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

Kim, Dohyung; Yu, Sunmoon; Zheng, Fan; Roh, Inwhan; Li, Yifan; Louisia, Sheena; Qi, Zhiyuan; Somorjai, Gabor A.; Frei, Heinz; Wang, Lin-Wang; Yang, Peidong

doi:10.1038/s41560-020-00730-4

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

Journal Article · Mon Nov 30 00:00:00 EST 2020 · Nature Energy

DOI:https://doi.org/10.1038/s41560-020-00730-4· OSTI ID:1786330

^[1]; ^[1]; Zheng, Fan ^[2]; ^[1]; Li, Yifan ^[1]; Louisia, Sheena ^[1]; Qi, Zhiyuan ^[2]; ^[1]; Frei, Heinz ^[2]; ^[2]; ^[3]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)

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. In this article, 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).

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Institutes of Health; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1786330

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 12 Vol. 5; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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