Heterointerface Created on Au-Cluster-Loaded Unilamellar Hydroxide Electrocatalysts as a Highly Active Site for the Oxygen Evolution Reaction

Sho Kitano; Tomohiro G Noguchi; Masamichi Nishihara; Kazutaka Kamitani; Takeharu Sugiyama; Satoru Yoshioka; Tetsuya Miwa; Kazunari Yoshizawa; Aleksandar Staykov; Miho Yamauchi

doi:10.1002/adma.202110552

Heterointerface Created on Au-Cluster-Loaded Unilamellar Hydroxide Electrocatalysts as a Highly Active Site for the Oxygen Evolution Reaction

Adv Mater. 2022 Apr;34(16):e2110552. doi: 10.1002/adma.202110552. Epub 2022 Mar 11.

Authors

Sho Kitano^{1

2}, Tomohiro G Noguchi², Masamichi Nishihara³, Kazutaka Kamitani⁴, Takeharu Sugiyama⁴, Satoru Yoshioka⁵, Tetsuya Miwa⁶, Kazunari Yoshizawa^{6

7}, Aleksandar Staykov^{2

8}, Miho Yamauchi^{2

6

8

9}

Affiliations

¹ Division of Applied Chemistry, Faculty of Engineering, Hokkaido University, Kita 13, Nishi 8, Kita-ku, Sapporo, Hokkaido, 060-8628, Japan.
² International Institute for Carbon-Neutral Energy Research (WPI-I 2CNER), Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395, Japan.
³ Next-Generation Fuel Cell Research Center, Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395, Japan.
⁴ Research Center for Synchrotron Light Applications, Kyushu University, 6-1 Kasuga-koen, Kasuga, Fukuoka, 816-8580, Japan.
⁵ Department of Applied Quantum Physics and Nuclear Engineering, Faculty of Engineering, Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395, Japan.
⁶ Institute for Materials Chemistry and Engineering (IMCE), Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395, Japan.
⁷ Integrated Research Consortium on Chemical Science (IRCCS), Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395, Japan.
⁸ Research Center for Negative Emissions Technologies (K-Nets), Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395, Japan.
⁹ Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, 980-8577, Japan.

PMID: 35212064
DOI: 10.1002/adma.202110552

Abstract

The oxygen evolution reaction (OER) is a critical element for all sorts of reactions that use water as a hydrogen source, such as hydrogen evolution and electrochemical CO₂ reduction, and novel design principles that provide highly active sites on OER electrocatalysts push the limits of their practical applications. Herein, Au-cluster loading on unilamellar exfoliated layered double hydroxide (ULDH) electrocatalysts for the OER is demonstrated to fabricate a heterointerface between Au clusters and ULDHs as an active site, which is accompanied by the oxidation state modulation of the active site and interfacial direct OO coupling ("interfacial DOOC"). The Au-cluster-loaded ULDHs exhibit excellent activities for the OER with an overpotential of 189 mV at 10 mA cm^-2 . X-ray absorption fine structure measurements reveal that charge transfer from the Au clusters to ULDHs modifies the oxidation states of trivalent metal ions, which can be active sites on the ULDHs. The present study, supported by highly sensitive spectroscopy combining reflection absorption infrared spectroscopy and modulation-excitation spectroscopy and density functional theory calculations, indicates that active sites at the interface between the Au clusters and ULDHs promote a novel OER mechanism through interfacial DOOC, thereby achieving outstanding catalytic performance.

Keywords: Au clusters; electrochemistry; layered double hydroxides; oxygen evolution reaction.

Abstract

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