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dc.contributor.authorChen, Kejun
dc.contributor.authorCao, Maoqi
dc.contributor.authorLin, Yiyang
dc.contributor.authorFu, Junwei
dc.contributor.authorLiao, Hanxiao
dc.contributor.authorXie, Feng
dc.contributor.authorZhou, Yajiao
dc.contributor.authorYang, Baopeng
dc.contributor.authorLiu, Kang
dc.contributor.authorChen, Guozhu
dc.contributor.authorLi, HongMei
dc.contributor.authorWu, Dawang
dc.contributor.authorQiu, Xiaoqing
dc.contributor.authorHu, Junhua
dc.contributor.authorZheng, Xu-Sheng
dc.contributor.authorShakouri, Mohsen
dc.contributor.authorXiao, Qunfeng
dc.contributor.authorHu, Yongfeng
dc.contributor.authorLi, Jun
dc.contributor.authorLiu, Min
dc.identifier.citationChen, K., Cao, M., Lin, Y., Fu, J., Liao, H., Xie, F., … Liu, M. (2021). Substituent-induced electronic localization of nickel phthalocyanine with enhanced electrocatalytic CO2 reduction. doi:10.21203/
dc.description.abstractAbstract Designing efficient catalysts with high activity and selectivity is desirable and challenging for CO2 reduction reaction (CO2RR). Nickel phthalocyanine (NiPc) is a promising molecule catalyst for CO2RR. However, the pristine NiPc suffers from poor CO2 adsorption and activation due to its electron deficiency of Ni–N4 site, which leads to inferior activity and stability during CO2RR. Here, we develop a substituent-induced electronic localization strategy to improve CO2 adsorption and activation, and thus catalytic performance. Theoretic calculations and experimental results indicate that the electronic localization on the Ni site induced by electron-donating substituents (hydroxyl or amino) of NiPc greatly enhances the CO2 adsorption and activation, which is positively associated with the electron-donating abilities of substituents. Employing the optimal catalyst of amino-substituted NiPc to catalyze CO2 into CO in flow cell can achieve an ultrahigh activity and selectivity of 99.8% at the current densities up to 400 mA cm$^{-2}$. This work offers a novel strategy to regulate the electronic structure of the active site by introducing substituents for highly efficient CO2RR.
dc.description.sponsorshipThe authors gratefully thank the International Science and Technology Cooperation Program (Grant No. 2017YFE0127800 and 2018YFE0203400), Natural Science Foundation of China (Grant No. 21872174 and U1932148), Hunan Provincial Science and Technology Program (No.2017XK2026), Shenzhen Science and Technology Innovation Project (Grant No. JCYJ20180307151313532). Natural Science Foundation of Education Department of Guizhou Province ([2016]110, [2015]342).
dc.publisherResearch Square Platform LLC
dc.rightsArchived with thanks to Research Square
dc.subjectenhanced electrocatalytic CO2 reduction
dc.subjecthighly efficient CO2RR
dc.titleSubstituent-induced electronic localization of nickel phthalocyanine with enhanced electrocatalytic CO2 reduction
dc.contributor.departmentChemical Science Program
dc.contributor.departmentChemical Science
dc.contributor.departmentBiological and Environmental Sciences and Engineering (BESE) Division
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.contributor.institutionCentral South University
dc.contributor.institutionQiannan Normal University for Nationalities
dc.contributor.institutionCollege of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China.
dc.contributor.institutionZhengzhou University
dc.contributor.institutionUniversity of Science and Technology of China
dc.contributor.institutionCanadian Light Source
dc.contributor.institutionCanadian Light Source (Canada)
dc.contributor.institutionUniversity of Toronto
kaust.personXie, Feng

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