Carbon Dioxide Electroreduction at Highly Porous Nitrogen and Sulfur Co-Doped Iron-Containing Heterogeneous Carbon Gel

被引:18
作者
Dembinska, Beata [1 ]
Kicinski, Wojciech [2 ]
Januszewska, Aneta [1 ]
Dobrzeniecka, Anna [1 ]
Kulesza, Pawel J. [1 ]
机构
[1] Univ Warsaw, Fac Chem, PL-02093 Warsaw, Poland
[2] Mil Univ Technol, Inst Chem, PL-00908 Warsaw, Poland
关键词
ELECTROCHEMICAL REDUCTION; OXYGEN REDUCTION; ELECTROCATALYTIC ACTIVITY; CATALYSTS; HYDROCARBONS; OXIDATION; ELECTRODE; POLYANILINE; COMPLEXES; PALLADIUM;
D O I
10.1149/2.0721707jes
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
The functionalized carbon nanostructure, nitrogen and sulfur co-doped iron-containing highly porous carbon gel (obtained via carbonization of corresponding organic gel) is considered here as a non-precious metal catalyst for the electroreduction of carbon dioxide in neutral solution (potassium bicarbonate at pH = 6.8). Various electrochemical measurements (performed in distinct modes and under different conditions) have been utilized to comment about the catalyst performance and the reactionmechanism, in particular about the reaction products and the relative contribution from hydrogen evolution. At low overpotentials, the carbon dioxide reduction is favored over the hydrogen evolution reaction. Combination of conventional (stationary) stripping-type and hydrodynamic (rotating ring-disk electrode) voltammetric approaches has been demonstrated to function as an unique electroanalytical tool here. The CO2-reduction products can be identified as adsorbates (oxidative stripping voltammetry) or monitored continuously (electrooxidation) at the Pt ring electrode. Finally, the results of both electrochemical diagnostic and parallel gas chromatographic analytical measurements are consistent with the view that, in the examined range of the potentials, CO is the main CO2-reduction product. (C) The Author(s) 2017. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY-NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email: oa@electrochem.org. All rights reserved.
引用
收藏
页码:II484 / II490
页数:7
相关论文
共 37 条
[1]   ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE ON VARIOUS METAL-ELECTRODES IN LOW-TEMPERATURE AQUEOUS KHCO3 MEDIA [J].
AZUMA, M ;
HASHIMOTO, K ;
HIRAMOTO, M ;
WATANABE, M ;
SAKATA, T .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1990, 137 (06) :1772-1778
[2]   ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE TO HIGHER HYDROCARBONS IN A KHCO3 AQUEOUS-SOLUTION [J].
AZUMA, M ;
HASHIMOTO, K ;
WATANABE, M ;
SAKATA, T .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1990, 294 (1-2) :299-303
[3]   A Novel Tripodal Ligand, Tris[(4′-methyl-2,2′-bipyridyl-4-yl)-methyl]carbinol and Its Trinuclear RuII/ReI Mixed-Metal Complexes: Synthesis, Emission Properties, and Photocatalytic CO2 Reduction [J].
Bian, Zhao-Yong ;
Sumi, Katsuhiro ;
Furue, Masaoki ;
Sato, Shunsuke ;
Koike, Kazuhide ;
Ishitani, Osamu .
INORGANIC CHEMISTRY, 2008, 47 (23) :10801-10803
[4]   Effects of process conditions and electrode material on reaction pathways for carbon dioxide electroreduction with particular reference to formate formation [J].
Chaplin, RPS ;
Wragg, AA .
JOURNAL OF APPLIED ELECTROCHEMISTRY, 2003, 33 (12) :1107-1123
[5]   Theoretical characterization of sulfur and nitrogen dual-doped graphene [J].
Denis, Pablo A. ;
Huelmo, C. Pereyra ;
Iribarne, Federico .
COMPUTATIONAL AND THEORETICAL CHEMISTRY, 2014, 1049 :13-19
[6]   A viable hydrogen-storage system based on selective formic acid decomposition with a ruthenium catalyst [J].
Fellay, Celine ;
Dyson, Paul J. ;
Laurenczy, Gabor .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (21) :3966-3968
[7]   Understanding Trends in the Electrocatalytic Activity of Metals and Enzymes for CO2 Reduction to CO [J].
Hansen, Heine A. ;
Varley, Joel B. ;
Peterson, Andrew A. ;
Norskov, Jens K. .
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2013, 4 (03) :388-392
[8]   FORMATION OF HYDROCARBONS IN THE ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE AT A COPPER ELECTRODE IN AQUEOUS-SOLUTION [J].
HORI, Y ;
MURATA, A ;
TAKAHASHI, R .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1989, 85 :2309-2326
[9]   CO2 Electroreduction at Bare and Cu-Decorated Pd Pseudomorphic Layers: Catalyst Tuning by Controlled and Indirect Supporting onto Au(111) [J].
Januszewska, Aneta ;
Jurczakowski, Rafal ;
Kulesza, Pawel J. .
LANGMUIR, 2014, 30 (47) :14314-14321
[10]   Recent advances in the homogeneous hydrogenation of carbon dioxide [J].
Jessop, PG ;
Joó, F ;
Tai, CC .
COORDINATION CHEMISTRY REVIEWS, 2004, 248 (21-24) :2425-2442