Citation: Xiaoyan Cai, Jiahao Du, Guangming Zhong, Yiming Zhang, Liang Mao, Zaizhu Lou. Constructing a CeO₂/Zn_xCd_1−xIn₂S₄ S-Scheme Hollow Heterostructure for Efficient Photocatalytic H₂ Evolution[J]. Acta Physico-Chimica Sinica, ;2023, 39(11): 230201. doi: 10.3866/PKU.WHXB202302017 shu

Constructing a CeO₂/Zn_xCd_1−xIn₂S₄ S-Scheme Hollow Heterostructure for Efficient Photocatalytic H₂ Evolution

Xiaoyan Cai ^{1, 2, 3} ,
Jiahao Du ² ,
Guangming Zhong ² ,
Yiming Zhang ² ,
Liang Mao ^2,, ,
Zaizhu Lou ^4,,

1.
School of Safety Engineering, China University of Mining and Technology, Xuzhou 221116, Jiangsu Province, China
2.
School of Materials Science and Physics, China University of Mining and Technology, Xuzhou 221116, Jiangsu Province, China
3.
Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization, China University of Mining and Technology, Xuzhou 221008, Jiangsu Province, China
4.
Guangdong Provincial Key Laboratory of Nanophotonic Manipulation, Institute of Nanophotonics, Jinan University, Guangzhou 511443, China

Corresponding author: Liang Mao, maoliang@cumt.edu.cn Zaizhu Lou, zzlou@jnu.edu.cn
Received Date: 13 February 2023
Revised Date: 16 March 2023
Accepted Date: 17 March 2023
Available Online: 23 March 2023
Fund Project: the National Natural Science Foundation of China 22209203the National Natural Science Foundation of China 22175076the China Postdoctoral Science Foundation 2021M693419the Pengcheng Shangxue Education Fund of Jiangsu Key Laboratory of Coal-Based Greenhouse Gas Control and Utilization PCSX202202the Material Science and Engineering Discipline Guidance Fund of China University of Mining and Technology CUMTMS202202the Material Science and Engineering Discipline Guidance Fund of China University of Mining and Technology CUMTMS202207the Undergraduate Training Program for Innovation and Entrepreneurship of China University of Mining and Technology 202210290200Y

With the exhaustion of fossil energy, the energy crisis is becoming increasingly serious, which greatly hinders the sustainable development of society. Therefore, the development of new energy technologies as a substitute for non-renewable and highly polluting fossil energy is extremely urgent. The environmental benefits and high energy density of hydrogen (H₂) make it an ideal clean energy source. Photocatalytic water splitting, which was first demonstrated in the pioneering work on TiO₂ photoelectrodes under UV-light irradiation, has been extensively researched and has been shown to be an effective method for addressing the global energy crisis. However, most of the photocatalysts used for H₂ production still suffer from low solar energy utilization and fast photogenerated charge recombination, which seriously limit their practical applications in the field of solar-to-hydrogen energy conversion. Therefore, it is necessary yet greatly challenging to develop a visible-light-responsive photocatalyst with efficient photogenerated charge separation through reasonable modification strategy. Layered structured ZnIn₂S₄ (ZIS) is a promising photocatalyst to split water for H₂ evolution owing to its suitable electronic structure, strong light absorption, chemical stability, and low toxicity. However, its low charge separation efficiency renders its photocatalytic performance unsatisfactory. Herein, to overcome this issue, a band structure regulation strategy that integrates solid solution formation with heterostructure construction was proposed. By growing Zn_xCd_1−xIn₂S₄ (ZCIS) nanosheets on the surface of CeO₂ hollow spheres in situ, a novel hollow heterostructure CeO₂/ZCIS with efficient charge separation was constructed as photocatalyst for H₂ generation. The introduction of the Cd cation in ZIS upshifts the conduction band (CB) and valence band (VB) of ZCIS, enhancing the built-in electrical field on the interface. Those electronic band changes induce the S-scheme structure in CeO₂/ZCIS, promoting charge separation for photocatalysis. Moreover, the upshift of the CB generates photoelectrons with high H₂ generation ability. As a result, the optimal 1:6-CeO₂/Zn_0.9Cd_0.1In₂S₄ heterostructure exhibits 4.09 mmol·g⁻¹·h⁻¹ H₂ generation during photocatalysis, which is 6.8-, 3.0-, and 2.2-fold as those of ZIS, ZCIS, and CeO₂/ZIS, respectively. This work provides one efficient strategy to develop highly active S-scheme photocatalysts for hydrogen generation.
- Photocatalysis,
- Hydrogen generation,
- S-scheme heterostructure,
- Build-in electrical field,
- Charge separation
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Constructing a CeO₂/Zn_xCd_1−xIn₂S₄ S-Scheme Hollow Heterostructure for Efficient Photocatalytic H₂ Evolution