In-Plane Carbon Lattice-Defect Regulating Electrochemical Oxygen Reduction to Hydrogen Peroxide Production over Nitrogen-Doped Graphene

被引:266
作者
Han, Lei [1 ]
Sun, Yanyan [2 ]
Li, Shuang [2 ]
Cheng, Chong [1 ]
Halbig, Christian E. [1 ]
Feicht, Patrick [1 ]
Huebner, Jessica Liane [2 ]
Strasser, Peter [2 ]
Eigler, Siegfried [1 ]
机构
[1] Free Univ Berlin, Inst Chem & Biochem, Takustr 3, D-14105 Berlin, Germany
[2] Tech Univ Berlin, Dept Chem, Div Chem Engn, D-10623 Berlin, Germany
来源
ACS CATALYSIS | 2019年 / 9卷 / 02期
关键词
carbon lattice-defect; oxygen reduction; hydrogen peroxide; nitrogen-doped graphene; electrocatalysis; selectivity; ELECTROCATALYTIC SYNTHESIS; FUNCTIONALIZED GRAPHENE; ELECTRODES; NANOPARTICLES; CATALYST; IDENTIFICATION; SELECTIVITY; SITES; OXIDE;
D O I
10.1021/acscatal.8b03734
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
Carbon-based materials are considered to be active for electrochemical oxygen reduction reaction (ORR) to hydrogen peroxide (H2O2) production. Nevertheless, less attention is paid to the investigation of the influence of in-plane carbon lattice defect on the catalytic activity and selectivity toward ORR. In the present work, graphene precursors were prepared from oxo-functionalized graphene (oxo-G) and graphene oxide (GO) with H2O2 hydrothermal treatment, respectively. Statistical Raman spectroscopy (SRS) analysis demonstrated the increased in-plane carbon lattice defect density in the order of oxo-G, oxo-G/H2O2, GO, GO/H2O2. Furthermore, nitrogen-doped graphene materials were prepared through ammonium hydroxide hydrothermal treatment of those graphene precursors. Rotating ring-disk electrode (RRDE) results indicate that the nitrogen-doped graphene derived from oxo-G with lowest in-plane carbon lattice defects exhibited the highest H2O2 selectivity of >82% in 0.1 M KOH. Moreover, a high H2O2 production rate of 224.8 mmol g(catalyst)(-1) h(-1) could be achieved at 0.2 VRHE in H-cell with faradaic efficiency of >43.6%. Our work provides insights for the design and synthesis of carbon-based electrocatalysts for H2O2 production.
引用
收藏
页码:1283 / 1288
页数:11
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