Citation: Kezhen Lai, Fengyan Li, Ning Li, Yangqin Gao, Lei Ge. Identification of Charge Transfer Pathways in Metal-Organic Framework- Derived Ni-CNT/ZnIn₂S₄ Heterojunctions for Photocatalytic Hydrogen Evolution[J]. Acta Physico-Chimica Sinica, ;2024, 40(1): 230401. doi: 10.3866/PKU.WHXB202304018 shu

Identification of Charge Transfer Pathways in Metal-Organic Framework- Derived Ni-CNT/ZnIn₂S₄ Heterojunctions for Photocatalytic Hydrogen Evolution

Kezhen Lai ^{1, 2} ,
Fengyan Li ^{1, 2} ,
Ning Li ^{1, 2} ,
Yangqin Gao ^{1, 2} ,
Lei Ge ^{1, 2,,}

1.
State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, China University of Petroleum Beijing, Beijing 102249, China
2.
Department of Materials Science and Engineering, College of New Energy and Materials, China University of Petroleum Beijing, Beijing 102249, China

Corresponding author: Lei Ge, gelei@cup.edu.cn
Received Date: 6 April 2023
Revised Date: 20 May 2023
Accepted Date: 22 May 2023
Available Online: 31 May 2023
Fund Project: the National Key R & D Program of China 2021YFA1501300the National Key R & D Program of China 2019YFC1907602National Natural Science Foundation of China 51572295National Natural Science Foundation of China 21273285National Natural Science Foundation of China 21003157

Hydrogen is an important zero-pollution green energy source with potential for alleviating environmental contamination and energy shortages. Hydrogen evolution via solar-energy-induced semiconducting water splitting is among the most environmentally friendly methods available to date. In this study, a metal–organic-framework-derived, Ni-decorated carbon nanotube (Ni-CNT) is used as a non-noble co-catalyst. This Ni-CNT is grown in situ on ZnIn₂S₄ nanosheets using a simple one-step oil bath strategy, wherein Ni nanoparticles are wrapped around the top and cross sections of the nanotubes, preventing their agglomeration. Notably, Ni-CNT/ZnIn₂S₄ heterostructures feature intimate contact interfaces that promote charge transfer, facilitating their use as efficient photocatalysts for hydrogen evolution. The 38Ni-CNT/ZnIn₂S₄ sample exhibits a high H₂ production rate (12267 μmol·h⁻¹·g⁻¹), with an apparent quantum efficiency (AQE) of 11.3% under 420 nm monochromatic light irradiation, which is nearly 6.4 times that of pure ZnIn₂S₄. The results of X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) corroborate the observations on Ni-CNT/ZnIn₂S₄ heterostructures. Electrochemical measurements reveal that the combination of the Ni-CNT and ZnIn₂S₄ facilitates the transfer of photogenerated electrons and effectively prevents rapid recombination of photocarriers, thus improving the hydrogen evolution performance of ZnIn₂S₄. Electron spin resonance (ESR) results further prove that co-catalyst Ni-CNTs are beneficial for prolonging the lifetimes of ZnIn₂S₄ photogenerated electrons, thereby achieving effective charge separation. A charge transfer pathway in the heterojunction interfaces is further explored and confirmed by density functional theory (DFT) calculations. The difference in the Fermi level energy (E_f) contributes to both charge migration and the generation of a built-in electronic field (BEF), indicating that the energy band of ZnIn₂S₄ bends downward, which is favorable for photogenerated electron flow from ZnIn₂S₄ to the Ni-CNT electron acceptor. The results of planar-averaged electron density difference analysis confirm that the hot electrons are transferred from Ni nanoparticles to the CNT and then to the ZnIn₂S₄ nanosheets, indicating the formation of a photogenerated electron transfer pathway of ZnIn₂S₄ → CNT → Ni. Furthermore, Gibbs free energy of H* adsorption (ΔG_H*) and crystal orbital Hamilton population (COHP) analysis indicate that Ni nanoparticles can serve as active sites, promoting H₂ evolution. Thus, the present study formulates a new strategy for developing low-cost, high-efficiency, non-noble-metal co-catalysts for photocatalytic hydrogen production.
- Ni-CNT,
- Photocatalysis,
- H₂ evolution,
- ZnIn₂S₄,
- Co-catalysts
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Identification of Charge Transfer Pathways in Metal-Organic Framework- Derived Ni-CNT/ZnIn2S4 Heterojunctions for Photocatalytic Hydrogen Evolution

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Identification of Charge Transfer Pathways in Metal-Organic Framework- Derived Ni-CNT/ZnIn₂S₄ Heterojunctions for Photocatalytic Hydrogen Evolution