超声辅助制备Cs2AgBiBr6/Bi2WO6 S型异质结用于可见光光催化CO2还原

doi:10.1016/S1872-2067(22)64091-9

摘要/Abstract

摘要：

光催化因其可以利用太阳能进行光解水产氢、CO₂还原、降解有机污染物及有机物转化而被认为是解决当前能源危机和环境问题的一种有效手段. 由于光催化反应是由光激发光催化材料生成光生载流子引发的, 因此理想的光催化剂应当具有宽的光响应范围、低的光生载流子复合率和足够的氧化还原能力来进行表面反应. 然而单一组分的半导体材料难以同时满足宽光谱响应(即窄带隙)和强氧化还原能力(即价带更正和导带更负). 通过耦合两个具有可见光响应且交错能带排布的半导体来构建S型异质结, 不仅能拓宽光催化剂的光吸收范围、促进电荷分离, 还同时保留了两种半导体的强氧化还原能力, 是发展高效光催化材料的一种有效途径.

Cs₂AgBiBr₆的导带和价带分别位于-0.65 V vs. NHE和1.60 V vs. NHE, 而Bi₂WO₆的导带和价带分别为-0.4 V vs. NHE和2.4 V vs. NHE, 两者能带位置匹配. 因此, 本文选择Cs₂AgBiBr₆和Bi₂WO₆用于构建S型异质结复合材料, 采用超声辅助方法处理含有Cs₂AgBiBr₆量子点和Bi₂WO₆微米花的乙酸乙酯溶液, 通过在Cs₂AgBiBr₆量子点和Bi₂WO₆微米花界面间形成Bi-Br键, 组装出了Cs₂AgBiBr₆量子点/Bi₂WO₆微米花异质结复合材料, 并考察了材料在可见光照射下还原CO₂的光催化活性. 结果表明, 所制备的Cs₂AgBiBr₆/Bi₂WO₆异质结复合材料具有优越的光催化还原CO₂生成CO和CH₄性能, 发现在一系列含有不同比例的x Cs₂AgBiBr₆/Bi₂WO₆异质结复合材料中(x为Cs₂AgBiBr₆与Bi₂WO₆的质量比, x = 0.2, 0.5, 1.0), 0.5 Cs₂AgBiBr₆/Bi₂WO₆异质结复合材料表现出最优的光催化性能, 在300 W氙灯(420 nm ≤ λ ≤ 800 nm)照射下8 h内生成了15.4 μmol g^-1的CO和3.2 μmol g^-1的CH₄. 其性能明显优于同等反应条件下单纯Cs₂AgBiBr₆, Bi₂WO₆以及等比例机械混合的Cs₂AgBiBr₆和Bi₂WO₆的光催化活性, 这归因于Cs₂AgBiBr₆和Bi₂WO₆间形成了有效的S型异质结, 该S型异质结可在不牺牲Bi₂WO₆价带空穴氧化能力和Cs₂AgBiBr₆导带电子还原能力的基础上, 促进光生电子-空穴对的分离. 综上, 本文结果表明耦合两种具有交错能带的光催化材料来形成S型异质结是开发高效光催化剂的一种有效策略, 也展示了无铅钙钛矿在光催化中的应用前景.

关键词: 铯银铋溴, 钨酸铋, S型异质结, 光催化CO₂还原, 可见光

Abstract:

In this manuscript, Cs₂AgBiBr₆/Bi₂WO₆ nanocomposites was fabricated via an ultrasonic-assisted process. The activity of the as-obtained Cs₂AgBiBr₆/Bi₂WO₆ nanocomposites for photocatalytic CO₂ reduction was studied under visible light. The as-obtained Cs₂AgBiBr₆/Bi₂WO₆ nanocomposites show a superior activity for photocatalytic CO₂ reduction to produce CH₄ and CO, with an optimum activity achieved over 0.5 Cs₂AgBiBr₆/Bi₂WO₆. The obvious superior activity observed over Cs₂AgBiBr₆/Bi₂WO₆ nanocomposites as compared with bare Cs₂AgBiBr₆ and bare Bi₂WO₆ as well as a mechanical mixture of Cs₂AgBiBr₆ and Bi₂WO₆ can be owe to the fabrication of an efficient S-scheme heterojunction, which accelerates the separation of the photogenerated charge carriers in Cs₂AgBiBr₆ and Bi₂WO₆ without sacrificing the high redox capability of Cs₂AgBiBr₆ and Bi₂WO₆. This work demonstrates that the coupling of two photocatalytic materials with staggered band alignment to form an S-scheme heterojunction is an effective strategy to develop efficient photocatalytic systems and also highlights the promising role of using lead free perovskites in photocatalysis.

