N-doped ordered mesoporous carbons prepared by a two-step nanocasting strategy as highly active and selective electrocatalysts for the reduction of O2 to H2O2

被引:122
|
作者
Sheng, Xia [1 ,2 ]
Daems, Nick [1 ]
Geboes, Bart [3 ,4 ]
Kurttepeli, Mert [5 ]
Bals, Sara [5 ]
Breugelmans, Tom [3 ,4 ]
Hubin, Annick [3 ]
Vankelecom, Ivo F. J. [1 ]
Pescarmona, Paolo P. [1 ,6 ]
机构
[1] Univ Leuven KU Leuven, Ctr Surface Chem & Catalysis, B-3001 Heverlee, Belgium
[2] Henan Univ Technol, Sch Chem & Chem Engn, Zhengzhou 450001, Peoples R China
[3] Vrije Univ Brussel, Res Grp Electrochem & Surface Engn, B-1050 Brussels, Belgium
[4] Univ Antwerp, Res Grp Adv Reactor Engn, B-2660 Hoboken, Belgium
[5] Univ Antwerp, EMAT, B-2020 Antwerp, Belgium
[6] Univ Groningen, Dept Chem Engn, NL-9747 AG Groningen, Netherlands
关键词
N-doped ordered mesoporous carbon; Two-step synthesis; Metal-free electrocatalyst; Oxygen reduction reaction; Hydrogen peroxide; NEUTRAL HYDROGEN-PEROXIDE; X-RAY-SCATTERING; OXYGEN REDUCTION; CATALYTIC SYNTHESIS; GRAPHENE; NANOTUBES; SULFUR; ALLOY; OXIDE; H-2;
D O I
10.1016/j.apcatb.2015.03.049
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
A new, two-step nanocasting method was developed to prepare N-doped ordered mesoporous carbon (NOMC) electrocatalysts for the reduction of O-2 to H2O2. Our strategy involves the sequential pyrolysis of two inexpensive and readily available N and C precursors, i.e. aniline and dihydroxynaphthalene (DHN), inside the pores of a SBA-15 hard silica template to obtain N-doped graphitic carbon materials with well-ordered pores and high surface areas (764 and 877 m(2)g(-1)). By tuning the ratio of carbon sources to silica template, it was possible to achieve an optimal filling of the pores of the SBA-15 silica and to minimise carbon species outside the pores. These NOMC materials displayed outstanding electrocatalytic activity in the oxygen reduction reaction, achieving a remarkably enhanced kinetic current density compared to state-of-the-art N-doped carbon materials (-16.7 mA cm(-2) at 0.35 V vs. Ag/AgCl in a 0.1 M KOH solution as electrolyte). The NOMC electrocatalysts showed high selectivity toward the two-electron reduction of oxygen to hydrogen peroxide and excellent long-term stability. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:212 / 224
页数:13
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