“电子集流体”Bi19S27Br3/BiOBr复合材料的制备及其增强光催化CO2还原性能

doi:10.1016/S1872-2067(21)64037-8

催化学报 ›› 2022, Vol. 43 ›› Issue (5): 1324-1330.DOI: 10.1016/S1872-2067(21)64037-8

“电子集流体”Bi₁₉S₂₇Br₃/BiOBr复合材料的制备及其增强光催化CO₂还原性能

赵君泽^a, 薛敏^a, 季梦夏^a, 王彬^a, 王雨^a, 李英杰^a, 陈自然^b, 李华明^a, 夏杰祥^a()

^a江苏大学化学化工学院, 能源研究所, 江苏镇江212013
^b四川职业技术学院建筑与环境工程系, 四川遂宁629000

收稿日期:2021-09-22 接受日期:2021-11-04 出版日期:2022-05-18 发布日期:2022-03-23
通讯作者: 夏杰祥
基金资助:
国家自然科学基金(21878134);国家自然科学基金(21676128);江苏省研究生科研和实践创新计划(KYCX19_1627)

“Electron collector” Bi₁₉S₂₇Br₃ nanorod-enclosed BiOBr nanosheet for efficient CO₂ photoconversion

Junze Zhao^a, Min Xue^a, Mengxia Ji^a, Bin Wang^a, Yu Wang^a, Yingjie Li^a, Ziran Chen^b, Huaming Li^a, Jiexiang Xia^a()

^aInstitute for Energy Research, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China
^bDepartment of Architecture and Environment Engineering, Sichuan Vocational and Technical College, Suining 629000, Sichuan, China

Received:2021-09-22 Accepted:2021-11-04 Online:2022-05-18 Published:2022-03-23
Contact: Jiexiang Xia
Supported by:
National Natural Science Foundation of China(21878134);National Natural Science Foundation of China(21676128);Postgraduate Research & Practice Innovation Program of Jiangsu Province(KYCX19_1627)

摘要/Abstract

摘要：

日益严峻的能源危机与全球变暖问题严重影响着人类的生存环境, 因此急需开发一种绿色环保的新型能源来缓解这一现状. 将CO₂气体转化为燃料或高附加值碳基化学品被认为是一种可以同时缓解能源危机和CO₂排放的绿色途径. 受自然界光合作用的启发, 光催化CO₂还原途径因其以太阳光为能量来源、反应过程无二次污染, 被认为是一种环境友好的CO₂转化途径. 然而, 受制于光催化剂电荷转移效率较低以及CO₂分子活化能力不理想等因素, 人工光合过程实现高效CO₂还原仍然具有很大挑战. 前期研究表明, 通过材料的调控可有效提升其光催化CO₂还原能力. 其中, 通过在材料表面引入电子集流体的方法可以有效收集并聚集产生的光生电荷, 提升材料的电荷传输效率, 实现材料光催化CO₂还原能力的提升. 受此启发, 本文以BiOBr(BOB)材料为主体, 在其表面引入“电子集流体”型Bi₁₉S₂₇Br₃(BSB)纳米棒材料, 成功制备BSB/BOB复合材料.

通过X射线衍射、扫描电镜和高分辨透射电镜表征证明了BSB棒状结构已成功复合在BOB材料表面. 同时, 对所制BSB/BOB材料进行了光催化CO₂还原活性结果表明, BSB/BOB材料相比于单体BSB和BOB均展现出更强的CO₂还原制备CO的能力. 其中, BSB/BOB-5材料CO产出速率为19.83 μmol g^‒1 h^‒1, 其活性分别约为单体BSB和BOB材料的8.74倍和2.40倍. 紫外-可见漫反射光谱和电化学测试结果表明, BSB的引入有效提升材料的光响应能力和光生载流子的分离传输效率. 结合莫特-肖特基测试和能带理论计算结果给出了光生电子可以从BOB材料导带传递并聚集在BSB材料导带的过程. 理论计算结果进一步显示, 在BSB/BOB材料中, BSB作为电子集流体, 可以有效收集并聚集BOB表面的电子. 此外, 由于BSB具备较强的CO₂吸附能力, 其在BSB/BOB材料中可以作为CO₂的吸附-活化位点, 进而有效提升材料的光催化活性. 结合原位红外漫反射光谱分析BSB/BOB材料表面光催化CO₂还原过程中生成的中间产物, 进而提出了可能的光催化CO₂还原机理. 综上, 本研究为高性能光催化CO₂还原催化剂的设计与制备提供了新思路.

