Xia Zhanghui, Zhai Jianxin, Lin Longfei, Chen Xiao, Xue Cheng, Jia Shuaiqiang, Jiao Jiapeng, Dong Mengke, Han Wanying, Zheng Xinrui, Xue Teng, Wu Haihong, Han Buxing
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
Institute of Eco-Chongming Shanghai 202162 China.
Chem Sci. 2025 Jun 17;16(29):13382-13389. doi: 10.1039/d5sc02602d. eCollection 2025 Jul 23.
The development of non-noble metal catalysts for efficient CO 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 CO methanation. Remarkably, the Co@CN-700 catalyst achieved a prominent CH production rate of 199.4 mmol g h with near-unity selectivity (99.4%) and high CO 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 CO methanation. This work offers a straightforward and effective approach for designing non-noble metal catalysts with high activity, selectivity, and stability.
开发用于在温和条件下高效进行CO甲烷化反应的非贵金属催化剂仍然是一项重大挑战。在此，通过热解还原策略制备了一种非贵金属催化剂，即封装在氮掺杂碳纳米管（Co@CN-700）中空通道内的钴纳米颗粒（Co NPs），用于光热CO甲烷化。值得注意的是，Co@CN-700催化剂在250°C下实现了199.4 mmol g h的显著CH生成速率，具有接近100%的选择性（99.4%）和高CO转化率（85.8%），与已报道的催化剂相比表现出色。电磁模拟和密度泛函理论计算表明Co NPs的等离子体共振效应增强了局部电场，从而改变了中间态和速率限制步骤，促进了CO甲烷化。这项工作为设计具有高活性、选择性和稳定性的非贵金属催化剂提供了一种直接有效的方法。
