2674页

作者： Ya-Nan Zhou Feng-Ge Wang Yi-Nuo Zhen Jun Nan Bin Dong yong-ming chai State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China CNOOC Tianjin Chemical Research and Design Institute Co. LtdTianjin 300131China

The correlation between crystal facets and electronic configurations of perovskite is closely related to the intrinsic activity for water ***,we proposed a unique molten-salt method(MSM)to manipulate the electronic properties of LaCoO_(3) by fine-tuning its crystal facet and atomic ***_(3) samples with oriented(110)(LCO(110))and(111)(LCO(111))facets were motivated by a capping agent(Sr^(2+)).Compared with the LCO(111)plane,the LCO(110)and Sr-doped LCO(111)(LSCO(111))planes possessed higher O 2p positions,stronger Co 3d-O 2p covalencies,and higher Co spin states by inducing CoO_(6) distortion,thus leading to superior oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)***,the overpotentials at 10 mA cm^(−2) were 299,322,and 289 mV for LCO(110),LCO(111),and LSCO(111),*** addition,the(110)crystal facet and Sr substitution bestowed enhanced stability on LaCoO_(3) due to the strengthened Co-O *** present work enlightens new avenues of regulating electronic properties by crystal facet engineering and atom doping and provides a valuable reference for the electron structure-electrocatalytic activity connection for OER and HER.

关键词： electronic structure crystal facet engineering Sr doping LaCoO_(3) water splitting

Effective regulation mechanisms of Fe-Ni(oxy)hydroxide:Ni-rich heteroatomic bonding(Ni–O–Fe–O–Ni)is essential

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Nano Research 2023年第10期16卷 12026-12034页

作者： Ruo-Yao Fan Hui-Ying Zhao Zi-Yi Zhao Wen-Hui Hu Xin Liu Jian-Feng Yu Han Hu yong-ming chai Bin Dong State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China Stanford PULSE Institute SLAC National Accelerator LaboratoryMenlo ParkCA 95025USA

Although Fe-Ni combination performs well in transition metal-based oxygen evolution reaction(OER)electrocatalysts,there are lack of clear and general regulations mechanism to fully play the synergistic catalytic ***,we made the utmost of the interaction of Fe–Ni heteroatomic pair to obtain a highly active Fe-Ni(oxy)hydroxide catalytic layer on iron foam(IF)and nickel foam(NF)by in-situ electrochemical deposition and rapid surface reconstruction,which only required 327 and 351 mV overpotential to provide a large current of 1,000 mA·cm^(−2),*** results confirm that the moderate Ni-rich heteroatomic bonding(Ni–O–Fe–O–Ni)formed by adjusting the Ni/Fe ratio on the catalyst surface is important to offer predominant OER *** is a key component that enhances OER activity of Ni(O)OH,but Fe-rich structural surface formed by Fe–O–Ni–O–Fe bonding is not ***,the remarkable oxygen evolution performance of the prepared Ni2Fe(O)OH/IF and FeNi2(O)OH/NF can be chalked up to the optimized electronic structure of Fe–Ni heteroatomic bonding,the efficient gas spillover,the fast electron transport,and nanosheet clusters *** summary,our work suggests a comprehensive regulation mechanism for the construction of efficient Fe-Ni(oxy)hydroxide catalytic layer on inexpensive,stable,and self-supporting metallic material surface.

关键词： Fe-Ni(oxy)hydroxide oxygen evolution reaction(OER) heteroatomic bonding Ni-rich structure regulation mechanisms

Fe-doped CoP core–shell structure with open cages as efficient electrocatalyst for oxygen evolution

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Journal of Energy Chemistry 2020年第9期29卷 328-333,I0010页

作者： Jing-Yi Xie Zi-Zhang Liu Jia Li Lei Feng Min Yang Yu Ma Da-Peng Liu Lei Wang yong-ming chai Bin Dong College of Science State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum(East China)Qingdao 266580ShandongChina Shandong Key Laboratory of Biochemical Analysis College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina

Developing a facile approach based on transition metal-based Prussian blue(PB)and its analogues(PBAs)with core-shell nanostructure is a very promising choice for constructing cost-effective electrocatalysts for oxygen evolution reaction(OER).Herein,a bimetallic core-shell structure with open cages of Fe-doped CoP(Fe-CoP cage)has been synthesized using CoFe-PBA cage-4 as precursor through a facile hydrothermal method and following phosphating ***,there is an open hole in each face center of Fe-CoP cage,which suggests the more exposure of active sites for *** measurements show that Fe-CoP cage can afford a current density of 10 mA cm-2 at a low overpotential(300 mV),which is better than that of *** excellent performance can be attributed to Fe doping composition and unique open-cage core-shell *** synergistic effect derived from bimetallic active for OER has been *** its great catalytic stability has been evaluated via 1000 cycles of CV and chronoamperometry *** work provides a potential method to design multiple transitional metal-doping electrocatalysts with complex framework derived from PBAs for water splitting.

关键词： Core-shell structure CoFe-PBA Cation exchange Phosphating Oxygen evolution reaction