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High-entropy alloy nanoparticles as a promising electrocatalyst to enhance activity and durability for oxygen reduction

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Nano Research 2022年第9期15卷 7868-7876页

作者： Yanan Yu Fanjie Xia Chengjie Wang Jinsong Wu Xianbiao Fu Dongsheng Ma Bencai Lin Jiaao Wang Qin Yue Yijin Kang Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Nanostructure Research CenterWuhan University of TechnologyWuhan 430070China Jiangsu Province Cultivation base for State Key Laboratory of Photovoltaic Science and Technology Changzhou UniversityChangzhou 213164China Department of Chemistry and the Oden Institute for Computational Engineering and Sciences The University of Texas at AustinTX 78712USA

Developing efficient platinum-based electrocatalysts with super durability for the oxygen reduction reaction(ORR)is highly desirable to promote the large-scale commercialization of fuel cells.Although progress has been made in this aspect,the electrochemical kinetics and stability of platinum-based catalysts are still far from the requirements of the practical applications.Herein,PtPdFeCoNi high-entropy alloy(HEA)nanoparticles were demonstrated via a high-temperature injection method.PtPdFeCoNi HEA nanocatalyst exhibits outstanding catalytic activity and stability towards ORR due to the high entropy,lattice distortion,and sluggish diffusion effects of HEA,and the HEA nanoparticles delivered a mass activity of 1.23 A/mgPt and a specific activity of 1.80 mA/cmPt 2,which enhanced by 6.2 and 4.9 times,respectively,compared with the values of the commercial Pt/C catalyst.More importantly,the high durability of PtPdFeCoNi HEA/C was evidenced by only 6 mV negativeshifted half-wave potential after 50,000 cycles of accelerated durability test(ADT).

关键词： high-entropy alloy oxygen reduction reaction electrocatalyst high durability

Sulfurization accelerator coupled Fe_(1-x)S electrocatalyst boosting SPAN cathode performance

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Nano Research 2023年第7期16卷 9231-9239页

作者： Jinlei Qin Yun Lu Rui Wang Zhizhan Li Tao Shen Deli Wang Key Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education Hubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Sulfurized polyacrylonitrile(SPAN)cathode exhibits improved cycling stability in carbonate electrolytes due to the existent of-S_(x)^(2-)-(2≤n≤4)units.However,it is still challenging for SPAN to achieve higher sulfur content,superior conductivity,and faster polysulfide conversion kinetics in ether electrolytes.Herein,polyacrylonitrile(PAN),2-morpholinothiobenzothiazole(MBS),and FeCl_(3)coated reduced graphene oxide(rGO)were used to fabricate advanced sulfur cathode through electrospinning technology to address these problems.During PAN sulfuration reactions,the MBS with abundant unsaturated bonds served as the vulcanization accelerator to facilitate the formation of longer chain sulfur species(-S_(3)-/-S_(4)-)and increase the sulfur content in the SPAN electrode system.Meanwhile,Fe_(1-x)S is in situ converted from FeCl_(3),which acts as the electrocatalyst to promote Li_(2)S nucleation and decomposition reactions.As a result,the Fe_(1-x)S/SPAN/rGO electrode with high sulfur loading of 2.0 mg·cm^(-2)delivers a reversible capacity of 1122 mAh·g^(-1)at 0.1 A·g^(-1).Notably,at a large current density of 5.0 A·g^(-1),the Fe_(1-x)S/SPAN/rGO electrode still displays a high specific capacity of 924 mAh·g^(-1)with an ultra-stable cycling life over 2000 cycles.The present work provides new insights into designing of high-performance electrode materials for long-lasting Li-S batteries.

关键词： Li-S batteries electrocatalyst electrospun sulfurized polyacrylonitrile(SPAN) vulcanization accelerators

Millisecond-timescale electrodeposition of platinum atom-doped molybdenum oxide as an efficient electrocatalyst for hydrogen evolution reaction

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Frontiers of Materials Science 2022年第3期16卷 171-180页

作者： Yi XIAO Wenxue SHANG Jiyuan FENG Airu YU Lu CHEN Liqiu ZHANG Hongxia SHEN Qiong CHENG Lichun LIU Song BAI College of Chemistry and Life Sciences Zhejiang Normal UniversityJinhua 321000China College of Biological Chemical Sciences and Engineering&Nanotechnology Research InstituteJiaxing UniversityJiaxing 314000China College of Petroleum Engineering Liaoning Petrochemical UniversityFushun 113000China Collegeof Chemistry Jilin Normal UniversityChangchun 130103China

