构建双通道路径增强iCOF/Bi2O3 S型异质结在纯水体系中光催化合成H2O2性能

引用本文: 夏阳, 张康延, 杨恒, 史利娟, 易群. 构建双通道路径增强iCOF/Bi₂O₃ S型异质结在纯水体系中光催化合成H₂O₂性能[J]. 物理化学学报, 2024, 40(11): 240701. doi: 10.3866/PKU.WHXB202407012 shu

Citation: Yang Xia, Kangyan Zhang, Heng Yang, Lijuan Shi, Qun Yi. Improving Photocatalytic H₂O₂ Production over iCOF/Bi₂O₃ S-Scheme Heterojunction in Pure Water via Dual Channel Pathways[J]. Acta Physico-Chimica Sinica, 2024, 40(11): 240701. doi: 10.3866/PKU.WHXB202407012 shu

构建双通道路径增强iCOF/Bi₂O₃ S型异质结在纯水体系中光催化合成H₂O₂性能

夏阳 ^{1,
,} ,
张康延 ^1, ,
杨恒 ^{2,
,} ,
史利娟 ^1, ,
易群 ^{1,
,}

1.
武汉工程大学化工与制药学院, 绿色化工过程教育部重点实验室, 武汉 430072
2.
武汉轻工大学化学与环境工程学院, 武汉 430023

通讯作者: 夏阳, xiayang410@sina.com; 杨恒, yhxg666@sina.com; 易群, yq20071001@163.com

基金项目:
国家自然科学基金 2210821

海南省重点研发项目 ZDYF2024GXJS005

武汉轻工大学校立研究与创新项目 2024Y18

摘要: 太阳能光催化技术是一种绿色、经济、可持续的制备H₂O₂方法，被认为是取代传统蒽醌法最有前景的策略。然而，由于有限的光捕获能力、快速的光生载流子复合以及氧化还原能力不足等问题，单一组分光催化剂表现出温和的光催化活性。并且，在光催化合成H₂O₂反应系统中需要额外添加牺牲剂。在这项研究中，我们通过光沉积法将Bi₂O₃ (BO)纳米颗粒负载于离子型有机共价框架材料(iCOF)纳米纤维上，构建一种S型异质结用于双通道路径光催化合成H₂O₂。在纯水体系中，在iCOF表面负载10 wt% BO时，复合催化剂iCOF/BO10表现出最高的H₂O₂产率，达到了9.76 mmol·g⁻¹·h⁻¹ (在420 nm处的量子效率为5.5%)。这一性能分别是纯iCOF的2.2倍，纯BO的5.6倍。原位表征技术(包括原位X射线光电子能谱、DFT理论计算、活性物种捕获实验以及原位漫反射红外傅里叶变换光谱)揭示该S型异质结不仅能促进光生载流子的分离和增强光吸收能力，而且能实现氧化还原能力最大化，使得反应体系同时通过间接2e⁻氧气还原反应和4e⁻水氧化反应双通道路径产生H₂O₂。此外，4e⁻水氧化反应生成的O₂能够通过间接2e⁻氧气还原反应加快H₂O₂生成的反应动力学，实现光催化H₂O₂的全合成。该项工作为开发新颖催化剂实现高效光催化合成H₂O₂提供了独特的见解。

关键词:

English

Improving Photocatalytic H₂O₂ Production over iCOF/Bi₂O₃ S-Scheme Heterojunction in Pure Water via Dual Channel Pathways

Yang Xia ^{1,
,} ,
Kangyan Zhang ^1, ,
Heng Yang ^{2,
,} ,
Lijuan Shi ^1, ,
Qun Yi ^{1,
,}

1.
Key Laboratory of Green Chemical Engineering Process of Ministry of Education, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430072, China
2.
College of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China

Corresponding author: Email: xiayang410@sina.com; Tel: +86-15827307205 (Y.X.); Email: yhxg666@sina.com; Tel: +86-13296543782 (H.Y.); Email: yq20071001@163.com; Tel: +86-15103400721 (Q.Y.)

Received Date: 09 July 2024
Accepted Date: 19 August 2024
Revised Date: 16 August 2024
Available Online: 15 November 2024
Fund Project:
the National Natural Science Foundation of China

the Key Research and Development Project of Hainan Province

the Research and Innovation Initiatives of WHPU

Abstract: Solar photocatalysis is a green, economical, and sustainable method for H₂O₂ synthesis, which has been regarded as the most promising alternative to the traditional anthraquinone oxidation method. However, single-component photocatalyst exhibits moderate activity owing to the limited light-harvesting range, fast charge recombination and inadequate redox capacity. Moreover, the addition of sacrificial agents is required in the reaction system. Herein, we present the development of an S-scheme heterojunction, achieved through photodepositing Bi₂O₃ nanoparticles (BO) on ionic covalent organic framework nanofiber (iCOF). The optimized photocatalyst iCOF/BO10 shows the highest H₂O₂ production performance in pure water, achieving an H₂O₂ yield of 9.76 mmol·g⁻¹·h⁻¹ with an apparent quantum yield (AQY) of 5.5% at 420 nm. This photocatalytic performance is approximately 2.2 and 5.6 times as high as that of pristine iCOF and BO, respectively. In-depth characterizations including in situ irradiated XPS, DFT-calculations, active species trapping experiments and in situ DRIFTS, reveal that the obtained sample not only facilitates charge carrier separation and enhances light absorption capability, but also maximizes the redox ability to concurrently achieve indirect 2e⁻ ORR and 4e⁻ WOR for H₂O₂ production. Additionally, the generated O₂ from the 4e⁻ WOR is capable of accelerating the reaction kinetics for H₂O₂ formation via the indirect 2e⁻ ORR pathway, enabling overall photocatalytic H₂O₂ synthesis. This work provides a new insight into creating innovative catalysts for achieving high-efficiency photosynthesis of H₂O₂.

Key words:

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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

构建双通道路径增强iCOF/Bi₂O₃ S型异质结在纯水体系中光催化合成H₂O₂性能

通讯作者: 夏阳, xiayang410@sina.com; 杨恒, yhxg666@sina.com; 易群, yq20071001@163.com

English

Improving Photocatalytic H₂O₂ Production over iCOF/Bi₂O₃ S-Scheme Heterojunction in Pure Water via Dual Channel Pathways

Corresponding author: Email: xiayang410@sina.com; Tel: +86-15827307205 (Y.X.); Email: yhxg666@sina.com; Tel: +86-13296543782 (H.Y.); Email: yq20071001@163.com; Tel: +86-15103400721 (Q.Y.)

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