高等学校化学学报

高等学校化学学报

• 研究论文 • 上一篇    下一篇

缺陷改性商业碳纳米管用于耐毒化二氧化碳电还原

李承育1,2，尚露1，张铁锐1,2   

  1. 1. 中国科学院理化技术研究所
    2. 中科院理化技术所
  • 收稿日期:2025-02-14 修回日期:2025-03-18 出版日期:2025-03-24 发布日期:2025-03-24
  • 通讯作者: 张铁锐 E-mail:tierui@mail.ipc.ac.cn
  • 基金资助:
    国家重点基础研究发展计划(批准号：2021YFA1500803)，国家自然科学基金(批准号：51825205、52422211、22421005、22279150、52120105002、22102202、22088102、52072382)，中国科学院DNL合作基金(批准号：DNL202016)，中国科学院稳定支持基础研究领域青年团队计划项目基金(批准号：YSBR-004)，中国博士后科学基金(批准号：BX2021323)资助

Defect-Modified Commercial Carbon Nanotubes for Poison-Resistant Electrochemical Carbon Dioxide Reduction

LI Chengyu1,2，SHANG Lu1，ZHANG Tierui1,2   

  1. 1. Technical Institute of Physics and Chemistry, Chinese Academy of Sciences
    2. University of Chinese Academy of Sciences
  • Received:2025-02-14 Revised:2025-03-18 Online:2025-03-24 Published:2025-03-24
  • Contact: ZHANG Tierui E-mail:tierui@mail.ipc.ac.cn
  • Supported by:
    Supported by the National Key Projects for Fundamental Research and Development of China (No. 2021YFA1500803), the National Natural Science Foundation of China (Nos. 51825205, 52422211, 22421005, 22279150, 52120105002, 22102202, 22088102, 52072382), the DNL Cooperation Fund, CAS (No. DNL202016), the CAS Project for Young Scientists in Basic Research (No. YSBR-004), and the China Postdoctoral Science Foundation (No. BX2021323)

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摘要： 在二氧化碳电还原反应（ECO2RR）中，催化材料面临着实际应用条件复杂中存在的易中毒等系列挑战。本研究使用商业化多壁碳纳米管，通过先引入氮元素再脱除的方法，制备了富含石墨化碳缺陷的材料，利用透射电子显微镜（TEM）、球差校正的扫描透射电子显微镜（AC STEM）、X射线衍射仪（XRD）、X射线光电子能谱（XPS）和拉曼光谱仪（Raman Spectrometer）对催化剂的形貌、晶体结构、元素组成和缺陷程度进行分析表征. 基于流动池测试体系结果表明，具有缺陷的碳纳米管，其电化学二氧化碳还原活性远高于未经处理的原始碳纳米管，且催化性能随缺陷程度增大而升高. 其中缺陷程度最高的MWCNT-N-800，在宽电位范围内展现出优异的将二氧化碳还原为一氧化碳的活性，一氧化碳法拉第效率最高可达99%以上，电流密度大于 200 mA cm-2. 此外，在模拟含有毒化物质的烟道气条件下，MWCNT-N-800的一氧化碳法拉第效率依然保持在96%以上，展现出良好的耐毒化性能. 本研究为开发高效、抗毒化的非金属ECO2RR催化剂提供了思路。

关键词: 二氧化碳还原, 电催化, 碳缺陷, 商业碳纳米管, 抗毒化

Abstract: In the electrochemical carbon dioxide reduction reaction (ECO2RR), catalytic materials face a series of challenges such as susceptibility to poisoning under complex practical application conditions. In this study, commercial multi-walled carbon nanotubes were used to prepare defect rich in graphitic carbon materials through nitrogen doping and removal methods. The morphology, crystal structure, elemental composition, and defect degree of the catalysts were analyzed and characterized by transmission electron microscopy (TEM), aberration-corrected scanning transmission electron microscopy (AC STEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman spectrometer. Based on the flow cell testing system, the results showed that the activity of defective carbon nanotubes is much higher than that of untreated carbon nanotubes, and the catalytic performance improved with the increase of defect degree. Among them, MWCNT-N-800 with the highest defect degree can achieve excellent electrochemical activity for carbon dioxide reduction to carbon monoxide over a broad potential range, with a maximum carbon monoxide Faraday efficiency of more than 99% and a current density of more than 200 mA cm-2. Furthermore, under the simulated flue gas conditions containing poisoning substances, the Faradaic efficiency of carbon monoxide for MWCNT-N-800 still remained above 96%, showing good poisoning resistance. This study provides ideas for the development of efficient and poison-resistant non-metallic ECO2RR catalysts.

Key words: Carbon dioxide reduction; Electrocatalysis, Carbon defects, Commercial carbon nanotubes, Poison-resistant

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