期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 36, 页码 11232-11240出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b03080
关键词
-
资金
- National Basic Research Program of China [2015CB932301]
- National Key Research and Development Program of China [2017YFA0206500, 2017YFA0206801]
- National Natural Science Foundation of China [21333008, 21603178, 21671163, 21721001, 21773190]
- China Postdoctoral Science Foundation [2016M602066, 2017T100468]
Developing active and durable electro-catalysts toward ethanol oxidation reaction (EOR) with high selectivity toward the C-C bond cleavage is an important issue for the commercialization of direct ethanol fuel cell. Unfortunately, current ethanol oxidation electro-catalysts (e.g., Pt, Pd) still suffer from poor selectivity for direct oxidation of ethanol to CO2, and rapid activity degradation. Here we report a facile route to the synthesis of a new kind of cyclic penta-twinned (CPT) Rh nanostructures that are self-supported nanobranches (NBs) built with 1-dimension CPT nanorods as subunits. Structurally, the as-prepared Rh NBs possess high percentage of open {100} facets with significant CPT-induced lattice strains. With these unique structural characteristics, the as-prepared CPT Rh NBs exhibit outstanding electrocatalytic performance toward EOR in alkaline solution. Most strikingly, the selectivity of complete conversion ethanol to CO, on the CPT Rh NBs is measured to be as high as 14.5 +/- 1.1% at -0.15 V, far exceeding that for single crystal tetrahedral nanocrystals, icosahedral nanocrystals, and commercial Rh black, as well as majority of reported values for Pt or Pd-based electro-catalysts. By combining with density functional theory calculation, the effects of different structural features of Rh on EOR are definitively elucidated. It was found that the large amount of open Rh (100) facets dominantly contribute to the outstanding activity and exceptionally high selectivity, while the additional tensile strain on (100) planes can further boost the catalytic activity by enhancing the adsorption strength and lowering the reaction barrier of dehydrogenation process of ethanol. As a proof of concept, the present work shows that rationally optimizing surface and electronic structure of electrocatalysts by simultaneously engineering their surface and bulk structures is a promising strategy to promote the performance of electro-catalysts.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据