缺陷改性商业碳纳米管用于耐毒化二氧化碳电还原  

Defect-modified Commercial Carbon Nanotubes for Poison-resistant Electrochemical Carbon Dioxide Reduction

作　　者：李承育 尚露[1] 张铁锐[1,2] LI Chengyu;SHANG Lu;ZHANG Tierui(Key Laboratory of Photochemical Conversion and Optoelectronic Materials,Technical Institute of Physics and Chemistry,Chinese Academy of Sciences,Beijing 100190,China;Center of Materials Science and Optoelectronics Engineering,University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院理化技术研究所光化学转换与功能材料重点实验室,北京100190 [2]中国科学院大学材料科学与光电技术中心,北京100049

出　　处：《高等学校化学学报》2025年第5期84-91,共8页Chemical Journal of Chinese Universities

基　　金：国家重点研发计划项目(批准号:2024YFE0103000);国家自然科学基金(批准号:52422211,52120105002,22279150,22421005)资助.

摘　　要：在二氧化碳电还原反应(ECO_(2)RR)中,催化材料面临着实际应用条件复杂的挑战,尤其是在耐毒化方面.本文使用商业化多壁碳纳米管(MWCNT),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)、球差校正的环形明场扫描透射电子显微镜(AC ABF-STEM)、X射线衍射仪(XRD)、X射线光电子能谱仪(XPS)和拉曼光谱仪(Raman)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的结果表明,具有缺陷的碳纳米管的电化学CO_(2)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的增大而升高.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CO_(2)还原为CO的活性,CO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CO法拉第效率依然保持在96%以上,展现出良好的耐毒化性能.In the electrochemical carbon dioxide reduction reaction(ECO_(2)RR),catalytic materials face the challenge of complex practical application conditions,especially in terms of poisoning resistance.In this study,commercial multi-walled carbon nanotubes(MWCNT)were used to prepare defects 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),aberrationcorrected 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 improves 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 ECO_(2)RR catalysts.

关 键 词：二氧化碳还原 电催化 碳缺陷 商业碳纳米管 抗毒化 

分 类 号：O643.3[理学—物理化学]