摘要
合成气是一种CO和H2的混合气, 是工业上生产烯烃、液体 燃料、聚合物、药物等产品的重要原料. 通过电化学还原的方法 将CO2转化为合成气, 不仅能够减少大气中的CO2含量, 同时还能 缓解能源危机. 但是目前仍然缺乏廉价高效的电催化剂来实现可 控比例CO/H2的合成. 因此, 我们发展了一种简易的等离子体处理 策略, 利用氮掺杂碳纳米管阵列作为电催化剂, 通过电化学CO2-H2O还原制备CO/H2比例可控的合成气. 在不同的等离子体处理条 件下, CO/H2比例的范围可达0.55–3.03, 符合下游化工生产的原料 气标准. 通过优化等离子体处理条件, CO的法拉第效率最高可达 75%, 并且能够维持稳定性长达10 h. 通过研究氮掺杂的碳纳米管 的结构随处理条件的变化, 并结合其CO2还原活性, 我们推断出氮 掺杂碳纳米管中的吡啶氮有利于CO2转化为CO, 而吡咯氮和sp2平 面外的碳则有利于氢气的产生. 利用等离子体处理的方法能够有 效调节催化剂中各活性组分的比例, 从而调控CO2还原反应和析氢 反应的速率, 最终实现CO/H2比例可控的合成气制备.
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Acknowledgements
We acknowledge the National Natural Science Foundation of China (21871206 and 21901180), and China Postdoctoral Science Foundation (2019TQ0226) for the financial support.
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Zhang B conceived and directed the project. Ji Y carried out the experiments. Shi Y analyzed the data and wrote the paper. Zhang B and Liu C revised the paper. All authors contributed to the general discussion.
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The authors declare no conflict of interest.
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Experimental details and supplementary figures are available in the online version of the paper.
Yan Ji received his BSc degree from Tianjin Normal University in 2017. Currently, he is a Master candidate at Tianjin University under the supervision of Prof. Bin Zhang. His research topic is the development of non-noble metal electrocatalysts for CO2RR.
Yanmei Shi received her PhD degree from Tianjin University in 2018 (supervised by Prof. Bin Zhang). She is currently conducting postdoctoral research at Tianjin University (with Prof. Bin Zhang). Her research focuses on exploring structural reconstruction and active species of catalytic materials under electrocatalytic conditions.
Bin Zhang received his PhD degree from the University of Science and Technology of China in 2007 (supervised by Prof. Yi Xie). He carried out postdoctoral research at the University of Pennsylvania (July 2007 to July 2008, with Prof. Ritesh Agarwal) and worked as an Alexander von Humboldt fellow at Max Planck Institute of Colloids and Interfaces (August 2008 to July 2009, with Dayang Wang). Currently, he is a Fellow of the Royal Society of Chemistry (FRSC), and a professor at Tianjin University and the Collaborative Innovation Center of Chemical Science and Engineering (Tianjin). His research mainly focuses on the controlled chemical transformation synthesis of advanced nanomaterials for catalytic applications.
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Ji, Y., Shi, Y., Liu, C. et al. Plasma-regulated N-doped carbon nanotube arrays for efficient electrosynthesis of syngas with a wide CO/H2 ratio. Sci. China Mater. 63, 2351–2357 (2020). https://doi.org/10.1007/s40843-020-1396-7
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DOI: https://doi.org/10.1007/s40843-020-1396-7