钴酞菁/多孔碳气凝胶复合结构用于高效电催化CO_(2)还原  

Cobalt phthalocyanine/porous carbon aerogel composite for efficient electrocatalytic CO_(2)reduction

作　　者：周暾 龚善和 吕晓萌[3] 冯玉祥 黄春霞 朱桂生 Zhou Tun;Gong Shanhe;Lv Xiaomeng;Feng Yuxiang;Huang Chunxia;Zhu Guisheng(Jiangsu Sopo Chemical Corporation Ltd.,Zhenjiang 212006,China;School of Chemistry and Chemical Engineering,Jiangsu University,Zhenjiang 212013,China;Jiangsu University,School of the Environment and Safety Engineering,Zhenjiang 212013,China;Jiangsu Sopo Polyester Technology Corporation Ltd.,Zhenjiang 212000,China)

机构地区：[1]江苏索普化工股份有限公司,江苏镇江212006 [2]江苏大学环境与安全工程学院,江苏镇江212013 [3]江苏大学化学化工学院,江苏镇江212013 [4]江苏索普聚酯科技有限公司,江苏镇江212000

出　　处：《煤炭与化工》2023年第11期132-140,156,共10页Coal and Chemical Industry

基　　金：镇江市重点研发计划:CO_(2)→CO高效稳定电催化转化关键技术的研发(GY2021004)。

摘　　要：利用可再生能源将CO_(2)转化成高附加值的燃料或化学品,是一项实现“碳中和,碳达峰”的新资源化技术,但目前高性能电催化CO_(2)转化的催化剂研发,仍然是一项热点问题。设计具有“类珊瑚状”结构的多级孔氮掺杂碳气凝胶(N-CA)作为优化气体传质的碳载体,利用非共价固定技术,将酞菁钴(CoPc)稳定于气凝胶骨架的表面,以实现活性位点和导电碳骨架稳定结合。CoPc@N-CA展现出优异的电催化CO_(2)还原(CO_(2)RR)活性,在较宽的电势窗口-0.5~-1.0 V vs.RHE下,对CO的选择性>80%,最高为99.05%;在-0.85 V vs.RHE电位下,CoPc@N-CA对CO的部分电流密度达到14.40 mA·cm^(-2),约是以商业碳黑(CB)为基底设计的CoPc@CB(3.66·mA cm^(-2))催化剂的4倍。内在活性分析发现,CoPc@N-CA优异的活性可归因于N-CA独特的多孔结构,这不仅促进了CO_(2)分子的传质,有利于CO_(2)RR反应动力学,而且有利于暴露Co活性位点,从而促进CO_(2)RR。Electrocatalytic CO_(2)reduction into high value-added fuels or chemicals by renewable energy to achieve the“carbon neutrality and peak”is attractive,but still challenged by developing high-performance electrocatalytic catalysts for electrocatalytic CO_(2)reduction reaction(CO_(2)RR).Herein,porous nitrogen-doped carbon aerogels(N-CA)with“coral-like”structure was designed as the substrate to optimize gas mass transfer,and cobalt phthalocyanine(CoPc)was stabilized on N-CA surface by non-covalent immobilization technology to obtain CoPc@N-CA,realizing the stable combination of active sites and conductive carbon skeleton.As a result,CoPc@N-CA exhibits excellent CO_(2)RR activity,CO Faradaic efficiency(FECO)80%at the wide potential window of-0.5 to-1.0 V vs.RHE,and the maximal FECO of 99.05%.Meanwhile,CoPc@N-CA reaches a high CO partial current density(jCO)of 14.40 mA·cm^(-2)at-0.85 V vs.RHE,which is close to 4 times of that of CoPc@CB(3.66 mA·cm^(-2)),where carbon black(CB)was chosen as substrate to obtain [e-mail] activity analysis illustrates that the excellent activity of CoPc@N-CA can be attributed to the unique porous structure of N-CA,which not only promotes the mass transfer of CO_(2)molecules,but also facilitates the reaction kinetics of CO_(2)RR,and exposes the active sites of Co,promoting the activity CO_(2)RR.

关 键 词：电催化CO_(2)还原 碳气凝胶 多相分子催化剂 CO产物 

分 类 号：TQ426.7[化学工程]