Oxygen and nitrogen co-doped ordered mesoporous carbon materials enhanced the electrochemical selectivity of O2 reduction to H2O2

被引:50
|
作者
Qin, Meichun [1 ]
Fan, Shiying [1 ]
Wang, Liang [1 ]
Gan, Guoqiang [1 ]
Wang, Xinyang [1 ]
Cheng, Jie [3 ]
Hao, Zhengping [3 ]
Li, Xinyong [1 ,2 ]
机构
[1] Dalian Univ Technol, Sch Environm Sci & Technol, State Key Lab Fine Chem, Key Lab Ind Ecol & Environm Engn MOE, Dalian 116024, Peoples R China
[2] Curtin Univ, Dept Chem Engn, GPO Box U1987, Perth, WA 6845, Australia
[3] Univ Chinese Acad Sci, Natl Engn Lab VOCs Pollut Control Mat & Technol, Beijing 101408, Peoples R China
基金
中国国家自然科学基金;
关键词
N/O co-doped; Ordered mesoporous carbon; Two-electron ORR; Electrocatalyst; Adsorption energy; HIGH ELECTROCATALYTIC ACTIVITY; HYDROGEN-PEROXIDE; ACTIVE-SITES; CATALYSTS; RESORCINOL; ARRAYS; PH;
D O I
10.1016/j.jcis.2019.11.080
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
Electrochemical hydrogen peroxide production from two-electron oxygen reduction reaction, a cost-effective, sustainable and reliable method compared with the traditional anthraquinone process, is attracting growing attention. However, it is challenged by the selectivity of electrocatalysts. In this context, nitrogen and oxygen co-doped ordered mesoporous carbon materials have been successfully fabricated. Benefiting from the ordered pore structure, better dispersion behavior and valid doping effect, a high selectivity (similar to 95.00%), good activity and stability toward H2O2 production were achieved. Systematic characterizations like physical adsorption, zeta potential, X-ray photoelectron spectroscopy and density functional theory (DFT) calculation revealed that interactive effects between pyridinic N and functional groups of COOH/C-O-C largely facilitated the desorption of intermediates (*OOH, * represents an unoccupied active site) in turn enhance the selectivity of electrocatalysts toward H2O2 production. Interestingly, H2O2 produced in situ was applied to Electro-Fenton, the formaldehyde mineralization rate was high to about 88.06%. These findings offer a rational chemical design of electrocatalysts toward H2O2 production and pollutant purification. (C) 2019 Elsevier Inc. All rights reserved.
引用
收藏
页码:540 / 549
页数:10
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