Controllable construction of cobalt nanoparticles in nitrogen-doped carbon nanotubes for photothermal CO2 methanation

Zhanghui Xia; Jianxin Zhai; Longfei Lin; Xiao Chen; Cheng Xue; Shuaiqiang Jia; Jiapeng Jiao; Mengke Dong; Wanying Han; Xinrui Zheng; Teng Xue; Haihong Wu; Buxing Han

doi:10.1039/d5sc02602d

Controllable construction of cobalt nanoparticles in nitrogen-doped carbon nanotubes for photothermal CO₂ methanation

Chem Sci. 2025 Jun 17. doi: 10.1039/d5sc02602d. Online ahead of print.

Authors

Zhanghui Xia^{1

2}, Jianxin Zhai^{1

2}, Longfei Lin^{3

4}, Xiao Chen^{1

2}, Cheng Xue^{1

2}, Shuaiqiang Jia^{1

2}, Jiapeng Jiao^{1

2}, Mengke Dong^{1

2}, Wanying Han^{1

2}, Xinrui Zheng^{1

2}, Teng Xue^{1

2}, Haihong Wu^{1

2}, Buxing Han^{1

3

2

4}

Affiliations

¹ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University Shanghai 200062 China hhwu@chem.ecnu.edu.cn.
² Institute of Eco-Chongming Shanghai 202162 China.
³ Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences Beijing 100190 China linlongfei@iccas.ac.cn hanbx@iccas.ac.cn.
⁴ School of Chemical Sciences, University of Chinese Academy of Sciences Beijing 100049 China.

Abstract

The development of non-noble metal catalysts for efficient CO₂ methanation reaction under mild conditions remains a significant challenge. Herein, a non-noble metal catalyst, cobalt nanoparticles (Co NPs) encapsulated within the hollow channels of nitrogen-doped carbon nanotubes (Co@CN-700), was prepared by a pyrolysis-reduction strategy for photothermal CO₂ methanation. Remarkably, the Co@CN-700 catalyst achieved a prominent CH₄ production rate of 199.4 mmol g_cat ^-1 h^-1 with near-unity selectivity (99.4%) and high CO₂ conversion (85.8%) at 250 °C, which is outstanding compared to the catalysts reported. The electromagnetic simulation and density functional theory calculations demonstrated that the plasmonic resonance effect of Co NPs enhances the local electric field and thereby alters the intermediate states and rate-limiting step to facilitate CO₂ methanation. This work offers a straightforward and effective approach for designing non-noble metal catalysts with high activity, selectivity, and stability.