TY - JOUR
T1 - Enhanced solar-driven benzaldehyde oxidation with simultaneous hydrogen production on Pt single-atom catalyst
AU - Wang, Lizhuo
AU - Tang, Rui
AU - Kheradmand, Amanj
AU - Jiang, Yijiao
AU - Wang, Hao
AU - Yang, Wenjie
AU - Chen, Zibin
AU - Zhong, Xia
AU - Ringer, Simon P.
AU - Liao, Xiaozhou
AU - Liang, Weibin
AU - Huang, Jun
N1 - Funding Information:
Acknowledge the financial supports from Australian Research Council Discovery Project ( DP180104010 ) and the University of Sydney SOAR fellowship, Sydney Nano Grand Challenge , and the International Project Development Funding. The authors also acknowledge the scientific and technical support from the Microscopy Australia node at the University of Sydney (Sydney Microscopy & Microanalysis) - particularly Dr. Magnus Garbrecht. The technical and scientific support from the team at Sydney Analytical at the University of Sydney are also gratefully acknowledged.
Publisher Copyright:
© 2020 Elsevier B.V.
PY - 2021/5/5
Y1 - 2021/5/5
N2 - Sustainable development requires the use of renewable and clean energy resources to manufacture end-user products with high efficiency. Herein, we report an artificial photocatalysis system that combines the oxidation of the biomass-derived benzaldehyde with simultaneous proton reduction in a closed redox cycle driven by supported nanocatalysts in an aqueous solution. Our results demonstrate a nearly 100 % reactant efficiency for water splitting on a per-atom basis, and generates two targeted end-user products: benzoic acid and clean H2 fuel. Nanocatalysts can be conveniently categorized into three groups according to their size: single atom, nanocluster, and nanoparticle. Nanocatalysts smaller in size are generally outstanding for oxidation, while larger particles are more efficient in proton reduction. To elucidate the size effects for the overall reaction in both half-reactions, we prepared Pt single atom (0.2 nm), nanocluster (1 nm), and nanoparticle (4 and 7 nm diameter) catalysts supported on polymeric carbon nitride (g-C3N4) for the artificial photocatalytic oxidation of benzaldehyde and hydrogen production. The reaction rate for both benzaldehyde oxidation and H2 production on the Pt nanocatalysts follows the order of single atom > nanocluster > nanoparticle. Photon-induced charge carriers are more likely to be trapped by single Pt atoms, which guarantees the efficiency of charge splitting and limits the recombination. In addition, the outstanding oxidation performance of the single atom and nanocluster catalysts consumes large amount of holes, which otherwise contribute more electrons for proton reduction and enhance H2 production. On the other hand, the large nanoparticles potentially provide a stage to trap both photo-induced electrons and holes, with the potential to reduce the photocatalysis rate of hydrogen production from the proton reduction via the excess electrons and the benzaldehyde oxidation and the excess holes.
AB - Sustainable development requires the use of renewable and clean energy resources to manufacture end-user products with high efficiency. Herein, we report an artificial photocatalysis system that combines the oxidation of the biomass-derived benzaldehyde with simultaneous proton reduction in a closed redox cycle driven by supported nanocatalysts in an aqueous solution. Our results demonstrate a nearly 100 % reactant efficiency for water splitting on a per-atom basis, and generates two targeted end-user products: benzoic acid and clean H2 fuel. Nanocatalysts can be conveniently categorized into three groups according to their size: single atom, nanocluster, and nanoparticle. Nanocatalysts smaller in size are generally outstanding for oxidation, while larger particles are more efficient in proton reduction. To elucidate the size effects for the overall reaction in both half-reactions, we prepared Pt single atom (0.2 nm), nanocluster (1 nm), and nanoparticle (4 and 7 nm diameter) catalysts supported on polymeric carbon nitride (g-C3N4) for the artificial photocatalytic oxidation of benzaldehyde and hydrogen production. The reaction rate for both benzaldehyde oxidation and H2 production on the Pt nanocatalysts follows the order of single atom > nanocluster > nanoparticle. Photon-induced charge carriers are more likely to be trapped by single Pt atoms, which guarantees the efficiency of charge splitting and limits the recombination. In addition, the outstanding oxidation performance of the single atom and nanocluster catalysts consumes large amount of holes, which otherwise contribute more electrons for proton reduction and enhance H2 production. On the other hand, the large nanoparticles potentially provide a stage to trap both photo-induced electrons and holes, with the potential to reduce the photocatalysis rate of hydrogen production from the proton reduction via the excess electrons and the benzaldehyde oxidation and the excess holes.
KW - Benzaldehyde oxidation
KW - Hydrogen production
KW - Photocatalysis
KW - Pt single atom
KW - Size effects
UR - http://www.scopus.com/inward/record.url?scp=85097889690&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2020.119759
DO - 10.1016/j.apcatb.2020.119759
M3 - Journal article
AN - SCOPUS:85097889690
SN - 0926-3373
VL - 284
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 119759
ER -
