用于改进H2O2制备的1D/0D异质结的ZnIn2S4@ZnO S型光催化剂

doi:10.1016/S1872-2067(23)64514-0

催化学报 ›› 2023, Vol. 53: 123-133.DOI: 10.1016/S1872-2067(23)64514-0

用于改进H₂O₂制备的1D/0D异质结的ZnIn₂S₄@ZnO S型光催化剂

吴优^a, 杨祎^a, 谷苗莉^a, 别传彪^b^,^*(), 谭海燕^c, 程蓓^a^,^*(), 许景三^d^,^*()

^a武汉理工大学材料复合新技术国家重点实验室, 湖北武汉430070, 中国
^b中国地质大学(武汉)材料与化学学院太阳燃料实验室, 湖北武汉430078, 中国
^c湖北民族学院化学与环境工程学院, 湖北恩施445000, 中国
^d昆士兰科技大学化学与物理学院材料科学中心, 布里斯班昆士兰, 澳大利亚

收稿日期:2023-07-24 接受日期:2023-08-28 出版日期:2023-10-18 发布日期:2023-10-25
通讯作者: *电子信箱: biechuanbiao@cug.edu.cn (别传彪), chengbei2013@whut.edu.cn (程蓓), jingsan.xu@qut.edu.au (许景三).
基金资助:
国家重点研发计划(2022YFB3803600);国家重点研发计划(2022YFE0115900);国家自然科学基金(22238009);国家自然科学基金(22261142666);国家自然科学基金(52073223);国家自然科学基金(22278324);国家自然科学基金(22262012);国家自然科学基金(51932007);国家自然科学基金(22202187);湖北省自然科学基金(2022CFA001);博士后创新人才支持计划(BX2021275);中国博士后科学基金(2022M712957)

1D/0D heterostructured ZnIn₂S₄@ZnO S-scheme photocatalysts for improved H₂O₂ preparation

You Wu^a, Yi Yang^a, Miaoli Gu^a, Chuanbiao Bie^b^,^*(), Haiyan Tan^c, Bei Cheng^a^,^*(), Jingsan Xu^d^,^*()

^aState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, Hubei, China
^bLaboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei, China
^cSchool of Chemistry and Environmental Engineering, Hubei University for Nationalities, Enshi 445000, Hubei, China
^dSchool of Chemistry and Physics & Centre for Materials Science, Queensland University of Technology, Queensland 4000, Brisbane, Australia

Received:2023-07-24 Accepted:2023-08-28 Online:2023-10-18 Published:2023-10-25
Contact: *E-mail: biechuanbiao@cug.edu.cn (C. Bie), chengbei2013@whut.edu.cn (B. Cheng), jingsan.xu@qut.edu.au (J. Xu).
Supported by:
The National Key Research and Development Program of China(2022YFB3803600);The National Key Research and Development Program of China(2022YFE0115900);National Natural Science Foundation of China(22238009);National Natural Science Foundation of China(22261142666);National Natural Science Foundation of China(52073223);National Natural Science Foundation of China(22278324);National Natural Science Foundation of China(22262012);National Natural Science Foundation of China(51932007);National Natural Science Foundation of China(22202187);The Natural Science Foundation of Hubei Province of China(2022CFA001);The National Postdoctoral Program for Innovative Talents(BX2021275);The Project funded by China Postdoctoral Science Foundation(2022M712957)

摘要/Abstract

摘要：

过氧化氢作为一种绿色氧化剂, 被广泛应用于食品工业、有机合成、医疗消毒和污水处理等领域. 目前, 大多数用于工业生产的过氧化氢是通过蒽醌法制备. 传统的蒽醌法能耗高、有机副产物多、环境污染严重, 因此, 利用清洁的太阳能进行半导体光催化生产过氧化氢备受关注. 其中, ZnO半导体因其高稳定性、无毒性、良好的生物相容性和合适的导带位置而成为一种潜在的过氧化氢生产材料. 然而, 单一的ZnO在光催化生产过氧化氢中面临着许多问题, 如载流子分离效率低、可见光吸收弱等, 从而导致其较低的光催化性能. 因此, 多种策略被用于解决上述问题, 如掺杂非贵金属元素、晶面调控和异质结构构建等. 在这些改性策略中, 异质结构建被认为是提高光催化性能最有效的方法之一, 特别是S型异质结因其较好的氧化还原能力和电子转移特性而备受关注. S型异质结通常由一个氧化型光催化剂和一个还原型光催化剂组成, 在两者的接触界面上形成内建电场, 促使无用的载流子复合, 从而保留更多具有强氧化还原能力的空穴和电子, 以此提高异质结光催化性能. ZnIn₂S₄具有合适的带隙和高导带位置, 可以作为还原型光催化剂与ZnO构建S型异质结, 从而提高光催化活性.

本文首先通过静电纺丝法制备了ZnO纳米纤维, 通过化学浴沉积在ZnO纳米纤维上原位生长出ZnIn₂S₄纳米颗粒, 从而合成具有S型异质结结构的ZnO/ZnIn₂S₄光催化剂. 由于ZnO和ZnIn₂S₄具有相同的金属元素Zn, ZnO纳米纤维中的Zn元素为ZnIn₂S₄提供了良好的原位生长位点, 从而使ZnO和ZnIn₂S₄之间形成紧密接触, 有利于光生载流子的分离和转移. 原位XPS结果表明, ZnO/ZnIn₂S₄复合材料中的In元素和S元素的结合能在光照下降低, 而O元素的结合能升高. 说明在光照下, ZnO/ZnIn₂S₄复合材料中ZnO失去电子, 而ZnIn₂S₄得到电子, 这与S型异质结的电荷转移机理一致. 电子顺磁共振(EPR)结果表明ZnO/ZnIn₂S₄复合材料能产生比单独ZnO或ZnIn₂S₄更强的超氧自由基和羟基自由基, 说明得益于S型异质结, ZnO/ZnIn₂S₄复合材料的氧化还原能力得到了提升. 此外, 电子顺磁共振谱和原位漫反射傅里叶变换红外光谱结果表明, 基于ZnO/ZnIn₂S₄复合材料的光催化双氧水合成反应是一种两步单电子氧还原过程. ZnO/ZnIn₂S₄复合材料的光催化双氧水生产活性得到显著提升, 可以达到928 μmol g^-1 h^-1, 超过ZnO和ZnIn₂S₄光催化双氧水生产活性的4倍.

