Citation: Jiawei Hu, Kai Xia, Ao Yang, Zhihao Zhang, Wen Xiao, Chao Liu, Qinfang Zhang. Interfacial Engineering of Ultrathin 2D/2D NiPS₃/C₃N₅ Heterojunctions for Boosting Photocatalytic H₂ Evolution[J]. Acta Physico-Chimica Sinica, ;2024, 40(5): 230504. doi: 10.3866/PKU.WHXB202305043 shu

Interfacial Engineering of Ultrathin 2D/2D NiPS₃/C₃N₅ Heterojunctions for Boosting Photocatalytic H₂ Evolution

Jiawei Hu ¹ ,
Kai Xia ¹ ,
Ao Yang ¹ ,
Zhihao Zhang ¹ ,
Wen Xiao ¹ ,
Chao Liu ^{1, 2,,} ,
Qinfang Zhang ^1,,

1.
School of Materials Science and Engineering, Yancheng Institute of Technology, Yancheng 224051, Jiangsu Province, China
2.
Jiangsu Provincial Key Laboratory of Eco-Environmental Materials, Yancheng Institute of Technology, Yancheng 224051, Jiangsu Province, China

Corresponding author: Chao Liu, cliu@ycit.edu.cn Qinfang Zhang, qfangzhang@gmail.com
Received Date: 22 May 2023
Revised Date: 12 July 2023
Accepted Date: 12 July 2023
Available Online: 19 July 2023
Fund Project: the National Natural Science Foundation of China 51902282the National Natural Science Foundation of China 12274361Natural Science Foundation of Jiangsu Province, China BK20211361College Natural Science Research Project of Jiangsu Province, China 20KJA430004

This study focuses on exploring efficient photocatalysts for water splitting, which holds great potential for harnessing hydrogen (H₂) as a renewable energy source. Modulating the heterojunction interface is known to enhance charge carrier separation and solar energy utilization, thereby boosting photocatalytic activity. In this work, a mechanical mixing-assisted self-assembly approach was developed to construct a heterojunction between NiPS₃ (NPS) nanosheets (NSs) and C₃N₅ (CN) NSs. Specifically, two-dimensional (2D) NPS NSs were tightly deposited on 2D CN NSs surface to gain a 2D/2D heterostructure. The photocatalytic performance of the synthesized photocatalysts was determined by their ability to generate H₂ through water splitting, both in deionized (DI) water and seawater, under visible light. The resulting NPS NSs/CN NSs (NPS/CN) composites possessed boosted photocatalytic hydrogen evolution (PHE) activity related to CN NSs and NPS NSs. This improvement was assigned to the synergistic effect of increased light-harvesting capacity and heterojunction formation. Nevertheless, an excessive amount of deposited NPS NSs on the surface of CN NSs was found to reduce the light absorption of the CN NSs component in the NPS/CN composites, resulting in decreased PHE activity. Therefore, it was determined that an appropriate mass ratio between the two components is necessary to achieve excellent photocatalytic activity for the NPS/CN composites. The optimized photocatalyst, referred to as 3-NPS/CN, demonstrated the highest visible-light-driven PHE efficiency of 47.71 μmol∙h⁻¹, which was 2385.50 times higher than that of CN NSs. Moreover, 3-NPS/CN also exhibited excellent PHE activity in seawater, with a rate of 8.99 μmol∙h⁻¹. The photoelectrochemical, steady-state photoluminescence (PL), time-resolved PL (TR-PL), steady-state surface photovoltage (SPV) and time-resolved surface photovoltage (TPV) techniques were performed to investigate the charge separation and migration behaviors of various photocatalysts. Based on the characterization results, our group proposed a reasonable PHE mechanism. In the NPS/CN photocatalysts, photo-induced electrons rapidly migrated from the conduction band (CB) of CN NSs to the CB of NPS NSs due to the potential difference and strong interfacial electronic coupling between the two materials. The photogenerated electrons accumulated on the CB of the NPS NSs component efficiently reduced protons to generate H₂ molecules. Concurrently, photogenerated holes on the valence band (VB) of CN NSs and NPS NSs were consumed with the assistance of triethanolamine (TEOA) molecules. This study presents a facile method for fabricating 2D/2D heterostructured photocatalysts, which hold promise for efficient and robust implementation in energy applications.
- C₃N₅ nanosheets,
- NiPS₃ nanosheets,
- Photocatalysis,
- Hydrogen production,
- Heterojunction
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Interfacial Engineering of Ultrathin 2D/2D NiPS3/C3N5 Heterojunctions for Boosting Photocatalytic H2 Evolution

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通讯作者: 陈斌, bchen63@163.com

Interfacial Engineering of Ultrathin 2D/2D NiPS₃/C₃N₅ Heterojunctions for Boosting Photocatalytic H₂ Evolution