Key words: Cs₂AgBiBr₆, Bi₂WO₆, S-Scheme heterojunction, Photocatalytic CO₂ reduction, Visible light

王佳琦, 程浩, 魏丁琼, 李朝晖. 超声辅助制备Cs₂AgBiBr₆/Bi₂WO₆ S型异质结用于可见光光催化CO₂还原[J]. 催化学报, 2022, 43(10): 2606-2614.

Jiaqi Wang, Hao Cheng, Dingqiong Wei, Zhaohui Li. Ultrasonic-assisted fabrication of Cs₂AgBiBr₆/Bi₂WO₆ S-scheme heterojunction for photocatalytic CO₂ reduction under visible light[J]. Chinese Journal of Catalysis, 2022, 43(10): 2606-2614.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(22)64091-9

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图/表 11

Scheme 1. An illustration of an S-scheme heterojunction system.

Fig. 1. XRD patterns of Cs2AgBiBr6, Bi2WO6 and 0.5 Cs2AgBiBr6/Bi2WO6 nanocomposite.

Fig. 2. TEM (a) and HRTEM (b) images of 0.5 Cs2AgBiBr6/Bi2WO6 nanocomposite.

Fig. 3. XPS spectra of samples. (a) Cs2AgBiBr6 and 0.5 Cs2AgBiBr6/Bi2WO6 in Br 3d region. (b) Cs2AgBiBr6, Bi2WO6, and 0.5 Cs2AgBiBr6/Bi2WO6 in Bi 4f region. Cs2AgBiBr6 and 0.5 Cs2AgBiBr6/Bi2WO6 in Cs 3d (c) and Ag 3d (d) region. (e) Bi2WO6 and 0.5 Cs2AgBiBr6/Bi2WO6 in W 4f region. (f) 0.5 Cs2AgBiBr6/Bi2WO6 in O 1s region.

Fig. 4. UV-vis DRS spectra of Bi2WO6, Cs2AgBiBr6 and 0.5 Cs2AgBiBr6/Bi2WO6 nanocomposite.

Fig. 5. Amount of CO and CH4 evolved in 8 h irradiation over different samples. (a) Cs2AgBiBr6; (b) Bi2WO6; (c) 0.2 Cs2AgBiBr6/Bi2WO6; (d) no catalyst or in dark; (e) a mechanical mixture of Cs2AgBiBr6 and Bi2WO6.

Fig. 6. Amount of CO and CH4 evolved in 8 h irradiation over 0.2 Cs2AgBiBr6/Bi2WO6, 0.5 Cs2AgBiBr6/Bi2WO6, and 1.0 Cs2AgBiBr6/Bi2WO6 nanocomposite.

Fig. 7. Nyquist plots of experimental impedance data for Cs2AgBiBr6, Bi2WO6 and 0.5 Cs2AgBiBr6/Bi2WO6.

Scheme 2. Schematic illustration of photocatalytic CO2 reduction over Cs2AgBiBr6/Bi2WO6 nanocomposite under visible light.

Fig. 8. ESR spectra of DMPO-•OH (a) and DMPO-•O2- (b) adducts over Cs2AgBiBr6, Bi2WO6 and 0.5 Cs2AgBiBr6/Bi2WO6 nanocomposite.

Fig. 9. (a) Cycling of photocatalytic CO2 reduction over 0.5 Cs2AgBiBr6/Bi2WO6 nanocomposite. (b) XRD patterns of the fresh and used 0.5 Cs2AgBiBr6/Bi2WO6 nanocomposite.

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超声辅助制备Cs₂AgBiBr₆/Bi₂WO₆ S型异质结用于可见光光催化CO₂还原

Ultrasonic-assisted fabrication of Cs₂AgBiBr₆/Bi₂WO₆ S-scheme heterojunction for photocatalytic CO₂ reduction under visible light

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