Direct integration of ultralow-platinum alloy into nanocarbon architectures for efficient oxygen reduction in fuel cells  

超低铂合金与纳米碳结构直接集成的高效氧还原催化剂的设计

作　　者：Shahid Zaman Xinlong Tian Ya-Qiong Su Weiwei Cai Ya Yan Ruijuan Qi Abdoulkader Ibro Douka Shenghua Chen Bo You Hongfang Liu Shujiang Ding Xingpeng Guo Bao Yu Xia Shahid Zaman;田新龙;苏亚琼;蔡卫卫;严雅;齐瑞娟;Abdoulkader Ibro Douka;陈圣华;游波;刘宏芳;丁书江;郭兴蓬;夏宝玉(School of Chemistry and Chemical Engineering,Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education),Hubei Key Laboratory of Material Chemistry and Service Failure,Hubei Engineering Research Center for Biomaterials and Medical Protective Materials,Wuhan National Laboratory for Optoelectronics,Huazhong University of Science and Technology(HUST),Wuhan 430074,China;School of Chemistry,Xi'an Key Laboratory of Sustainable Energy Materials Chemistry,Ministry of Education Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter,State Key Laboratory of Electrical Insulation and Power Equipment,Xi'an Jiaotong University,Xi'an 710049,China;Sustainable Energy Laboratory,Faculty of Material Science and Chemistry,China University of Geosciences,Wuhan 430074,China;School of Materials Science and Engineering,University of Shanghai for Science and Technology,Shanghai 200093,China;Department of Information Science and Technology,East China Normal University,Shanghai 200240,China)

机构地区：[1]School of Chemistry and Chemical Engineering,Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education),Hubei Key Laboratory of Material Chemistry and Service Failure,Hubei Engineering Research Center for Biomaterials and Medical Protective Materials,Wuhan National Laboratory for Optoelectronics,Huazhong University of Science and Technology(HUST),Wuhan 430074,China [2]School of Chemistry,Xi'an Key Laboratory of Sustainable Energy Materials Chemistry,Ministry of Education Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter,State Key Laboratory of Electrical Insulation and Power Equipment,Xi'an Jiaotong University,Xi'an 710049,China [3]Sustainable Energy Laboratory,Faculty of Material Science and Chemistry,China University of Geosciences,Wuhan 430074,China [4]School of Materials Science and Engineering,University of Shanghai for Science and Technology,Shanghai 200093,China [5]Department of Information Science and Technology,East China Normal University,Shanghai 200240,China

出　　处：《Science Bulletin》2021年第21期2207-2216,M0004,共11页科学通报（英文版）

基　　金：the National Natural Science Foundation of China(22075092 and 21805104);the Program for Huazhong University of Science and Technology(HUST)Academic Frontier Youth Team(2018QYTD15);The Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。

摘　　要：Developing efficient platinum(Pt)-based electrocatalysts is enormously significant for fuel cells.Herein,we report an integrated electrocatalyst of ultralow-Pt alloy encapsulated into nitrogen-doped nanocarbon architecture for efficient oxygen reduction reaction.This hybrid Pt-based catalyst achieves a mass activity of 3.46 A mg^(-1)_(pt)the potential of 0.9 V vs.RHE with a negligible stability decay after 10,000 cycles.More importantly,this half-cell activity can be expressed at full cell level with a high Pt utilization of 10.22 W mg^(-1)_(Pt cathode)and remarkable durability after 30,000 cycles in single-cell.Experimental and theoretical investigations reveal that a highly strained Pt structure with an optimal Pt-0 binding energy is induced by the incorporation of Co/Ni into Pt lattice,which would account for the improved reaction kinetics.The synergistic catalysis due to nitrogen-doped nanocarbon architecture and active Pt component is responsible for the enhanced catalytic activity.Meanwhile,the strong metal-support interaction and optimized hydrophilic properties of nanocarbon matrix facilitate efficient mass transport and water management.This work may provide significant insights in designing the low-Pt integrated electrocatalysts for fuel cells and beyond.开发高效的铂(Pt)基电催化剂对于燃料电池的发展具有极其重要的意义.本文报道了一种氮掺杂纳米碳结构包覆的超低Pt合金集成电催化剂并用于燃料电池氧还原反应.该Pt基催化剂复合材料在0.9 V vs.RHE的电位下展现出3.46 A mg^(-1)_(Pt)质量活性,并且在10000圈循环后几乎没有衰减.单电池测试结果表明,其Pt利用率高达10.22 W mg^(-1)_(Pt)阴极,并具有30000圈循环的优异耐久性.实验和理论研究表明,将Co/Ni掺入Pt晶格可产生具有最佳Pt-O结合能的高应变Pt结构,这可显著加快反应动力学.氮掺杂纳米碳结构和活性Pt组分产生的协同催化作用是提高催化活性的主要原因,同时增强的金属-载体相互作用和优化的亲水性能可促进传质过程和水管理.这项工作可为燃料电池及其他领域的低Pt集成电催化剂的设计提供重要见解.

关 键 词：Fuel cells Oxygen reduction reaction ELECTROCATALYST Low-platinum alloy NANOCARBON 

分 类 号：O643.36[理学—物理化学] TM911.4[理学—化学]