TY - JOUR
T1 - Two-Dimensional Metal-Organic Framework Acts as a Hydrogen Evolution Cocatalyst for Overall Photocatalytic Water Splitting
AU - Guan, Jingyan
AU - Pal, Tigmansu
AU - Kamiya, Kazuhide
AU - Fukui, Naoya
AU - Maeda, Hiroaki
AU - Sato, Tetsu
AU - Suzuki, Hajime
AU - Tomita, Osamu
AU - Nishihara, Hiroshi
AU - Abe, Ryu
AU - Sakamoto, Ryota
N1 - Funding Information:
This work was supported by JST-FOREST (JPMJFR203F), JST-CREST (JPMJCR18R3; JPMJCR15F2), JSPS KAKENHI under grant nos. 19H05460, 21H00395, 20H02547, 18KK0395, 20H02568, Chubei Ito Foundation, Kondo Zaidan, Nippon Sheet Glass Foundation for Materials Science and Engineering, the Asahi Glass Foundation, and SEI Group CSR Foundation. This work was partly achieved through the use of SQUID at the Cybermedia Center, Osaka University. The X-ray absorption experiments were performed at the BL01B1 beamline with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (Proposal No. 2021A1489).
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/4/1
Y1 - 2022/4/1
N2 - Water-splitting semiconductor photocatalysts require hydrogen evolution reaction (HER) cocatalysts, the majority of which are robust metals and metal oxides. Metal complexes feature designability and reaction selectivity. This feature should be appreciated in the application as HER cocatalysts by suppressing unfavorable back reactions; however, low stability hampers their application. In this research, we demonstrate that a fully π-conjugated and conductive two-dimensional metal-organic framework (2D MOF), which possesses both virtues of metals/metal oxides and metal complexes, serves as an ideal HER cocatalyst candidate. NiBHT, a kind of 2D MOF, is deposited on the photocatalyst SrTiO3:Al with CoOxas an oxygen evolution cocatalyst to show long-term overall one-step water splitting with an apparent quantum efficiency (AQE) of 6.5% at 350 nm. In comparison to Pt as a representative HER cocatalyst, NiBHT turns out to be a suppressor of back reactions related to oxygen reduction reactions, which is proven both experimentally and theoretically.
AB - Water-splitting semiconductor photocatalysts require hydrogen evolution reaction (HER) cocatalysts, the majority of which are robust metals and metal oxides. Metal complexes feature designability and reaction selectivity. This feature should be appreciated in the application as HER cocatalysts by suppressing unfavorable back reactions; however, low stability hampers their application. In this research, we demonstrate that a fully π-conjugated and conductive two-dimensional metal-organic framework (2D MOF), which possesses both virtues of metals/metal oxides and metal complexes, serves as an ideal HER cocatalyst candidate. NiBHT, a kind of 2D MOF, is deposited on the photocatalyst SrTiO3:Al with CoOxas an oxygen evolution cocatalyst to show long-term overall one-step water splitting with an apparent quantum efficiency (AQE) of 6.5% at 350 nm. In comparison to Pt as a representative HER cocatalyst, NiBHT turns out to be a suppressor of back reactions related to oxygen reduction reactions, which is proven both experimentally and theoretically.
KW - back-reaction regulation
KW - hydrogen evolution reaction cocatalysts
KW - metal-organic frameworks
KW - non-noble metals
KW - particulate photocatalyst water-splitting
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U2 - 10.1021/acscatal.1c05889
DO - 10.1021/acscatal.1c05889
M3 - Article
AN - SCOPUS:85127206769
SN - 2155-5435
VL - 12
SP - 3881
EP - 3889
JO - ACS Catalysis
JF - ACS Catalysis
IS - 7
ER -