Ultrafast Hole Transfer in Graphitic Carbon Nitride Imide Enabling Efficient H2O2 Photoproduction
Solar-driven photocatalysis is a promising approach for renewable energy application. H2O2 photocatalysis by metal-free graphitic carbon nitride has been gaining attention. Compared with traditional thermal catalysis, metal-free graphitic carbon nitride photocatalysis could lower material cost and achieve greener production of H2O2. Also, to better guide photocatalyst design, a fundamental understanding of the reaction mechanism is needed. Here, we develop a series of model cost-effective metal-free H2O2 photocatalysts made from graphitic carbon nitride (melem) and common imide groups. With 4,4'-oxydiphthalic anhydride (ODPA)-modified g-C3N4, a H2O2 yield rate of 10781 μmol/h·g·L could be achieved. Transient absorption and ex situ Fourier transform infrared (FTIR) measurements revealed an ultrafast charge transfer from the melem core to water with ∼3 ps to form unique N-OH intermediates. The electron withdrawing ability of the anhydride group plays a role in governing the rate of electron transfer, ensuring efficient charge separation. Our strategy represents a new way to achieve a low material cost, simple synthesizing strategy, good environment impact, and high H2O2 production for renewable energy application.
Shenzhen Science and Technology Innovation Commission[JCYJ20220818100212027] ; Science, Technology, and Innovation Commission of Shenzhen under Shenzhen Virtual University Park Special Fund[2021Szvup129]
|WOS Research Area|
Science & Technology - Other Topics ; Materials Science
Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
|WOS Accession No|
Cited Times [WOS]:1
|Document Type||Journal Article|
|Department||Department of Mechanical and Energy Engineering|
1.SUSTech Energy Institute for Carbon Neutrality,Department of Mechanical and Energy Engineering,Southern University of Science and Technology,Shenzhen,518055,China
2.State Key Laboratory of Marine Pollution,Department of Chemistry,City University of Hong Kong,Hong Kong,China
|First Author Affilication||Department of Mechanical and Energy Engineering|
|First Author's First Affilication||Department of Mechanical and Energy Engineering|
Hu，Qiushi,Huang，Yuling,Yu，Xuemeng,et al. Ultrafast Hole Transfer in Graphitic Carbon Nitride Imide Enabling Efficient H2O2 Photoproduction[J]. ACS applied materials & interfaces,2023,15(36):42611-42621.
Hu，Qiushi.,Huang，Yuling.,Yu，Xuemeng.,Gong，Shaokuan.,Wen，Yifan.,...&Chen，Xihan.(2023).Ultrafast Hole Transfer in Graphitic Carbon Nitride Imide Enabling Efficient H2O2 Photoproduction.ACS applied materials & interfaces,15(36),42611-42621.
Hu，Qiushi,et al."Ultrafast Hole Transfer in Graphitic Carbon Nitride Imide Enabling Efficient H2O2 Photoproduction".ACS applied materials & interfaces 15.36(2023):42611-42621.
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