We present a straightforward method for one-pot electrodeposition of platinum atoms-doped molybdenum oxide(Pt·MoO_(3-x))films and show their superior electrocatalytic activity in the hydrogen evolution reaction(HER).A~15-nm-thick Pt·MoO_(3-x) film was prepared by one-pot electrodeposition at-0.8 V for 1 ms.Due to considerably different solute concentrations,the content of Pt atoms in the electrode-posited composite electrocatalyst is low.No Pt crystals or islands were observed on the flat Pt-MoO_(3-x) films,indicating that Pt atoms were homogeneously dispersed within the MoO_(3-x) thin film.The catalytic performance and physicochemical features of Pt·MoO_(3-x) as a HER electrocatalyst were characterized.The results showed that our Pt·MoO_(3-x) film exhibits 23-and 11-times higher current density than Pt and MoO_(3-x) electrodeposited individually under the same conditions,respectively.It was found that the dramatic enhancement in the HER performance was principally due to the abundant oxygen defects.The use of the developed one-pot electrodeposition and doping method can potentially be extended to various catalytically active metal oxides or hydroxides for enhanced performance in various energy storage and conversion applications.

关键词： platinum molybdenum oxide electrodeposition hydrogen evolution reaction doping electrocatalyst

Facile synthesis of defect-rich Fe-N-C hybrid from fullerene/ferrotetraphenylporphyrin as efficient oxygen reduction electrocatalyst for Zn-air battery

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Chinese Chemical Letters 2023年第5期34卷 616-620页

作者： Hai Wang Liyun Cao Yongqiang Feng Junsheng Chen Weihang Feng Tianmi Luo Yuzhu Hu Chengke Yuan Yajuan Zhao Yong Zhao Koji Kajiyoshi Yijun Liu Zhenjiang Li Jianfeng Huang School of Material Science and Engineering International S&T Cooperation Foundation of Shaanxi ProvinceShaanxi University of Science and TechnologyXi'an 710021China Kochi University Research Laboratory of Hydrothermal ChemistryKochi 780-8520Japan Guangdong Mona Lisa Group Co. Ltd.Foshan 528211China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China

Exploring remarkable oxygen reduction reaction(ORR)electrocatalysts for regenerative fuel cells and metal-air batteries is highly essential.Herein,a novel non-noble metal-based heterogeneous electrocatalyst with rich defects were successfully synthesized by liquid-liquid interfacial precipitation(LLIP)of fullerene(C_(60))and ferrotetraphenylporphyrin(FeTPP)followed by one step pyrolysis.The obtained product annealed at 700℃(C_(60)/FeTPP-700),when employed as ORR electrocatalyst,revealed a positive halfwave potential(E_(1/2))of 0.877 V vs.reversible hydrogen electrode(RHE),which was superior to that of the commercial 25%Pt/C.Delightfully,the assembled Zn-air battery(ZAB)using C_(60)/FeTPP-700 as an air-electrode catalyst exhibited a high power density of 153 m W/cm^(2),specific capacity of 668 mAh/g and long-term cycling stability for more than 250 h.Experimental results proved that the excellent electrocatalytic ORR activity of C_(60)/FeTPP-700 would attribute to the synergistic effect between FeN_xsites,Fe_(3)C/Fe nanoparticles and the structure defects.This work provides a feasible and simple method to prepare nonnoble metal-based ORR electrocatalysts for the application of energy storage and conversion.

关键词： Oxygen reduction reaction electrocatalyst Fullerene Defect Zn-air battery

Flower-like NiCo_(2)S_(4)/NiFeP/NF composite material as an effective electrocatalyst with high overall water splitting performance

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Chinese Chemical Letters 2022年第9期33卷 4367-4374页

作者： Jing Jiang Fengyan Li Hui Su Yangqin Gao Ning Li Lei Ge State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of Petroleum BeijingBeijing 102249China Department of Materials Science and Engineering College of New Energy and MaterialsChina University of Petroleum BeijingBeijing 102249China

