Efficient upgrading of CO to C<sub>3</sub> fuel using asymmetric C-C coupling active sites.

Wang, Xue; Wang, Ziyun; Zhuang, Tao-Tao; Dinh, Cao-Thang; Li, Jun; Nam, Dae-Hyun; Li, Fengwang; Huang, Chun-Wei et al. · Nat Commun · 2019

basic_science · Level V

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Abstract

The electroreduction of C<sub>1</sub> feedgas to high-energy-density fuels provides an attractive avenue to the storage of renewable electricity. Much progress has been made to improve selectivity to C<sub>1</sub> and C<sub>2</sub> products, however, the selectivity to desirable high-energy-density C<sub>3</sub> products remains relatively low. We reason that C<sub>3</sub> electrosynthesis relies on a higher-order reaction pathway that requires the formation of multiple carbon-carbon (C-C) bonds, and thus pursue a strategy explicitly designed to couple C<sub>2</sub> with C<sub>1</sub> intermediates. We develop an approach wherein neighboring copper atoms having distinct electronic structures interact with two adsorbates to catalyze an asymmetric reaction. We achieve a record n-propanol Faradaic efficiency (FE) of (33 ± 1)% with a conversion rate of (4.5 ± 0.1) mA cm<sup>-2</sup>, and a record n-propanol cathodic energy conversion efficiency (EE<sub>cathodic half-cell</sub>) of 21%. The FE and EE<sub>cathodic half-cell</sub> represent a 1.3× improvement relative to previously-published CO-to-n-propanol electroreduction reports.