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Title: Surface-modified, dye-sensitized niobate nanosheets enabling an efficient solar-driven Z-scheme for overall water splitting

Abstract

While dye-sensitized metal oxides are good candidates as H2evolution photocatalysts for solar-driven Z-scheme water splitting, their solar-to-hydrogen (STH) energy conversion efficiencies remain low because of uncontrolled charge recombination reactions. Here, we show that modification of Ru dye–sensitized, Pt-intercalated HCa2Nb3O10nanosheets (Ru/Pt/HCa2Nb3O10) with both amorphous Al2O3and poly(styrenesulfonate) (PSS) improves the STH efficiency of Z-scheme overall water splitting by a factor of ~100, when the nanosheets are used in combination with a WO3-based O2evolution photocatalyst and an I3-/I-redox mediator, relative to an analogous system that uses unmodified Ru/Pt/HCa2Nb3O10. By using the optimized photocatalyst, PSS/Ru/Al2O3/Pt/HCa2Nb3O10, a maximum STH of 0.12% and an apparent quantum yield of 4.1% at 420 nm were obtained, by far the highest among dye-sensitized water splitting systems and comparable to conventional semiconductor-based suspended particulate photocatalyst systems.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [2]; ORCiD logo [3]; ORCiD logo [1];  [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Tokyo Institute of Technology (Japan)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States)
  3. National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
  4. Univ. of Pennsylvania, Philadelphia, PA (United States); National Institute for Materials Science (NIMS), Tsukuba (Japan)
Publication Date:
Research Org.:
Univ. of Pennsylvania, Philadelphia, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); Japan Society for the Promotion of Science (JSPS)
OSTI Identifier:
1904316
Grant/Contract Number:  
SC0019781; JP19H02511; JP22H01862; JP22H05148; JP21K20555
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 8; Journal Issue: 32; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Science & Technology

Citation Formats

Nishioka, Shunta, Hojo, Koya, Xiao, Langqiu, Gao, Tianyue, Miseki, Yugo, Yasuda, Shuhei, Yokoi, Toshiyuki, Sayama, Kazuhiro, Mallouk, Thomas E., and Maeda, Kazuhiko. Surface-modified, dye-sensitized niobate nanosheets enabling an efficient solar-driven Z-scheme for overall water splitting. United States: N. p., 2022. Web. doi:10.1126/sciadv.adc9115.
Nishioka, Shunta, Hojo, Koya, Xiao, Langqiu, Gao, Tianyue, Miseki, Yugo, Yasuda, Shuhei, Yokoi, Toshiyuki, Sayama, Kazuhiro, Mallouk, Thomas E., & Maeda, Kazuhiko. Surface-modified, dye-sensitized niobate nanosheets enabling an efficient solar-driven Z-scheme for overall water splitting. United States. https://doi.org/10.1126/sciadv.adc9115
Nishioka, Shunta, Hojo, Koya, Xiao, Langqiu, Gao, Tianyue, Miseki, Yugo, Yasuda, Shuhei, Yokoi, Toshiyuki, Sayama, Kazuhiro, Mallouk, Thomas E., and Maeda, Kazuhiko. Wed . "Surface-modified, dye-sensitized niobate nanosheets enabling an efficient solar-driven Z-scheme for overall water splitting". United States. https://doi.org/10.1126/sciadv.adc9115. https://www.osti.gov/servlets/purl/1904316.
@article{osti_1904316,
title = {Surface-modified, dye-sensitized niobate nanosheets enabling an efficient solar-driven Z-scheme for overall water splitting},
author = {Nishioka, Shunta and Hojo, Koya and Xiao, Langqiu and Gao, Tianyue and Miseki, Yugo and Yasuda, Shuhei and Yokoi, Toshiyuki and Sayama, Kazuhiro and Mallouk, Thomas E. and Maeda, Kazuhiko},
abstractNote = {While dye-sensitized metal oxides are good candidates as H2evolution photocatalysts for solar-driven Z-scheme water splitting, their solar-to-hydrogen (STH) energy conversion efficiencies remain low because of uncontrolled charge recombination reactions. Here, we show that modification of Ru dye–sensitized, Pt-intercalated HCa2Nb3O10nanosheets (Ru/Pt/HCa2Nb3O10) with both amorphous Al2O3and poly(styrenesulfonate) (PSS) improves the STH efficiency of Z-scheme overall water splitting by a factor of ~100, when the nanosheets are used in combination with a WO3-based O2evolution photocatalyst and an I3-/I-redox mediator, relative to an analogous system that uses unmodified Ru/Pt/HCa2Nb3O10. By using the optimized photocatalyst, PSS/Ru/Al2O3/Pt/HCa2Nb3O10, a maximum STH of 0.12% and an apparent quantum yield of 4.1% at 420 nm were obtained, by far the highest among dye-sensitized water splitting systems and comparable to conventional semiconductor-based suspended particulate photocatalyst systems.},
doi = {10.1126/sciadv.adc9115},
journal = {Science Advances},
number = 32,
volume = 8,
place = {United States},
year = {Wed Aug 10 00:00:00 EDT 2022},
month = {Wed Aug 10 00:00:00 EDT 2022}
}

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