期刊
NATURE COMMUNICATIONS
卷 13, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-022-32740-z
关键词
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资金
- National Natural Science Foundation of China [22072101, 22075193]
- Natural Science Foundation of Jiangsu Province [BK20211306, BK20220027]
- Six Talent Peaks Project in Jiangsu Province [TD-XCL-006]
- Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions
- Australian Research Council [FT190100636, DP190103472]
- Australian Government
- Honorary Professor Program of Jiangsu Province
- Collaborative Innovation Center of Suzhou Nano Science Technology
- Users with Excellence Program of Hefei Science Center CAS [2019HSC-UE002]
In this study, the authors successfully electrocatalytically reduced CO2 into high-value alcohols through the synergy between inorganic and organic phases. They found that copper complexes with higher intramolecular tension and coordination asymmetry exhibited higher catalytic activity. This study highlights the exploitation of structure-dependent electrochemical property to guide CO2 reduction pathways and provides a potential strategy for targeted alcohol synthesis by constructing organic/inorganic Cu hybrids.
Electrocatalytic reduction of CO2 into multi-carbon alcohols of high economic merit offers an effective means to close the carbon cycle. Here the authors show the synergy between inorganic and organic phases derived from rationally designed molecular precursors to produce alcohols in high efficiency. Electrocatalytic reduction of CO2 into alcohols of high economic value offers a promising route to realize resourceful CO2 utilization. In this study, we choose three model bicentric copper complexes based on the expanded and fluorinated porphyrin structure, but different spatial and coordination geometry, to unravel their structure-property-performance correlation in catalyzing electrochemical CO2 reduction reactions. We show that the complexes with higher intramolecular tension and coordination asymmetry manifests a lower electrochemical stability and thus more active Cu centers, which can be reduced during electrolysis to form Cu clusters accompanied by partially-reduced or fragmented ligands. We demonstrate the hybrid structure of Cu cluster and partially reduced O-containing hexaphyrin ligand is highly potent in converting CO2 into alcohols, up to 32.5% ethanol and 18.3% n-propanol in Faradaic efficiencies that have been rarely reported. More importantly, we uncover an interplay between the inorganic and organic phases to synergistically produce alcohols, of which the intermediates are stabilized by a confined space to afford extra O-Cu bonding. This study underlines the exploitation of structure-dependent electrochemical property to steer the CO2 reduction pathway, as well as a potential generic tactic to target alcohol synthesis by constructing organic/inorganic Cu hybrids.
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