TY - JOUR
T1 - Enhanced Solar-to-Hydrogen Generation with Broadband Epsilon-Near-Zero Nanostructured Photocatalysts
AU - Tian, Yi
AU - García de Arquer, Francisco Pelayo
AU - Dinh, Cao-Thang
AU - Favraud, Gael
AU - Bonifazi, Marcella
AU - Li, Jun
AU - Liu, Min
AU - Zhang, Xixiang
AU - Zheng, Xueli
AU - Kibria, Md. Golam
AU - Hoogland, Sjoerd
AU - Sinton, David
AU - Sargent, Edward H.
AU - Fratalocchi, Andrea
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): OSR-2016-CRG5-2995
Acknowledgements: Y.T. and F.P.G.d.A. contributed equally to this work. For the computer time, the authors used the resources of the KAUST Supercomputing Laboratory and the Redragon cluster of the Primalight group. This work was supported by KAUST (Award No. OSR-2016-CRG5-2995), the Ontario Research Fund-Research Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, and the Connaught Global Challenges program of the University of Toronto.
PY - 2017/5/8
Y1 - 2017/5/8
N2 - The direct conversion of solar energy into fuels or feedstock is an attractive approach to address increasing demand of renewable energy sources. Photocatalytic systems relying on the direct photoexcitation of metals have been explored to this end, a strategy that exploits the decay of plasmonic resonances into hot carriers. An efficient hot carrier generation and collection requires, ideally, their generation to be enclosed within few tens of nanometers at the metal interface, but it is challenging to achieve this across the broadband solar spectrum. Here the authors demonstrate a new photocatalyst for hydrogen evolution based on metal epsilon-near-zero metamaterials. The authors have designed these to achieve broadband strong light confinement at the metal interface across the entire solar spectrum. Using electron energy loss spectroscopy, the authors prove that hot carriers are generated in a broadband fashion within 10 nm in this system. The resulting photocatalyst achieves a hydrogen production rate of 9.5 µmol h-1 cm-2 that exceeds, by a factor of 3.2, that of the best previously reported plasmonic-based photocatalysts for the dissociation of H2 with 50 h stable operation.
AB - The direct conversion of solar energy into fuels or feedstock is an attractive approach to address increasing demand of renewable energy sources. Photocatalytic systems relying on the direct photoexcitation of metals have been explored to this end, a strategy that exploits the decay of plasmonic resonances into hot carriers. An efficient hot carrier generation and collection requires, ideally, their generation to be enclosed within few tens of nanometers at the metal interface, but it is challenging to achieve this across the broadband solar spectrum. Here the authors demonstrate a new photocatalyst for hydrogen evolution based on metal epsilon-near-zero metamaterials. The authors have designed these to achieve broadband strong light confinement at the metal interface across the entire solar spectrum. Using electron energy loss spectroscopy, the authors prove that hot carriers are generated in a broadband fashion within 10 nm in this system. The resulting photocatalyst achieves a hydrogen production rate of 9.5 µmol h-1 cm-2 that exceeds, by a factor of 3.2, that of the best previously reported plasmonic-based photocatalysts for the dissociation of H2 with 50 h stable operation.
UR - http://hdl.handle.net/10754/623488
UR - http://onlinelibrary.wiley.com/doi/10.1002/adma.201701165/full
UR - http://www.scopus.com/inward/record.url?scp=85019020568&partnerID=8YFLogxK
U2 - 10.1002/adma.201701165
DO - 10.1002/adma.201701165
M3 - Article
C2 - 28481018
SN - 0935-9648
VL - 29
SP - 1701165
JO - Advanced Materials
JF - Advanced Materials
IS - 27
ER -