关键词: Bi₁₉S₂₇Br₃, BiOBr, 光催化CO₂还原, 电子集流体, 电荷迁移

Abstract:

Although CO₂ photoreduction is a promising method for solar-to-fuel conversion, it suffers from low charge transfer efficiency of the photocatalysts. To improve the CO₂ photoreduction performance, introduction of electron-accumulated materials on the photocatalyst surface is considered an effective method. In this study, the Bi₁₉S₂₇Br₃/BiOBr composites were designed and synthesized. The Bi₁₉S₂₇Br₃ nanorod in this photocatalytic system acts as an electron-accumulated active site for extracting the photogenerated electrons on the BiOBr surface and for effectively activating the CO₂ molecules. As a result, Bi₁₉S₂₇Br₃/BiOBr composites exhibit the higher charge carrier transfer efficiency and further improves the CO₂ photoreduction performance relative to that of pure Bi₁₉S₂₇Br₃ and BiOBr. The rate of CO formation using Bi₁₉S₂₇Br₃/BiOBr-5 is about 8.74 and 2.40 times that using Bi₁₉S₂₇Br₃ and BiOBr, respectively. This work provides new insights for the application of Bi₁₉S₂₇Br₃ as an electron-accumulating site for achieving high photocatalytic CO₂ reduction performance in the future.

Key words: Bi₁₉S₂₇Br₃, BiOBr, CO₂ photoreduction, Electron-accumulated material, Charge transfer

赵君泽, 薛敏, 季梦夏, 王彬, 王雨, 李英杰, 陈自然, 李华明, 夏杰祥. “电子集流体”Bi₁₉S₂₇Br₃/BiOBr复合材料的制备及其增强光催化CO₂还原性能[J]. 催化学报, 2022, 43(5): 1324-1330.

Junze Zhao, Min Xue, Mengxia Ji, Bin Wang, Yu Wang, Yingjie Li, Ziran Chen, Huaming Li, Jiexiang Xia. “Electron collector” Bi₁₉S₂₇Br₃ nanorod-enclosed BiOBr nanosheet for efficient CO₂ photoconversion[J]. Chinese Journal of Catalysis, 2022, 43(5): 1324-1330.

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图/表 7

Scheme 1. Schematic illustration of the formation of the BSB/BOB composites.

Fig. 1. (a) XRD patterns of BOB and the BSB/BOB composites. (b) SEM, (c) TEM, and (d) HR-TEM images of the BSB/BOB-5 composite.

Fig. 2. (a) Photocatalytic CO yield and (b) rate of photocatalytic CO generation using BOB, BSB, and the BSB/BOB composites. (c) Photocatalytic CO evolution using BSB/BOB-5 under various conditions. (d) Long-term photocatalytic CO2RR performance of BSB/BOB-5.

Fig. 3. (a) Electrochemical impedance spectra and (b) photocurrent patterns of BSB, BOB, and BSB/BOB-5 composites.

Fig. 4. (a) UV-vis diffuse reflectance spectra of BOB, BSB and the BSB/BOB composites. Mott-Schotty plots of (b) BSB and (c) BOB. (d) Plausible photocatalytic mechanism of the BSB/BOB composite.

Fig. 5. DFT calculations: (a) charge density difference image and (b) ELF of the BSB/BOB composites. (c) Simulated CO2 adsorption model of BOB and BSB. (d) In situ FT-IR spectra for the photocatalytic CO2RR using the BSB/BOB-5 composites.

Scheme 2. Schematic illustration of the CO2 photoreduction in the presence of the BSB/BOB composites (* denotes the adsorption state at the surface of the catalyst).

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“电子集流体”Bi₁₉S₂₇Br₃/BiOBr复合材料的制备及其增强光催化CO₂还原性能

“Electron collector” Bi₁₉S₂₇Br₃ nanorod-enclosed BiOBr nanosheet for efficient CO₂ photoconversion

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