Citation: Zhao Lu, Hu Lv, Qinzhuang Liu, Zhongliao Wang. Modulating NH₂ Lewis Basicity in CTF-NH₂ through Donor-Acceptor Groups for Optimizing Photocatalytic Water Splitting[J]. Acta Physico-Chimica Sinica, ;2024, 40(12): 240500. doi: 10.3866/PKU.WHXB202405005 shu

Modulating NH₂ Lewis Basicity in CTF-NH₂ through Donor-Acceptor Groups for Optimizing Photocatalytic Water Splitting

Zhao Lu ¹ ,
Hu Lv ² ,
Qinzhuang Liu ³ ,
Zhongliao Wang ^3,,

1.
HKUST Shenzhen-Hong Kong Collaborative Innovation Research Institute, Shenzhen 518000, Guangdong Province, China
2.
School of Construction Engineering, Shenzhen Polytechnic University, Shenzhen 518000, Guangdong Province, China
3.
Anhui Province Industrial Generic Technology Research Center for Alumics Materials, Anhui Province Key Laboratory of Pollutant Sensitive Materials and Environmental Remediation, School of Physics and Electronic Information, Huaibei Normal University, Huaibei 235000, Anhui Province, China

Corresponding author: Zhongliao Wang, wangzl@chnu.edu.cn
Received Date: 7 May 2024
Revised Date: 27 May 2024
Accepted Date: 28 May 2024
Available Online: 4 June 2024
Fund Project: the Project of Hetao Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone HZQB-KCZYB-2020083Shenzhen Science and Technology Program KCXFZ20211020163816023Shenzhen Zhongdi Construction Engineering Co., Ltd. cooperation project 22100245Key Research Project in Natural Sciences for Higher Education Institutions by the Ministry of Education 2022AH050396

Photocatalytic water splitting (PWS) provides an optimal approach for the sustainable production of green hydrogen. NH₂-modified covalent triazine frameworks (CTFs-NH₂) hold potential in PWS due to robust light uptake, optimal charge separation, and considerable redox potential. However, the high surface reaction barriers hinder the efficiency of PWS owing to the conversion difficulty of intermediate products. Modulating the Lewis basicity of NH₂ on CTFs offers a feasible route for addressing this challenge. In this work, electron-donating ethyl (C₂H₅) and electron-withdrawing 5-fluoroethyl groups (C₂F₅) are introduced at the para position of amine groups, producing C₂H₅-CTF-NH₂ and C₂F₅-CTF-NH₂, to adjust the Lewis basicity of CTF-NH₂. Through DFT calculations, the optical properties, excited states, electronic structures, dipole moments, and surface reaction processes of the CTF-NH₂, C₂H₅-CTF-NH₂ and C₂F₅-CTF-NH₂ are simulated. The results indicate that the electron-withdrawing C₂F₅ group can decrease the electron density and Lewis basicity on NH₂, thereby lowering the energy barriers for hydrogen and oxygen evolution reactions, effectively ameliorating the PWS efficiency of CTF-NH₂. This work unveils an innovative approach for donor-acceptor-regulated CTFs for the application of PWS.
- Donor,
- Acceptor,
- Water splitting,
- CTFs,
- Lewis basicity
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Modulating NH₂ Lewis Basicity in CTF-NH₂ through Donor-Acceptor Groups for Optimizing Photocatalytic Water Splitting