Intrinsic Relationship between Enhanced Oxygen Reduction Reaction Activity and Nanoscale Work Function of Doped Carbons

被引:382
作者
Cheon, Jae Yeong [1 ]
Kim, Jong Hun [3 ,4 ]
Kim, Jae Hyung [2 ]
Goddeti, Kalyan C. [3 ,4 ]
Park, Jeong Young [3 ,4 ]
Joo, Sang Hoon [1 ,2 ]
机构
[1] Ulsan Natl Inst Sci & Technol, Dept Chem, Ulsan 689798, South Korea
[2] Ulsan Natl Inst Sci & Technol, Sch Energy & Chem Engn, Ulsan 689798, South Korea
[3] Inst for Basic Sci Korea, Ctr Nanomat & Chem React, Taejon 305701, South Korea
[4] Korea Adv Inst Sci & Technol, Grad Sch EEWS, Taejon 305701, South Korea
基金
新加坡国家研究基金会;
关键词
METAL-FREE ELECTROCATALYSTS; GRAPHENE NANOPLATELETS; CATALYSTS; BORON; POLYANILINE; NANOTUBES; SULFUR; ARRAYS; OXIDE; IRON;
D O I
10.1021/ja503557x
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Nanostructured carbon materials doped with a variety of heteroatoms have shown promising electrocatalytic activity in the oxygen reduction reaction (ORR). However, understanding of the working principles that underpin the superior ORR activity observed with doped nanocarbons is still limited to predictions based on theoretical calculations. Herein, we demonstrate, for the first time, that the enhanced ORR activity in doped nanocarbons can be correlated with the variation in their nanoscale work function. A series of doped ordered mesoporous carbons (OMCs) were prepared using N, S, and O as dopants; the triple-doped, N,S,O-OMC displayed superior ORR activity and four-electron selectivity compared to the dual-doped (N,O-OMC and S,O-OMC) and the monodoped (O-OMC) OMCs. Significantly, the work functions of these heteroatom-doped OMCs, measured by Kelvin probe force microscopy, display a strong correlation with the activity and reaction kinetics for the ORR This unprecedented experimental insight can be used to provide an explanation for the enhanced ORR activity of heteroatom-doped carbon materials.
引用
收藏
页码:8875 / 8878
页数:4
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