Selective CO2 electrocatalysis at the pseudocapacitive nanoparticle/ordered-ligand interlayer

Dohyung Kim, Sunmoon Yu, Fan Zheng, Inwhan Roh, Yifan Li, Sheena Louisia, Zhiyuan Qi, Gabor A. Somorjai, Heinz Frei, Lin-Wang Wang and Peidong Yang ()
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Dohyung Kim: University of California
Sunmoon Yu: University of California
Fan Zheng: Lawrence Berkeley National Laboratory
Inwhan Roh: University of California
Yifan Li: University of California
Sheena Louisia: University of California
Zhiyuan Qi: Lawrence Berkeley National Laboratory
Gabor A. Somorjai: University of California
Heinz Frei: Lawrence Berkeley National Laboratory
Lin-Wang Wang: Lawrence Berkeley National Laboratory
Peidong Yang: University of California

Nature Energy, 2020, vol. 5, issue 12, 1032-1042

Abstract: Abstract Enzymes feature the concerted operation of multiple components around an active site, leading to exquisite catalytic specificity. Realizing such configurations on synthetic catalyst surfaces remains elusive. Here, we report a nanoparticle/ordered-ligand interlayer that contains a multi-component catalytic pocket for high-specificity CO2 electrocatalysis. The nanoparticle/ordered-ligand interlayer comprises a metal nanoparticle surface and a detached layer of ligands in its vicinity. This interlayer possesses unique pseudocapacitive characteristics where desolvated cations are intercalated, creating an active-site configuration that enhances catalytic turnover by two orders and one order of magnitude against a pristine metal surface and nanoparticle with tethered ligands, respectively. The nanoparticle/ordered-ligand interlayer is demonstrated across several metals with up to 99% CO selectivity at marginal overpotentials and onset overpotentials of as low as 27 mV, in aqueous conditions. Furthermore, in a gas-diffusion environment with neutral media, the nanoparticle/ordered-ligand interlayer achieves nearly unit CO selectivity at high current densities (98.1% at 400 mA cm−2).

Date: 2020
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DOI: 10.1038/s41560-020-00730-4

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