Understanding Selective Reduction of CO2 to CO on Modified Carbon Electrocatalysts

被引:20
作者
Jung, Hyejin [1 ,2 ]
Lee, Si Young [1 ,2 ]
Won, Da Hye [1 ]
Kim, Ki-Jeong [3 ]
Chae, Sang Youn [1 ]
Oh, Hyung-Suk [1 ]
Min, Byoung Koun [1 ,4 ]
Hwang, Yun Jeong [1 ,2 ]
机构
[1] Korea Inst Sci & Technol, Clean Energy Res Ctr, 5,Hwarang Ro 14 Gil, Seoul 02792, South Korea
[2] Korea Univ Sci & Technol, KIST Sch, Div Energy & Environm Technol, Seoul 02792, South Korea
[3] Pohang Accelerator Lab, Beamline Res Div, Pohang 37673, South Korea
[4] Korea Univ, Green Sch, 145 Anam Ro, Seoul 02841, South Korea
来源
CHEMELECTROCHEM | 2018年 / 5卷 / 12期
基金
新加坡国家研究基金会;
关键词
CO2; reduction; electrochemistry; doped carbon; materials science; selective CO production; OXYGEN REDUCTION; ELECTROCHEMICAL REDUCTION; DIOXIDE ELECTROREDUCTION; NANOTUBE ARRAYS; PERFORMANCE; CONVERSION; CATALYSIS; SITES; POLYANILINE; ELECTRODES;
D O I
10.1002/celc.201701337
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
Modified carbon powders are attractive electrocatalysts for chemical conversion due to their low cost and high activity. Here, we demonstrate that electrochemical conversion activities of CO2 to CO in aqueous media are enhanced by the incorporation of transition metals into nitrogen-doped carbon (M-N/C; M=Fe, Co, Cu). The type of the metals is thereby critical to achieve selective CO production over H-2. Among M-N/C and N/C catalysts, Fe-N/C exhibited the highest faradaic efficiency for CO conversion, significantly enhanced compared with the metal-free N-doped carbon electrocatalyst. In addition, the catalysts containing higher pyridinic N and graphitic N but lower pyrrolic N contents favor CO production at lower bias potentials. Meanwhile, the total amount of N content in the carbon material is less important. Our CO2 reduction reaction results combined with X-ray photoelectron spectroscopy analysis propose that the modification of nitrogen states in the carbon structure is crucial in CO2RR activity.
引用
收藏
页码:1615 / 1621
页数:7
相关论文
共 41 条
[1]   Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries [J].
Centi, Gabriele ;
Quadrelli, Elsje Alessandra ;
Perathoner, Siglinda .
ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (06) :1711-1731
[2]   Molecular Catalysis of the Electrochemical and Photochemical Reduction of CO2 with Earth-Abundant Metal Complexes. Selective Production of CO vs HCOOH by Switching of the Metal Center [J].
Chen, Lingjing ;
Guo, Zhenguo ;
Wei, Xi-Guang ;
Gallenkamp, Charlotte ;
Bonin, Julien ;
Anxolabehere-Mallart, Elodie ;
Lau, Kai-Chung ;
Lau, Tai-Chu ;
Robert, Marc .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (34) :10918-10921
[3]   Direct and Highly Selective Conversion of Synthesis Gas into Lower Olefins: Design of a Bifunctional Catalyst Combining Methanol Synthesis and Carbon-Carbon Coupling [J].
Cheng, Kang ;
Gu, Bang ;
Liu, Xiaoliang ;
Kang, Jincan ;
Zhang, Qinghong ;
Wang, Ye .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (15) :4725-4728
[4]   Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction [J].
Cheon, Jae Yeong ;
Kim, Taeyoung ;
Choi, YongMan ;
Jeong, Hu Young ;
Kim, Min Gyu ;
Sa, Young Jin ;
Kim, Jaesik ;
Lee, Zonghoon ;
Yang, Tae-Hyun ;
Kwon, Kyungjung ;
Terasaki, Osamu ;
Park, Gu-Gon ;
Adzic, Radoslav R. ;
Joo, Sang Hoon .
SCIENTIFIC REPORTS, 2013, 3
[5]   The path towards sustainable energy [J].
Chu, Steven ;
Cui, Yi ;
Liu, Nian .
NATURE MATERIALS, 2017, 16 (01) :16-22
[6]   Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst [J].
Chung, Hoon T. ;
Cullen, David A. ;
Higgins, Drew ;
Sneed, Brian T. ;
Holby, Edward F. ;
More, Karren L. ;
Zelenay, Piotr .
SCIENCE, 2017, 357 (6350) :479-483
[7]   Metal-free doped carbon materials as electrocatalysts for the oxygen reduction reaction [J].
Daems, Nick ;
Sheng, Xia ;
Vankelecom, Ivo F. J. ;
Pescarmona, Paolo P. .
JOURNAL OF MATERIALS CHEMISTRY A, 2014, 2 (12) :4085-4110
[8]   Metal-Free Carbon Materials for CO2 Electrochemical Reduction [J].
Duan, Xiaochuan ;
Xu, Jiantie ;
Wei, Zengxi ;
Ma, Jianmin ;
Guo, Shaojun ;
Wang, Shuangyin ;
Liu, Huakun ;
Dou, Shixue .
ADVANCED MATERIALS, 2017, 29 (41)
[9]   Electrochemical Reduction of CO2 at Functionalized Au Electrodes [J].
Fang, Yuxin ;
Flake, John C. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (09) :3399-3405
[10]   Extracellular entrapment and degradation of single-walled carbon nanotubes [J].
Farrera, Consol ;
Bhattacharya, Kunal ;
Lazzaretto, Beatrice ;
Andon, Fernando T. ;
Hultenby, Kjell ;
Kotchey, Gregg P. ;
Star, Alexander ;
Fadeel, Bengt .
NANOSCALE, 2014, 6 (12) :6974-6983