期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 38, 页码 34854-34861出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b09315
关键词
metal free electrocatalyst; amino-rich carbon framework; operando technique; Fourier-transform infrared spectroscopy; oxygen evolution reaction
资金
- National Key Research and Development Programme of China [2017YFA0402800]
- National Natural Science Foundation of China [11875257, 21603207, U1532265, 11621063, 21533007]
- Fundamental Research Funds for the Central Universities [WK2310000070]
Operando insight into the catalytic kinetics under working conditions is important for further rationalizing the design of advanced catalysts toward efficient renewable energy applications. Here, we enable a ubiquitous carbon material as an efficient acidic oxygen evolution reaction (OER) electrocatalyst, synthesized via a facile and controllable amino-assisted polymerization and carbonization strategy. This as-developed metal-free amino-rich hierarchical-network carbon (amino-HNC) framework directly supported on carbon paper can catalyze OER at a quite low overpotential of 281 mV and a small Tafel slope of 96 mV dec(-1) in an acid solution, and maintain similar to 98% of its initial catalytic activity after 100 h oxygen evolution operation. By using the operando synchrotron infrared spectroscopy, a crucial structurally evolved H2N-(*O-C)-C, formed by adsorbing the *O intermediate on the active H2N-C=C moiety, is observed on amino-HNC electrocatalysts during the OER process in the acid medium. Furthermore, theoretical calculations reveal that the optimization of the sp(2) electronic structure of C=C by amino radicals could effectively lower the kinetic formation barrier of the *O intermediate on the H2N-C=C moiety, contributing to a prominent acidic oxygen-involved catalysis.
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