Affiliation:
1. Institute of Molecular Engineering and Applied Chemistry Anhui University of Technology Ma'anshan Anhui 243002 P. R. China
2. National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES (Ministry of Education) Key Laboratory of ETESPG (GHEI) School of Chemistry South China Normal University Guangzhou 510006 P. R. China
Abstract
AbstractThe efficient CO2 electroreduction into high‐value products largely relies on the CO2 adsorption/activation or electron‐transfer of electrocatalysts, thus site‐specific functionalization methods that enable boosted related interactions of electrocatalysts are much desired. Here, an oriented coordination strategy is reported to introduce N‐rich auxiliary (i.e., hexamethylenetetramine, HMTA) into metalloporphyrin metal organic frameworks (MOFs) to synthesize a series of site‐specific functionalized electrocatalysts (HMTA@MOF‐545‐M, M = Fe, Co, and Ni) and they are successfully applied in light‐assisted CO2 electroreduction. Noteworthy, thus‐obtained HMTA@MOF‐545‐Co presents approximately two times enhanced CO2 adsorption‐enthalpy and electrochemical active surface‐area with largely decreased impedance‐value after modification, resulting in almost twice higher CO2 electroreduction performance than its unmodified counterpart. Besides, its CO2 electroreduction performance can be further improved under light‐illumination and displays superior FECO (≈100%), high CO generation rate (≈5.11 mol m−2 h−1 at −1.1 V) and energy efficiency (≈70% at −0.7 V). Theoretical calculations verify that the oriented coordination of HMTA can increase the charge density of active sites, almost doubly enhance the CO2 adsorption energy, and largely reduce the energy barrier of rate determining step for the boosted performance improvement. This work might promote the development of modifiable porous crystalline electrocatalysts in high‐efficiency CO2 electroreduction.
Funder
National Natural Science Foundation of China
Natural Science Foundation of Guangdong Province
Subject
General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)
Cited by
4 articles.
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