Effect of the nitrogen/carbon ratio in the organic ligand of a nickel single-atom catalyst on its electrochemical activity in CO2 reduction

被引：5

作者：

Choi, Hyeonuk ^{[1
]}

Flah, Min Gwan ^{[2
]}

Suh, Jungwon ^{[1
]}

Lim, Chulwan ^{[2
]}

Kim, Beomil ^{[1
]}

Wang, Sun Eon ^{[1
]}

Lee, Jang Yong ^{[3
]}

Oh, Hyung-Suk ^{[2
,4
]}

Oh, Jihun ^{[1
]}

机构：

[1] Korea Adv Inst Sci & Technol KAIST, Dept Mat Sci & Engn, 291 Daehak Ro, Daejeon 34141, South Korea

[2] Korea Inst Sci & Technol KIST, Clean Energy Res Ctr, Hwarang Ro 14 Gil 5, Seoul 02792, South Korea

[3] Korea Res Inst Chem Technol KRICT, Hydrogen Energy Res Ctr, Daejeon 34114, South Korea

[4] Sungkyunkwan Univ SKKU, KIST SKKU Carbon Neutral Res Ctr, Suwon 16419, South Korea

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2024年 / 355卷

基金：

新加坡国家研究基金会;

关键词：

Single-atom catalyst; Small organic ligands; Electrochemical CO2 reduction; Large-scale synthesis; CO production; GENERAL-SYNTHESIS; CARBON-DIOXIDE; METAL; EFFICIENT;

D O I：

10.1016/j.apcatb.2024.124192

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：

Simple, large-scale synthesis of metal single-atom catalysts (SACs) is limited by the aggregation of metal atoms on the support material surface. The N atoms in small organic ligands (SOLs) can anchor single metal atoms, affording abundant surface-active sites. In this study, we investigated the effect of the nitrogen/carbon ratio (N/C) in SOLs on the properties of the resultant Ni single-atom confined nitrogen-doped carbon black (Ni-NCB). The N/C ratio affected the thermal stability of Ni-NCB_N/Cs during carbonization, and the optimal Ni-NCB (Ni-NCB_0.5) was synthesized with the SOL 2-methylimidazole. Ni-NCB_0.5 achieved a CO partial current density of > 500 mA cm(-2) and high CO Faradaic efficiency (96.4 %) in the CO2 reduction reaction. The 3- and 4-cell stack systems with Ni-NCB_0.5 (25 cm(2) area per unit cell) exhibited an overall current of 10 A, high CO selectivity (> 96.0 %), and long-term stability (50 h). This synthetic strategy for SACs can be commercialized and even extended to other industrial electrocatalysts.

引用

页数：10

共 37 条

[1] Synthesis of a Nickel Single-Atom Catalyst Based on Ni-N4-xCx Active Sites for Highly Efficient CO2 Reduction Utilizing a Gas Diffusion Electrode [J].

Abbas, Syed Asad ;

Song, Jun Tae ;

Tan, Ying Chuan ;

Nam, Ki Min ;

Oh, Jihun ;

Jung, Kwang-Deog .

ACS APPLIED ENERGY MATERIALS, 2020, 3 (09) :8739-8745

[2] Review-Non-Noble Metal-Based Single-Atom Catalysts for Efficient Electrochemical CO2 Reduction Reaction [J].

Choi, Hyeonuk ;

Lee, Dong-Kyu ;

Han, Mi-Kyung ;

Janani, Gnanaprakasam ;

Surendran, Subramani ;

Kim, Jin Hyeok ;

Kim, Jung Kyu ;

Cho, Hoonsung ;

Sim, Uk .

JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2020, 167 (16)

[3] A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature [J].

Deng, Dehui ;

Chen, Xiaoqi ;

Yu, Liang ;

Wu, Xing ;

Liu, Qingfei ;

Liu, Yun ;

Yang, Huaixin ;

Tian, Huanfang ;

Hu, Yongfeng ;

Du, Peipei ;

Si, Rui ;

Wang, Junhu ;

Cui, Xiaoju ;

Li, Haobo ;

Xiao, Jianping ;

Xu, Tao ;

Deng, Jiao ;

Yang, Fan ;

Duchesne, Paul N. ;

Zhang, Peng ;

Zhou, Jigang ;

Sun, Litao ;

Li, Jianqi ;

Pan, Xiulian ;

Bao, Xinhe .

SCIENCE ADVANCES, 2015, 1 (11)

[4] Transforming Energy with Single-Atom Catalysts [J].

Ding, Shipeng ;

Hulsey, Max J. ;

Perez-Ramirez, Javier ;

Yang, Ning .

JOULE, 2019, 3 (12) :2897-2929

[5] Operando cathode activation with alkali metal cations for high current density operation of water-fed zero-gap carbon dioxide electrolysers [J].

Endrodi, B. ;

Samu, A. ;

Kecsenovity, E. ;

Halmagyi, T. ;

Sebok, D. ;

Janaky, C. .

NATURE ENERGY, 2021, 6 (04) :439-448

[6] Multilayer Electrolyzer Stack Converts Carbon Dioxide to Gas Products at High Pressure with High Efficiency [J].

Endrodi, B. ;

Kecsenovity, E. ;

Samu, A. ;

Darvas, F. ;

Jones, R. V. ;

Torok, V. ;

Danyi, A. ;

Janaky, C. .

ACS ENERGY LETTERS, 2019, 4 (07) :1770-1777

[7] General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities [J].

Fei, Huilong ;

Dong, Juncai ;

Feng, Yexin ;

Allen, Christopher S. ;

Wan, Chengzhang ;

Volosskiy, Boris ;

Li, Mufan ;

Zhao, Zipeng ;

Wang, Yiliu ;

Sun, Hongtao ;

An, Pengfei ;

Chen, Wenxing ;

Guo, Zhiying ;

Lee, Chain ;

Chen, Dongliang ;

Shakir, Imran ;

Liu, Mingjie ;

Hu, Tiandou ;

Li, Yadong ;

Kirkland, Angus I. ;

Duan, Xiangfeng ;

Huang, Yu .

NATURE CATALYSIS, 2018, 1 (01) :63-72

[8] Challenges and Opportunities in Engineering the Electronic Structure of Single-Atom Catalysts [J].

Giulimondi, Vera ;

Mitchell, Sharon ;

Perez-Ramirez, Javier .

ACS CATALYSIS, 2023, 13 (05) :2981-2997

[9] Regulating the Coordination Environment of MOF-Templated Single-Atom Nickel Electrocatalysts for Boosting CO2 Reduction [J].

Gong, Yun-Nan ;

Jiao, Long ;

Qian, Yunyang ;

Pan, Chun-Yang ;

Zheng, Lirong ;

Cai, Xuechao ;

Liu, Bo ;

Yu, Shu-Hong ;

Jiang, Hai-Long .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2020, 59 (07) :2705-2709

[10]

Gore JP, 2011, CARBON NANOTUBES - SYNTHESIS, CHARACTERIZATION, APPLICATIONS, P121

← 1 2 3 4 →