Rational design and building of high efficiency,secure and inexpensive electrocatalyst is a pressing demand and performance to promote sustainable improvement of hydrogen energy.The bifunctional electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution response(HER)with high catalytic performance and steadiness in the equal electrolyte are extra treasured and meaningful.Herein,a unique three-dimensional(3D)structure electrocatalyst for NiCo_(2)S_(4)growing on the flower-like NiFeP was designed and synthesized in this study.The results show that the flower-like NiCo_(2)S_(4)/NiFeP/NF composite electrocatalyst has large specific surface area,appropriate electrical conductivity,and greater lively websites uncovered in the three-dimensional structure,and affords extraordinary electrocatalytic overall performance for the ordinary water splitting.In alkaline solution,the OER and HER overpotentials of NiCo_(2)S_(4)/NiFeP/NF only need 293 mV and 205 mV overpotential to provide the current densities of 100 mA/cm^(2)and 50 mA/cm^(2),respectively.This high electrocatalytic activity exceeds the catalytic activity of most nickel-iron based electrocatalysts for OER and HER process.Accordingly,the optimized NiCo_(2)S_(4)/NiFeP/NF sample has higher stability(24 h)at 1.560 and 10 mA/cm^(2),which extensively speeds up the overall water splitting process.In view of the above performance,this work offers a fine approach for the further improvement of low fee and excessive effectivity electrocatalyst.

关键词： NiCo_(2)S_(4) electrocatalyst NiFeP Hydrogen evolution reaction Water splitting

Phase-mediated cobalt phosphide with unique core-shell architecture serving as efficient and bifunctional electrocatalyst for hydrogen evolution and oxygen reduction reaction

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Chinese Chemical Letters 2022年第8期33卷 3752-3756页

作者： Junsheng Chen Jianfeng Huang Hai Wang Weihang Feng Tianmi Luo Yuzhu Hu Chengke Yuan Liyun Cao Yanni Jie Koji Kajiyoshi Yongqiang Feng School of Material Science and Engineering International S&T Cooperation Foundation of Shaanxi ProvinceXi'an Key Laboratory of Green Manufacture of Ceramic MaterialsShaanxi University of Science and TechnologyXi'an 710021China Kochi University Research Laboratory of Hydrothermal ChemistryKochi 780-8520Japan

Hydrogen evolution reaction(HER)and oxygen reduction reaction(ORR)have been considered as two critical processes in the field of electrocatalytic water-splitting for hydrogen production and fuel cells.However,the sluggish reaction kinetics of HER and ORR required efficient electrocatalyst such as Pt to promote such process.Transition metal phosphides(TMPs)exhibit great potential to replace noble metal electrocatalysts to accelerate HER and ORR due to their high activity and easy availability.Herein,a highly-efficient bifunctional CoP electrocatalyst for HER and ORR,featuring a unique core-shell structure decorated on nitrogen-doped carbon matrix was designed and constructed via etching a cobalt-based zeolitic imidazolate framework(ZIF-67)with phytic acid(PA)followed by pyrolysis treatment(PA-ZIF-67-900).Experimental results revealed that the pure-phase single-crystalline Co P exhibited outstanding electrocatalytic performance in HER and ORR,superior to Co(PO_(3))_(2) in PA-ZIF-67-700,hybrid phase of Co(PO_(3))_(2) and CoP in PA-ZIF-67-800 and Co_(2)P-doped CoP in PA-ZIF-67-1000.To reach the current density of 10 mA/cm^(2)the as-synthesized Co P required an overpotential of 120 m V for HER in 1 mol/L KOH and half-wave potential of 0.85 V in O_(2)-saturated 0.1 mol/L KOH.This work present new clue for construction of efficient and bifunctional electrocatalyst in the field of energy conversion and storage.

