Furan-Based HTCC/In2S3 Heterojunction Achieves Fast Charge Separation To Boost the Photocatalytic Generation of H2O2 in Pure Water

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-10-19 DOI:10.1021/acscatal.4c0434110.1021/acscatal.4c04341
Xiaolong Tang, Changlin Yu*, Jiaming Zhang, Kaiwei Liu, Debin Zeng, Fang Li, Feng Li, Guijun Ma, Yanbin Jiang and Yongfa Zhu*, 
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Abstract

The limitations imposed by the high carrier recombination rate in the current photocatalytic H2O2 production system substantially restrict the rate of H2O2 generation. Herein, we successfully prepared an In2S3/HTCC dense heterojunction bridged by In–S–C bonds through in situ polymerization of glucose on In2S3. This interfacial In–S–C bond provides a fast transfer channel for electrons at the interface to achieve a highly efficient interfacial charge transfer efficiency, leading to the formation of an enhanced built-in electric field between In2S3 and HTCC, thus dramatically accelerating the rate of charge separation and effectively prolonging the lifetime of the photogenerated carriers. Moreover, the coverage of HTCC enhances the absorption of visible light and sorption of O2 by In2S3, while lowering its two-electron oxygen reduction reaction (ORR) energy barrier. Notably, our research demonstrates that In2S3/HTCC can generate H2O2 not only through the well-known two-step one-electron ORR but also via an alternative pathway utilizing 1O2 as an intermediate, thereby enhancing H2O2 production. Benefiting from these advantages, In2S3/HTCC-2 can produce H2O2 at a rate of up to 1392 μmol g–1 h–1 in a pure aqueous system, which is 18.2 and 5.2 times higher than that of pure In2S3 and HTCC, respectively. Our work not only provides a novel synthesis method of new organic/inorganic heterojunction photocatalysts based on HTCC but also offers new insights into the potential mechanism of interfacial bonding of heterostructures to regulate the photocatalytic H2O2 production activity.

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呋喃基 HTCC/In2S3 异质结实现快速电荷分离,促进纯水中 H2O2 的光催化生成
在目前的光催化 H2O2 生产系统中,载流子的高重组率极大地限制了 H2O2 的生成速度。在此,我们通过原位聚合 In2S3 上的葡萄糖,成功制备了以 In-S-C 键桥接的 In2S3/HTCC 致密异质结。这种界面 In-S-C 键为电子在界面上提供了一个快速转移通道,实现了高效的界面电荷转移效率,从而在 In2S3 和 HTCC 之间形成了一个增强的内置电场,从而大大加快了电荷分离的速度,有效延长了光生载流子的寿命。此外,HTCC 的覆盖增强了 In2S3 对可见光的吸收和对 O2 的吸附,同时降低了其双电子氧还原反应 (ORR) 的能垒。值得注意的是,我们的研究表明,In2S3/HTCC 不仅可以通过众所周知的两步一电子氧还原反应生成 H2O2,还可以通过利用 1O2 作为中间体的另一种途径生成 H2O2,从而提高 H2O2 的生成。得益于这些优势,In2S3/HTCC-2 在纯水体系中产生 H2O2 的速率可达 1392 μmol g-1 h-1,分别是纯 In2S3 和 HTCC 的 18.2 倍和 5.2 倍。我们的工作不仅为基于 HTCC 的新型有机/无机异质结光催化剂提供了一种新的合成方法,而且为异质结构界面键调节光催化 H2O2 生成活性的潜在机制提供了新的见解。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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