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Pb-rich Cu grain boundary sites for selective CO-to-n-propanol electroconversion.
- Source :
- Nature Communications; 8/12/2023, Vol. 14 Issue 1, p1-12, 12p
- Publication Year :
- 2023
-
Abstract
- Electrochemical carbon monoxide (CO) reduction to high-energy-density fuels provides a potential way for chemical production and intermittent energy storage. As a valuable C<subscript>3</subscript> species, n-propanol still suffers from a relatively low Faradaic efficiency (FE), sluggish conversion rate and poor stability. Herein, we introduce an "atomic size misfit" strategy to modulate active sites, and report a facile synthesis of a Pb-doped Cu catalyst with numerous atomic Pb-concentrated grain boundaries. Operando spectroscopy studies demonstrate that these Pb-rich Cu-grain boundary sites exhibit stable low coordination and can achieve a stronger CO adsorption for a higher surface CO coverage. Using this Pb-Cu catalyst, we achieve a CO-to-n-propanol FE (FE<subscript>propanol</subscript>) of 47 ± 3% and a half-cell energy conversion efficiency (EE) of 25% in a flow cell. When applied in a membrane electrode assembly (MEA) device, a stable FE<subscript>propanol</subscript> above 30% and the corresponding full-cell EE of over 16% are maintained for over 100 h with the n-propanol partial current above 300 mA (5 cm<superscript>2</superscript> electrode). Furthermore, operando X-ray absorption spectroscopy and theoretical studies reveal that the structurally-flexible Pb-Cu surface can adaptively stabilize the key intermediates, which strengthens the *CO binding while maintaining the C–C coupling ability, thus promoting the CO-to-n-propanol conversion. CO electroreduction to valuable high-energy content fuels is desired yet improving multicarbon C3 selectivity remains challenging. Here, authors enhance the n-propanol formation on a Cu-based electrocatalyst by introducing Pb atoms into the Cu lattice to induce Pb-rich Cu grain boundary sites. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 20411723
- Volume :
- 14
- Issue :
- 1
- Database :
- Complementary Index
- Journal :
- Nature Communications
- Publication Type :
- Academic Journal
- Accession number :
- 169912977
- Full Text :
- https://doi.org/10.1038/s41467-023-40689-w