综上所述, 本文合成了低维S型ZnO/ZnIn₂S₄复合光催化剂, 实现过氧化氢生产性能的提升, 提供了一种利用相同元素设计和制备高效S型异质结光催化剂的新思路, 对异质结在光催化、电催化、太阳能电池等领域的研究起到一定的借鉴作用.

关键词: S型异质结, 过氧化氢生产, 低维异质结构, 原位光谱学, 纳米纤维

Abstract:

Solar photocatalysis is a promising, green, and sustainable technique for the synthesis of H₂O₂. In this study, low-dimensional ZnO/ZnIn₂S₄ S-scheme heterojunction photocatalysts are fabricated using electrostatic spinning and chemical bath deposition methods for the efficient photocatalytic production of H₂O₂. ZnO nanofibers loaded with 20 wt% ZnIn₂S₄ exhibit a superior H₂O₂ production rate of 928 μmol g^-1 h^-1, which is more than four times higher than that seen in pristine hexagonal phase ZnO and ZnIn₂S₄. First-principles calculations and in-situ X-ray photoelectron spectroscopy reveal the charge separation and transfer mechanisms in the S-scheme heterojunction. The construction of the S-scheme heterojunction facilitates the spatial separation of charge carriers, and electrons and holes with higher redox abilities are retained. Photoelectrochemical and photoluminescence tests further show that the formation of an S-scheme heterojunction is beneficial for the separation of photoinduced charge carriers. Electrochemical tests and electron paramagnetic resonance measurements indicate that H₂O₂ production is primarily via a two-step single-electron O₂ reduction path. This study provides a new approach for the construction of S-scheme heterojunction materials that can efficiently produce H₂O₂ under solar irradiation.

Key words: S-scheme heterojunction, Hydrogen peroxide production, Low-dimensional heterostructure, In-situ spectroscopy, Nanofiber

吴优, 杨祎, 谷苗莉, 别传彪, 谭海燕, 程蓓, 许景三. 用于改进H₂O₂制备的1D/0D异质结的ZnIn₂S₄@ZnO S型光催化剂[J]. 催化学报, 2023, 53: 123-133.

You Wu, Yi Yang, Miaoli Gu, Chuanbiao Bie, Haiyan Tan, Bei Cheng, Jingsan Xu. 1D/0D heterostructured ZnIn₂S₄@ZnO S-scheme photocatalysts for improved H₂O₂ preparation[J]. Chinese Journal of Catalysis, 2023, 53: 123-133.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(23)64514-0

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图/表 11

Fig. 1. Schematic diagram for the synthesis of ZnO/ZnIn2S4 heterostructures.

Fig. 2. XRD patterns of ZnO, ZnIn2S4, and heterostructures with different ratios of ZnO/ZnIn2S4.

Fig. 3. SEM images of ZnO (a) and ZZS-20 (b) nanofibers. (c) TEM images of ZZS-20. (d) HRTEM images of ZZS-20. (e) HAADF image and EDX elemental mappings of Zn, O, In, and S elements in ZZS-20.

Fig. 4. (a) The UV-vis spectra of catalysts. (b,c) Mott-Schottky plots of ZnIn2S4 and ZnO. (d) Band structures of ZnO and ZnIn2S4.

Fig. 5. ISIXPS of the survey (a), In 3d (b), O 1s (c), and S 2p (d) for ZnO, ZnIn2S4, and ZZS-20 in dark condition and under light condition.

Fig. 6. Calculated electrostatic potentials of ZnO (a) and ZnIn2S4 (b). (c) Charge density difference of ZnO/ZnIn2S4 (the yellow region signifies the accumulation layer of electrons and the cyan region is the electron depletion layer).

Fig. 7. (a) Electron transfer mechanism of ZnO/ZnIn2S4 S-scheme heterojunction. (b) Photocatalytic H2O2 evolution performance of different photocatalysts. (c) Stability cycle test of H2O2 production by ZZS-20.

Fig. 8. PL (a) and TRPL (b) spectra of ZnO, ZnIn2S4, and ZZS-20. Transient photocurrent response (c) and EIS analysis (d) of photocatalysts.

Fig. 9. LSV of ZnO (a), ZnIn2S4 (b), and ZZS-20 (c). (d) K-L curves of samples.

Fig. 10. (a) EPR spectra for ?O2? of ZnO, ZnIn2S4, and ZZS-20 in methanol. (b) EPR spectra for ?OH of ZnO, ZnIn2S4, and ZZS-20 in water.

Fig. 11. In-situ DRFTIS spectra of ZZS-20 adsorption process (a) and illumination process (λ = 365 nm) (b).

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用于改进H₂O₂制备的1D/0D异质结的ZnIn₂S₄@ZnO S型光催化剂

1D/0D heterostructured ZnIn₂S₄@ZnO S-scheme photocatalysts for improved H₂O₂ preparation

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