Enhancing the activity and tuning the mechanism of formic acid oxidation at tetrahexahedral Pt nanocrystals by Au decoration

被引:36
作者
Liu, Hai-Xia [1 ]
Tian, Na [1 ]
Brandon, Michael P. [2 ]
Pei, Jun [1 ]
Huangfu, Zhi-Chao [1 ]
Zhan, Chi [1 ]
Zhou, Zhi-You [1 ]
Hardacre, Christopher [2 ]
Lin, Wen-Feng [2 ]
Sun, Shi-Gang [1 ]
机构
[1] Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Dept Chem, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China
[2] Queens Univ Belfast, Ctr Theory & Applicat Catalysis CenTACat, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland
基金
英国工程与自然科学研究理事会;
关键词
SINGLE-CRYSTAL ELECTRODES; FUEL-CELLS; ELECTROCATALYTIC ACTIVITY; HCOOH OXIDATION; NANOPARTICLE CATALYSTS; PLATINUM NANOPARTICLES; ETHYLENE-GLYCOL; ELECTROOXIDATION; SURFACES; METHANOL;
D O I
10.1039/c2cp42930f
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Tetrahexahedral Pt nanocrystals (THH Pt NCs), bound by high index facets, belong to an emerging class of nanomaterials that promise to bridge the gap between model and practical electrocatalysts. The atomically stepped surfaces of THH Pt NCs are extremely active for the electrooxidation of small organic molecules but they also readily accommodate the dissociative chemisorption of such species, resulting in poisoning by strongly adsorbed CO. Formic acid oxidation is an ideal reaction for studying the balance between these competing catalyst characteristics, since it can proceed by either a direct or a CO mediated pathway. Herein, we describe electrochemical and in situ FTIR spectroscopic investigations of formic acid electrooxidation at both clean and Au adatom decorated THH Pt NC surfaces. The Au decoration leads to higher catalytic currents and enhanced CO2 production in the low potential range. As the CO oxidation behaviour of the catalyst is not improved by the presence of the Au, it is likely that the role of the Au is to promote the direct pathway. Beyond their fundamental importance, these results are significant in the development of stable, poison resistant anodic electrocatalysts for direct formic acid fuel cells.
引用
收藏
页码:16415 / 16423
页数:9
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