通过供体-受体基团调节CTF-NH<sub>2</sub>中NH<sub>2</sub>的Lewis碱性优化光催化水分解性能

引用本文: 陆钊, 吕虎, 刘亲壮, 王中辽. 通过供体-受体基团调节CTF-NH₂中NH₂的Lewis碱性优化光催化水分解性能[J]. 物理化学学报, 2024, 40(12): 240500. doi: 10.3866/PKU.WHXB202405005 shu

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

通过供体-受体基团调节CTF-NH₂中NH₂的Lewis碱性优化光催化水分解性能

陆钊 ^1, ,
吕虎 ^2, ,
刘亲壮 ^3, ,
王中辽 ^{3,
,}

1.
香港科技大学深港协同创新研究院, 广东深圳 518000;
2.
深圳职业技术大学建筑工程学院, 广东深圳 518000;
3.
淮北师范大学物理与电子信息学院, 安徽省陶铝新材料产业共性技术研究中心, 安徽省污染物敏感材料与环境修复重点实验室, 安徽淮北 235000

通讯作者: 王中辽,Email:wangzl@chnu.edu.cn

基金项目:
河套深港科技创新合作区项目(HZQB-KCZYB-2020083),深圳市科技计划项目(KCXFZ20211020163816023),深圳市中地建设工程有限公司合作项目(22100245),教育部高等学校自然科学重点研究项目(2022AH050396)资助

摘要: 光催化水分解(PWS)为可持续生产绿色氢气提供了最佳方法。NH₂修饰的共价三嗪框架(CTF-NH₂)由于其强大的光吸收能力、最佳的电荷分离能力和相当大的氧化还原电位，在PWS中具有潜力。然而，由于中间产物的转化困难，高表面反应势垒阻碍了PWS的效率。调节CTF上NH₂的路易斯碱性为解决这一挑战提供了一条可行的途径。本工作在胺基的对位引入给电子乙基(C₂H₅)和吸电子5氟乙基(C₂F₅)，生成C₂H₅-CTF-NH₂和C₂F₅-CTF-NH₂，以调节路易斯碱性CTF-NH₂。通过DFT计算，模拟了CTF-NH₂、C₂H₅-CTF-NH₂和C₂F₅-CTF-NH₂的光学性质、激发态、电子结构、偶极矩和表面反应过程。结果表明，吸电子C₂F₅基团可以降低NH₂上的电子密度和路易斯碱性，从而降低析氢析氧反应的能垒，有效提高CTF-NH₂的PWS效率。这项工作揭示了一种用于PWS应用的供体-受体调控CTF的创新方法。

关键词:

给体
/ 受体
/ 水分解
/ CTF
/ 路易斯碱性

English

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

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: 07 May 2024
Accepted Date: 28 May 2024
Revised Date: 27 May 2024
Available Online: 04 June 2024
Fund Project:
This work was supported by the Project of Hetao Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone (HZQB-KCZYB-2020083), Shenzhen Science and Technology Program (KCXFZ20211020163816023), Shenzhen Zhongdi Construction Engineering Co., Ltd. cooperation project (22100245), Key Research Project in Natural Sciences for Higher Education Institutions by the Ministry of Education (2022AH050396).

Abstract: 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.

Key words:

Donor
/ Acceptor
/ Water splitting
/ CTFs
/ Lewis basicity

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沈阳化工大学材料科学与工程学院沈阳 110142

通过供体-受体基团调节CTF-NH₂中NH₂的Lewis碱性优化光催化水分解性能

通讯作者: 王中辽,Email:wangzl@chnu.edu.cn

English

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

Corresponding author: Zhongliao Wang, wangzl@chnu.edu.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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通讯作者: 陈斌, bchen63@163.com

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通过供体-受体基团调节CTF-NH2中NH2的Lewis碱性优化光催化水分解性能

通讯作者: 王中辽,Email:wangzl@chnu.edu.cn

English

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

Corresponding author: Zhongliao Wang, wangzl@chnu.edu.cn

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通讯作者: 陈斌, bchen63@163.com

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通过供体-受体基团调节CTF-NH₂中NH₂的Lewis碱性优化光催化水分解性能

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