Bimetallic phthalocyanine heterostructure used for highly selective electrocatalytic CO_(2) reduction  

双金属酞菁异质结构高选择性电催化CO_(2)还原

作　　者：Chenhuai Yang Zengqiang Gao Dingjia Wang Shuyu Li Junjun Li Yating Zhu Haiqing Wang Wenjuan Yang Xuejiao J.Gao Zhicheng Zhang Wenping Hu 杨宸槐;高增强;王定佳;李舒豫;李俊俊;朱亚廷;王海青;杨文娟;高雪娇;张志成;胡文平(Tianjin Key Laboratory of Molecular Optoelectronic Sciences,Department of Chemistry,School of Science,Tianjin University,Tianjin 300072,China;College of Chemistry and Chemical Engineering,Jiangxi Normal University,Nanchang 330022,China;Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong,Institute for Advanced Interdisciplinary Research(iAIR),University of Jinan,Jinan 250022,China;SZU-NUS Collaborative Innovation Centre for Optoelectronic Science&Technology,International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education,Institute of Microscale Optoelectronics,Shenzhen University,Shenzhen 518060,China)

机构地区：[1]Tianjin Key Laboratory of Molecular Optoelectronic Sciences,Department of Chemistry,School of Science,Tianjin University,Tianjin 300072,China [2]College of Chemistry and Chemical Engineering,Jiangxi Normal University,Nanchang 330022,China [3]Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong,Institute for Advanced Interdisciplinary Research(iAIR),University of Jinan,Jinan 250022,China [4]SZU-NUS Collaborative Innovation Centre for Optoelectronic Science&Technology,International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education,Institute of Microscale Optoelectronics,Shenzhen University,Shenzhen 518060,China

出　　处：《Science China Materials》2022年第1期155-162,共8页中国科学（材料科学（英文版）

基　　金：supported by the National Natural Science Foundation of China(22071172,91833306,21875158,51633006,and 51733004).

摘　　要：Heterogeneous molecular catalysts,such as metal phthalocyanines,are efficient electrocatalysts for CO_(2) reduction reaction(CO_(2)RR).However,the rational design and synthesis of a molecular catalyst-based heterostructure for CO_(2)RR remains challenging.Herein,we developed a crystalline bimetallic phthalocyanine heterostructure electrocatalyst(CoPc/FePc HS),which achieved an excellent CO_(2)-to-CO conversion efficiency(99%)and outstanding long-term stability after 10 h of electrocatalysis.Density functional theory calculations revealed that the enhancement of CO_(2)RR performance could be attributed to the distinct electron transfer pattern between FePc and CoPc.The heterostructural engineering in molecular catalysts would inspire a unique approach for improving CO_(2)RR performance.自工业革命以来,化石燃料的大量消耗导致大气中CO_(2)浓度显著增加,引发了全球气候变暖等问题.电化学CO_(2)还原能够利用可再生能源产生的间歇性电力可持续地将CO_(2)转化为高附加值化学品或燃料,是实现碳中和的有效途径.目前,非均相分子催化剂如金属酞菁能够有效催化CO_(2)还原反应(CO_(2)RR),但是分子催化剂异质结构的合理设计与合成仍极具挑战.基于此,我们发展了一种具有高结晶度的双金属酞菁异质结构(CoPc/FePc HS),其电催化CO_(2)还原为CO的法拉第效率高达99%,并在运行10小时后性能基本保持不变.密度泛函理论计算表明,FePc和CoPc之间不同的电子转移模式能够有效提高CO_(2)RR性能.构筑分子催化剂异质结构有望成为CO_(2)RR性能提升的有效策略.

关 键 词：molecular catalyst phthalocyanine heterostructure CO_(2)reduction electronic effect 

分 类 号：X701[环境科学与工程—环境工程] TQ426[化学工程]