Highly efficient electrocatalytic CO2 reduction by a CrIII quaterpyridine complex
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA(2024)
Abstract
Design tactics and mechanistic studies both remain as fundamental challenges during the exploitations of earth- abundant molecular electrocatalysts for CO2 reduction, especially for the rarely studied Cr-based ones. Herein, a quaterpyridyl Cr-III catalyst is found to be highly active for CO2 electroreduction to CO with 99.8% Faradaic efficiency in DMF/phenol medium. A nearly one order of magnitude higher turnover frequency (86.6 s(-1)) over the documented Cr- based catalysts (<10 s(-1)) can be achieved at an applied overpotential of only 190 mV which is generally 300 mV lower than these precedents. Such a high performance at this low driving force originates from the metal-ligand cooperativity that stabilizes the low- valent intermediates and serves as an efficient electron reservoir. Moreover, a synergy of electrochemistry, spectroelectrochemistry, electron paramagnetic resonance, and quantum chemical calculations allows to characterize the key Cr-II, Cr-I, Cr-0, and CO- bound Cr-0 intermediates as well as to verify the catalytic mechanism.
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Key words
CO2 reduction,molecular catalysis,chromium complex,CO binding,mechanism
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