关键词： electrocatalyst Hydrogen evolution reaction Oxygen reduction reaction Transitional metal phosphide CoP

CoFe-LDH nanowire arrays on graphite felt: A high-performance oxygen evolution electrocatalyst in alkaline media

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Chinese Chemical Letters 2022年第2期33卷 890-892页

作者： Biao Deng Jie Liang Luchao Yue Tingshuai Li Qian Liu Yang Liu Shuyan Gao Abdulmohsen Ali Alshehri Khalid Ahmed Alzahrani Yonglan Luo Xuping Sun Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province School of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong 637002China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Institute for Advanced Study Chengdu UniversityChengdu 610106China School of Materials Science and Engineering Henan Normal UniversityXinxiang 453007China Chemistry Department Faculty of ScienceKing Abdulaziz UniversityP.O.Box 80203Jeddah 21589Saudi Arabia

Developing non-noble-metal oxygen evolution reaction(OER) electrocatalysts with high performance is critical to electrocatalytic water splitting. In this work, we fabricated Co Fe-layered double hydroxide(LDH) nanowire arrays on graphite felt(Co Fe-LDH/GF) via a hydrothermal method. The Co Fe-LDH/GF, as a robust integrated 3 D OER anode, exhibits excellent catalytic activity with the need of low overpotential of 252 and 285 mV to drive current densities of 10 and 100 mA/cm^(2) in 1.0 mol/L KOH, respectively. In addition, it also maintains electrochemical durability for at least 24 h. This work would open up avenues for the development of GF like attractive catalyst supports for oxygen evolution applications.

关键词： LDH Graphite felt electrocatalyst Oxygen evolution Alkaline media

A highly efficient atomically thin curved Pd Ir bimetallene electrocatalyst

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National Science Review 2021年第9期8卷 100-110页

作者： Fan Lv Bolong Huang Jianrui Feng Weiyu Zhang Kai Wang Na Li Jinhui Zhou Peng Zhou Wenxiu Yang Yaping Du Dong Su Shaojun Guo School of Materials Science and Engineering Peking University Department of Applied Biology and Chemical Technology Hong Kong Polytechnic University Frontier Institute of Science and Technology jointly with College of Science Xi'an Jiaotong University Center for Functional Nanomaterials Brookhaven National Laboratory School of Materials Science and Engineering & National Institute for Advanced Materials Nankai University College of Engineering Peking University

The multi-metallene with an ultrahigh surface area has great potential in precise tuning of surface heterogeneous d-electronic correlation by surface strain effect for the distinctive surface electronic structure, which is a brand new class of promising 2 D electrocatalyst for sustainable energy device application. However, achieving such an atomically thin multi-metallene still presents a great challenge.Herein, we present a new synthetic method for an atomic-level palladium-iridium(Pd Ir) bimetallene with an average thickness of only～1.0 nm for achieving superior catalysis in the hydrogen evolution reaction(HER) and the formic acid oxidation reaction(FAOR). The curved Pd Ir bimetallene presents a top-ranked high electrochemical active area of 127.5 ± 10.8 m~2 g Pd+Ir-1in the reported noble alloy materials, and exhibits a very low overpotential, ultrahigh activity and improved stability for HER and FAOR. DFT calculation reveals that the Pd Ir bimetallene herein has a unique lattice tangential strain, which can induce surface distortion while concurrently creating a variety of concave-convex featured micro-active regions formed by variously coordinated Pd sites agglomeration. Such a strong strain effect correlates the abnormal on-site active 4 d10-t2g-orbital Coulomb correlation potential and directly elevates orbital-electronegativity exposure within these active regions, resulting in a preeminent barrier-free energetic path for significant enhancement of FAOR and HER catalytic performance.

关键词： strain metallene PdIr alloy atomically thin electrocatalyst

Synthesis and application of transition metal phosphides as electrocatalyst for water splitting

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Science Bulletin 2017年第9期62卷 633-644页

作者： Jinzhan Su Jinglan Zhou Lu Wang Cong Liu Yubin Chen International Research Center for Renewable Energy (IRCRE) State Key Laboratory for Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 China

With continuous research on photocatalytic water splitting, searching for efficient catalyst for hydrogen evolution reaction(HER) becomes popular topic in addition to main catalyst research. Transition metal phosphides are receiving intense attention due to its abundance in the Earth's crust and comparable catalytic properties to noble metals. In this review, the synthesis approaches, HER reaction mechanism,photocatalytic activity, approaches to improve the activity of transition metal phosphides were reviewed and discussed. It was showed that the transition metal phosphides have great potential to reduce the cost of photocatalyst and promising application on water splitting. The stability problem and participation of poisonous reactant and product in its synthesis reaction limit its application and developing in a certain extent, but with the continuous efforts on the development and improvement of the synthesis methods,transition metal phosphides will find wide application in water splitting.

关键词： Transition metal phosphide electrocatalyst HER Photocatalytic water splitting