首页|Boosting Electrocatalytic CO2 Reduction with Conjugated Bimetallic Co/Zn Polyphthalocyanine Frameworks

Boosting Electrocatalytic CO2 Reduction with Conjugated Bimetallic Co/Zn Polyphthalocyanine Frameworks

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Development of high-efficiency electrode materials for the electrochemical CO2 reduction reaction(CO2RR)with high current density and selectivity compatible with industry is an important but signifi-cant challenge.Herein,we describe a facile strategy to enhance the selectivity and current density by regu-lating the local electron density of the cobalt site in a series of stable,conjugated,bimetallic Co/Zn poly-phthalocyanine frameworks CoxZnyPPc with an AB stacking model under alkaline aqueous conditions.When adjusting the ratio of Co and Zn to 3:1,the optimal Co3Zn1PPc exhibits an industry-compatible CO partial current density of 212 mA cm-2 at-0.9 V versus reversible hydrogen electrode in a flow cell,which is 1.7 and 9.1 times that of the single metal polyphthalocyanine CoPPc and ZnPPc,respectively.Co3Zn1PPc shows a high CO Faraday efficiency of more than 90％in a wide operating potential win-dow of-0.3 to-0.9 V.In-depth experimental and theoretical analysis revealed that introduction of electron-rich Zn atoms modified the electron densi-ty of the active Co center,placing Co in the electron-rich region and weakening the bonding strength with the reaction intermediate,thereby improving the CO2RR performance.These results clarify the interaction mechanism of dual metal sites at the atomic level and provide a new avenue for the de-sign of electrocatalysts with potential in industrial applications.

CO2 electrocatalysisflow cellcobalt polyphthalocyaninezinc polyphthalocyanineAB stacking

Nan Li、Duan-Hui Si、Qiu-jin Wu、Qiao Wu、Yuan-Biao Huang、Rong Cao

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State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou,Fujian 350002

University of Chinese Academy of Science,Beijing 100049

Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou,Fujian 350108

国家重点研发计划国家重点研发计划国家自然科学基金国家自然科学基金国家自然科学基金Fujian Science& Technology Innovation Laboratory for Optoelectronic Information of China

2018YFA02086002018YFA07045022187126322071245220330082021ZZ103

2023

10.31635/ccschem.022.202201943

中国化学会会刊(英文)

中国化学会会刊(英文)

CSCD
ISSN：
年,卷(期)：2023.5(5)
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