Robust Interface Ru Centers for High-Performance Acidic Oxygen Evolution

被引:215
作者
Cui, Xiaoju [1 ,2 ]
Ren, Pengju [3 ]
Ma, Chao [4 ]
Zhao, Jia [2 ]
Chen, Ruixue [1 ,2 ]
Chen, Shiming [2 ]
Rajan, N. Pethan [2 ]
Li, Haobo [2 ]
Yu, Liang [2 ]
Tian, Zhongqun [1 ]
Deng, Dehui [1 ,2 ]
机构
[1] Xiamen Univ, Collaborat Innovat Ctr Chem Energy Mat, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, Collaborat Innovat Ctr Chem Energy Mat, State Key Lab Catalysis, Dalian 116023, Peoples R China
[3] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
[4] Hunan Univ, Coll Mat Sci & Engn, Ctr High Resolut Electron Microscopy, Changsha 410082, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金; 国家重点研发计划;
关键词
acidic electrolytes; DFT calculations; electrocatalysis; interface active centers; oxygen evolution reaction; WATER OXIDATION; ELECTROCATALYSTS; CATALYST; EFFICIENT; SURFACE; DESIGN; SITES;
D O I
10.1002/adma.201908126
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
RuO2 is considered as the state-of-the-art electrocatalyst for the oxygen evolution reaction (OER) in acidic media. However, its practical application is largely hindered by both the high reaction overpotential and severe electrochemical corrosion of the active centers. To overcome these limitations, innovative design strategies are necessary, which remains a great challenge. Herein, robust interface Ru centers between RuO2 and graphene, via a controllable oxidation of graphene encapsulating Ru nanoparticles, are presented to efficiently enhance both the activity and stability of the acidic OER. Through precisely controlling the reaction interface, a much lower OER overpotential of only 227 mV at 10 mA cm(-2) in acidic electrolyte, compared with that of 290 mV for commercial RuO2, but a significantly higher durability than the commercial RuO2, are achieved. Density functional theory (DFT) calculations reveal that the interface Ru centers between the RuO2 and the graphene can break the classic scaling relationships between the free energies of HOO* and HO* to reduce the limiting potential, rendering an enhancement in the intrinsic OER activity and the resistance to over-oxidation and corrosion for RuO2.
引用
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页数:7
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