Efficient Electrochemical Hydrogen Peroxide Production from Molecular Oxygen on Nitrogen-Doped Mesoporous Carbon Catalysts

被引:450
作者
Sun, Yanyan [1 ]
Sinev, Ilya [2 ]
Ju, Wen [1 ]
Bergmann, Arno [1 ]
Dresp, Soeren [1 ]
Kuehl, Stefanie [1 ]
Spoeri, Camillo [1 ]
Schmies, Henrike [1 ]
Wang, Huan [1 ]
Bernsmeier, Denis [1 ]
Paul, Benjamin [1 ]
Schmack, Roman [1 ]
Kraehnert, Ralph [1 ]
Roldan Cuenya, Beatriz [2 ,3 ]
Strasser, Peter [1 ]
机构
[1] Tech Univ Berlin, Chem Engn Div, Dept Chem, D-10623 Berlin, Germany
[2] Ruhr Univ Bochum, Dept Phys, D-44780 Bochum, Germany
[3] Max Planck Gesell, Fritz Haber Inst, Dept Interface Sci, D-14195 Berlin, Germany
来源
ACS CATALYSIS | 2018年 / 8卷 / 04期
关键词
nitrogen-doped carbon; two-electron oxygen reduction; hydrogen peroxide production; selectivity; electrocatalysis; REDUCTION REACTION; POROUS CARBONS; SITE ISOLATION; H2O2; OXIDATION; SELECTIVITY; ELECTROCATALYSTS; ELECTROSYNTHESIS; INTERCALATION; MECHANISMS;
D O I
10.1021/acscatal.7b03464
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 (H2O2) production by two-electron oxygen reduction is a promising alternative process to the established industrial anthraquinone process. Current challenges relate to finding cost-effective electrocatalysts with high electrocatalytic activity, stability, and product selectivity. Here, we explore the electrocatalytic activity and selectivity toward H2O2 production of a number of distinct nitrogen-doped mesoporous carbon catalysts and report a previously unachieved H2O2 selectivity of similar to 95-98% in acidic solution. To explain our observations, we correlate their structural, compositional, and other physicochemical properties with their electrocatalytic performance and uncover a close correlation between the H2O2 product yield and the surface area and interfacial zeta potential. Nitrogen doping was found to sharply boost H2O2 activity and selectivity. Chronoamperometric H2O2 electrolysis confirms the exceptionally high H2O2 production rate and large H2O2 faradaic selectivity for the optimal nitrogen-doped CMK-3 sample in acidic, neutral, and alkaline solutions. In alkaline solution, the catalytic H2O2 yield increases further, where the production rate of the HO2- anion reaches a value as high as 561.7 mmol g(catalyst)(-1) h(-1) with H2O2 faradaic selectivity above 70%. Our work provides a guide for the design, synthesis, and mechanistic investigation of advanced carbon-based electrocatalysts for H2O2 production.
引用
收藏
页码:2844 / 2856
页数:25
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