Citation: Xiaoxu Duan, Junli Xu, Jiwei Li, Congcong Du, Kai Chen, Teng Xu, Yifei Sun, Haifeng Xiong. Enhancing CO₂ reduction efficiency with axial oxygen coordinated Ni-N₄ active sites on hierarchical pore N-doped carbon[J]. Chinese Chemical Letters, ;2025, 36(7): 110340. doi: 10.1016/j.cclet.2024.110340 shu

Enhancing CO₂ reduction efficiency with axial oxygen coordinated Ni-N₄ active sites on hierarchical pore N-doped carbon

Xiaoxu Duan ^{a, b, e} ,
Junli Xu ^{a, b, e} ,
Jiwei Li ^{a, b, e} ,
Congcong Du ^{a, b, c, e} ,
Kai Chen ^{a, b, e} ,
Teng Xu ^{a, b, e} ,
Yifei Sun ^{a, d, e, *,} ,
Haifeng Xiong ^{a, b, e, *,}

a.
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
b.
Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen 361102, China
c.
Qingyuan Innovation Laboratory, Quanzhou 362801, China
d.
Shenzhen Research Institute of Xiamen University, Shenzhen 518057, China
e.
College of Energy, Xiamen University, Xiamen 361102, China

yfsun@xmu.edu.cn

haifengxiong@xmu.edu.cn

Received Date: 19 February 2024
Revised Date: 13 July 2024
Accepted Date: 13 August 2024
Available Online: 22 August 2024

Figures(5)

The electrochemical reduction of carbon dioxide (CO₂RR) is a promising strategy for achieving carbon neutralization. The Ni-N₄ site is well known as the active site in metal single atoms on N-doped carbon catalysts, while its symmetric charge distribution nature is not favorable for electron transfer and then hindering the efficient CO₂RR. Herein, we constructed a Ni SA/CNs single-atom catalyst. Notably, it features unique Ni-N_4-O active sites, featuring one axial O atom and four planar N atoms, constituting a broken symmetrical electronic structure of Ni-N₄ sites. Furthermore, hierarchical pore structures were obtained with the assistance of NaNO₃ pore-forming agent during thermal treatment process, which promote electronic and mass transfer. And the resulting high specific surface area can host more Ni-N_4-O active sites. These specialized active sites promote the key intermediate (^*CO) adsorption/desorption and suppresses hydrogen evolution. Consequently, the Ni SA/CNs catalyst exhibits a high turnover frequency (TOF) value, reaching 34,081 h⁻¹ at -0.98 V vs. RHE. Additionally, it achieves an excellent CO Faradaic efficiency, exceeding 90%, over a wide potential range from -0.4 V to -1.0 V vs. RHE. This work not only offers a new method for the rational synthesize single-atom catalysts with unique Ni-N_4-O active sites, but also provides in-depth insight into the origin of catalytic activity of porous carbon-base catalysts.
- Nickel single-atom catalyst,
- N_i-n₄-O active site,
- CO₂ electroreduction,
- Hierarchical pore structure,
- N-doped carbon
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Enhancing CO2 reduction efficiency with axial oxygen coordinated Ni-N4 active sites on hierarchical pore N-doped carbon

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通讯作者: 陈斌, bchen63@163.com

Enhancing CO₂ reduction efficiency with axial oxygen coordinated Ni-N₄ active sites on hierarchical pore N-doped carbon