Citation: Ping Wang, Haitao Li, Yanjie Cao, Huogen Yu. Carboxyl-Functionalized Graphene for Highly Efficient H₂-Evolution Activity of TiO₂ Photocatalyst[J]. Acta Physico-Chimica Sinica, ;2021, 37(6): 200804. doi: 10.3866/PKU.WHXB202008047 shu

Carboxyl-Functionalized Graphene for Highly Efficient H₂-Evolution Activity of TiO₂ Photocatalyst

Ping Wang ^1,, ,
Haitao Li ¹ ,
Yanjie Cao ¹ ,
Huogen Yu ^{1, 2,,}

1.
School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, China
2.
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China

Corresponding author: Ping Wang, wangping0904@whut.edu.cn Huogen Yu, yuhuogen@whut.edu.cn
Received Date: 17 August 2020
Revised Date: 21 September 2020
Accepted Date: 22 September 2020
Available Online: 28 September 2020
Fund Project: the National Natural Science Foundation of China 21771142the National Natural Science Foundation of China 51872221the Fundamental Research Funds for the Central Universities, China WUT2019IB002

The use of semiconductor photocatalysts (CdS, g-C₃N₄, TiO₂, etc.) to generate hydrogen (H₂) is a prospective strategy that can convert solar energy into hydrogen energy, thereby meeting future energy demands. Among the numerous photocatalysts, TiO₂ has attracted significant attention because of its suitable reduction potential and excellent chemical stability. However, the photoexcited electrons and holes of TiO₂ are easily quenched, leading to limited photocatalytic performance. Furthermore, graphene has been used as an effective electron cocatalyst in the accelerated transport of photoinduced electrons to enhance the H₂-production performance of TiO₂, owing to its excellent conductivity and high charge carrier mobility. For an efficient graphene-based photocatalyst, the rapid transfer of photogenerated electrons is extremely important along with an effectual interfacial H₂-production reaction on the graphene surface. Therefore, it is necessary to further optimize the graphene microstructures (functionalized graphene) to improve the H₂-production performance of graphene-based TiO₂ photocatalysts. The introduction of H₂-evolution active sites onto the graphene surface is an effective strategy for the functionalization of graphene. Compared with the noncovalent functionalization of graphene (such as loading Pt, MoS_x, and CoS_x on the graphene surface), its covalent functionalization can provide a strong interaction between graphene and organic molecules in the form of H₂-evolution active sites that are produced by chemical reactions. In this study, carboxyl-functionalized graphene (rGO-COOH) was successfully modified via ring-opening and esterification reactions on the TiO₂ surface by using an ultrasound-assisted self-assembly method to prepare a high-activity TiO₂/rGO-COOH photocatalyst. The Fourier transform infrared (FTIR) spectra, X-ray photoelectron spectroscopy (XPS), and thermogravimetric (TG) curves revealed the successful covalent functionalization of GO to rGO-COOH by significantly enhanced ―COOH groups in FTIR and increased peak area of carboxyl groups in XPS. A series of characterizations, including X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), XPS, and UV-Vis adsorption spectra, were performed to demonstrate the successful synthesis of TiO₂/rGO-COOH photocatalysts. The experimental data for the hydrogen-evolution rate showed that the TiO₂/rGO-COOH displayed an extremely high hydrogen-generation activity (254.2 μmol∙h⁻¹∙g⁻¹), which was 2.06- and 4.48-fold higher than those of TiO₂/GO and TiO₂, respectively. The enhanced photocatalytic activity of TiO₂/rGO-COOH is ascribed to the carboxyl groups of carboxyl-functionalized graphene, which act as effective hydrogen-generation active sites and enrich hydrogen ions owing to their excellent nucleophilicity that facilitates the interfacial hydrogen production reaction of TiO₂. This study provides novel insights into the development of high-activity graphene-supported photocatalysts in the hydrogen-generation field.
- Carboxyl-functionalized graphene,
- Carboxyl groups,
- TiO₂,
- Photocatalytic H₂ evolution
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Carboxyl-Functionalized Graphene for Highly Efficient H2-Evolution Activity of TiO2 Photocatalyst

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Carboxyl-Functionalized Graphene for Highly Efficient H₂-Evolution Activity of TiO₂ Photocatalyst