Intermediate Modulation on Noble Metal Hybridized to 2D Metal-Organic Framework for Accelerated Water Electrocatalysis

被引:199
作者
Guo, Chunxian [1 ]
Jiao, Yan [1 ]
Zheng, Yao [1 ]
Luo, Jun [2 ]
Davey, Kenneth [1 ]
Qiao, Shi-Zhang [1 ]
机构
[1] Univ Adelaide, Sch Chem Engn, Adelaide, SA 5005, Australia
[2] Tianjin Univ Technol, Inst New Energy Mat & Low Carbon Technol, Tianjin 300384, Peoples R China
基金
澳大利亚研究理事会;
关键词
HYDROGEN EVOLUTION ACTIVITY; OXYGEN EVOLUTION; EFFICIENT; CATALYSTS; SURFACE; NANOPARTICLES; REDUCTION; DESIGN; AMMONIA;
D O I
10.1016/j.chempr.2019.06.016
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The rational modulation of reaction intermediates is critical to achieving high-performance heterogeneous catalysis. However, practical realization remains challenging. Using water electrocatalysis as a model reaction, we report an interfacial-bond-induced intermediate modulation to accelerate the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) by hybridizing a 2D nickel metal-organic framework (MOF) and Pt nanocrystals into a heterostructure. The design is initially verified via theoretical calculations, indicating charge relocation on newly formed Ni-O-Pt interfacial bonds for increased OH* adsorption energy together with reduced H* adsorption energy. Experimental findings confirm the formation of the Ni-O-Pt bonds, which electronically modify the heterostructure to increase electron density for Pt and the high-energy Ni 3d state for the MOF, optimizing the adsorption for H* and OH*, respectively. This hybridized material delivered HER activity of 7.92 mA mu g(-1) Pt, which is among the best reported for alkaline electrocatalysts, and an improved OER activity.
引用
收藏
页码:2429 / 2441
页数:13
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