Ultrafast Hole Transfer in Graphitic Carbon Nitride Imide Enabling Efficient H2O2 Photoproduction

Hu，Qiushi1,2; Huang，Yuling1; Yu，Xuemeng1; Gong，Shaokuan1; Wen，Yifan1; Liu，Yong2; Li，Geng2; Zhang，Qiang2; Ye，Ruquan2; Chen，Xihan1

2023-09-13

10.1021/acsami.3c08466

ACS applied materials & interfaces   Impact Factor & Quartile

1944-8244

1944-8252

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.

charge transfer mechanism graphitic carbon nitride hydrogen peroxide metal-free photocatalysis ultrafast spectroscopy

SCI

English

First

Shenzhen Science and Technology Innovation Commission[JCYJ20220818100212027] ; Science, Technology, and Innovation Commission of Shenzhen under Shenzhen Virtual University Park Special Fund[2021Szvup129]

Science & Technology - Other Topics ; Materials Science

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:001066777800001

AMER CHEMICAL SOC

2-s2.0-85171202454

Scopus

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

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.