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论文类型： 期刊论文

发表时间： 2018-07-01

发表刊物： ACS SUSTAINABLE CHEMISTRY & ENGINEERING

收录刊物： SCIE

卷号： 6

期号： 7

页面范围： 8437-8446

ISSN号： 2168-0485

关键字： N-doped graphene aerogel; platinum nanocluster; ammonia electrolysis cell; hydrogen production

摘要： Ammonia oxidation reaction (AOR) is an environmentally friendly electrochemical technology for hydrogen production. Nowadays, exploiting low-costing, high-performance and robust catalysts for AOR is essential to improve the overall efficiency of ammonia electrolysis cell (AEC). Here, we report the synthesis and characterization of a novel free-standing three-dimensional (3D) porous N-doped graphene aerogel (NGA) anchored with Pt nanocluster (Pt/NGA) monolithic material as a high-performance and robust electrocatalyst for hydrogen production from AEC. The NGA substrate was facilely fabricated through a self -assemble process into the randomly arranged 3D porous backbone structure with graphene oxide (GO) and poly(oxypropylene)-diamine D400 as precursors in a pure water solvent. Then, the uniformly dispersed and embedded onto NGA through the simple electrodeposition method. The as-prepared Pt/NGA monolithic materials exhibited a higher ammonia electro-oxidation activity with the mass activity of 1.77 mA mu g(pt)(-1) and the specific activity of 0.64 mA cm(EcsA)(-2), due mainly to the uniformly dispersed Pt nanocluster-like morphology, the improved electrical conductivity, the 3D porous NGA networks as well as the N-doping structure in graphene framework. When the 3D Pt/NGA monolith was directly used as working electrodes of AEC, a considerable hydrogen volume of 8.5 mL (about 1.90 mL mg(pt)(-1)) was produced at 0.8 V in 3 h. This novel free-standing 3D porous NGA monolith is expected to be a potential and promising material for application in the fields of electrocatalysis and electrochemical energy transform.