Ag(I) ions working as a hole-transfer mediator in photoelectrocatalytic water oxidation on WO3 film

Tae Hwa Jeon; Damián Monllor–Satoca; Gun–hee –H Moon; Wooyul Kim; Hyoung–il –I Kim; Detlef W. Bahnemann; Hyunwoong Park; Wonyong Choi

doi:10.1038/s41467-020-14775-2

Ag(I) ions working as a hole-transfer mediator in photoelectrocatalytic water oxidation on WO₃ film

Tae Hwa Jeon
, Damián Monllor–Satoca
, Gun–hee –H Moon
, Wooyul Kim
, Hyoung–il –I Kim
, Detlef W. Bahnemann
, Hyunwoong Park
, Wonyong Choi

School of Energy Engineering

Pohang University of Science and Technology
Ramon Llull University
Sookmyung Women's University
Yonsei University
Leibniz University Hannover

Research output: Contribution to journal › Article › peer-review

105 Scopus citations

Abstract

Ag(I) is commonly employed as an electron scavenger to promote water oxidation. In addition to its straightforward role as an electron acceptor, Ag(I) can also capture holes to generate the high-valent silver species. Herein, we demonstrate photoelectrocatalytic (PEC) water oxidation and concurrent dioxygen evolution by the silver redox cycle where Ag(I) acts as a hole-transfer mediator. Ag(I) enhances the PEC performance of WO₃ electrodes at 1.23 V vs. RHE with increasing O₂ evolution, while forming Ag(II) complexes (Ag^IINO₃ ⁺). Upon turning off both light and potential bias, the photocurrent immediately drops to zero, whereas O₂ evolution continues over ~10 h with gradual bleaching of the colored complexes. This phenomenon is observed neither in the Ag(I)-free PEC reactions nor in the photocatalytic (i.e., bias-free) reactions with Ag(I). This study finds that the role of Ag(I) is not limited as an electron scavenger and calls for more thorough studies on the effect of Ag(I).

Original language	English
Article number	967
Journal	Nature Communications
Volume	11
Issue number	1
DOIs	https://doi.org/10.1038/s41467-020-14775-2
State	Published - 1 Dec 2020

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title = "Ag(I) ions working as a hole-transfer mediator in photoelectrocatalytic water oxidation on WO3 film",

abstract = "Ag(I) is commonly employed as an electron scavenger to promote water oxidation. In addition to its straightforward role as an electron acceptor, Ag(I) can also capture holes to generate the high-valent silver species. Herein, we demonstrate photoelectrocatalytic (PEC) water oxidation and concurrent dioxygen evolution by the silver redox cycle where Ag(I) acts as a hole-transfer mediator. Ag(I) enhances the PEC performance of WO3 electrodes at 1.23 V vs. RHE with increasing O2 evolution, while forming Ag(II) complexes (AgIINO3 +). Upon turning off both light and potential bias, the photocurrent immediately drops to zero, whereas O2 evolution continues over \textasciitilde{}10 h with gradual bleaching of the colored complexes. This phenomenon is observed neither in the Ag(I)-free PEC reactions nor in the photocatalytic (i.e., bias-free) reactions with Ag(I). This study finds that the role of Ag(I) is not limited as an electron scavenger and calls for more thorough studies on the effect of Ag(I).",

author = "Jeon, \{Tae Hwa\} and Dami{\'a}n Monllor–Satoca and Moon, \{Gun–hee –H\} and Wooyul Kim and Kim, \{Hyoung–il –I\} and Bahnemann, \{Detlef W.\} and Hyunwoong Park and Wonyong Choi",

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T1 - Ag(I) ions working as a hole-transfer mediator in photoelectrocatalytic water oxidation on WO3 film

AU - Jeon, Tae Hwa

AU - Monllor–Satoca, Damián

AU - Moon, Gun–hee –H

AU - Kim, Wooyul

AU - Kim, Hyoung–il –I

AU - Bahnemann, Detlef W.

AU - Park, Hyunwoong

AU - Choi, Wonyong

PY - 2020/12/1

Y1 - 2020/12/1

N2 - Ag(I) is commonly employed as an electron scavenger to promote water oxidation. In addition to its straightforward role as an electron acceptor, Ag(I) can also capture holes to generate the high-valent silver species. Herein, we demonstrate photoelectrocatalytic (PEC) water oxidation and concurrent dioxygen evolution by the silver redox cycle where Ag(I) acts as a hole-transfer mediator. Ag(I) enhances the PEC performance of WO3 electrodes at 1.23 V vs. RHE with increasing O2 evolution, while forming Ag(II) complexes (AgIINO3 +). Upon turning off both light and potential bias, the photocurrent immediately drops to zero, whereas O2 evolution continues over ~10 h with gradual bleaching of the colored complexes. This phenomenon is observed neither in the Ag(I)-free PEC reactions nor in the photocatalytic (i.e., bias-free) reactions with Ag(I). This study finds that the role of Ag(I) is not limited as an electron scavenger and calls for more thorough studies on the effect of Ag(I).

AB - Ag(I) is commonly employed as an electron scavenger to promote water oxidation. In addition to its straightforward role as an electron acceptor, Ag(I) can also capture holes to generate the high-valent silver species. Herein, we demonstrate photoelectrocatalytic (PEC) water oxidation and concurrent dioxygen evolution by the silver redox cycle where Ag(I) acts as a hole-transfer mediator. Ag(I) enhances the PEC performance of WO3 electrodes at 1.23 V vs. RHE with increasing O2 evolution, while forming Ag(II) complexes (AgIINO3 +). Upon turning off both light and potential bias, the photocurrent immediately drops to zero, whereas O2 evolution continues over ~10 h with gradual bleaching of the colored complexes. This phenomenon is observed neither in the Ag(I)-free PEC reactions nor in the photocatalytic (i.e., bias-free) reactions with Ag(I). This study finds that the role of Ag(I) is not limited as an electron scavenger and calls for more thorough studies on the effect of Ag(I).

UR - https://www.scopus.com/pages/publications/85079803212

U2 - 10.1038/s41467-020-14775-2

DO - 10.1038/s41467-020-14775-2

M3 - Article

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AN - SCOPUS:85079803212

SN - 2041-1723

VL - 11

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 967

ER -

Ag(I) ions working as a hole-transfer mediator in photoelectrocatalytic water oxidation on WO₃ film

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