具有高效电荷分离的2D/2D α-Fe2O3/Bi2WO6 S型异质结增强光-芬顿催化活性

doi:10.1016/S1872-2067(20)63602-6

催化学报 ›› 2021, Vol. 42 ›› Issue (1): 97-106.DOI: 10.1016/S1872-2067(20)63602-6

具有高效电荷分离的2D/2D α-Fe₂O₃/Bi₂WO₆ S型异质结增强光-芬顿催化活性

王文亮^a, 赵稳立^a, 张灏纯^a, 窦新城^a, 史海峰^a^,^b^,^*()

^a江南大学理学院, 江苏无锡214122
^b江南大学江苏省轻工光电工程技术研究中心, 江苏无锡214122

收稿日期:2020-02-28 接受日期:2020-04-08 出版日期:2021-01-18 发布日期:2021-01-18
通讯作者: 史海峰
基金资助:
国家自然科学基金(21203077);国家自然科学基金(21773099);中央高校基本科研业务费(JUSRP51716A);江苏省青蓝工程项目

2D/2D step-scheme α-Fe₂O₃/Bi₂WO₆ photocatalyst with efficient charge transfer for enhanced photo-Fenton catalytic activity

Wenliang Wang^a, Wenli Zhao^a, Haochun Zhang^a, Xincheng Dou^a, Haifeng Shi^a^,^b^,^*()

^aSchool of Science, Jiangnan University, Wuxi 214122, Jiangsu, China
^bJiangsu Provincial Research Center of Light Industrial Optoelectronic Engineering and Technology, Jiangnan University, Wuxi 214122, Jiangsu, China

Received:2020-02-28 Accepted:2020-04-08 Online:2021-01-18 Published:2021-01-18
Contact: Haifeng Shi
About author:^*Tel: +86-15052262655; E-mail: hfshi@jiangnan.edu.cn
Supported by:
National Natural Science Foundation of China(21203077);TNational Natural Science Foundation of China(21773099);Fundamental Research Funds for the Central Universities(JUSRP51716A);Qing Lan Project of Jiangsu Province

摘要/Abstract

摘要：

近年来, Fenton反应由于其成本低, 反应速度快, 操作简单等优势受到了广泛的研究. 传统的均相Fenton反应可通过H₂O₂氧化Fe²⁺产生具有强氧化性的羟基自由基, 用于处理难降解的有机物. 然而, Fenton反应存在两个主要问题, 首先, 在Fenton反应中需要加入大量的酸来维持酸性环境, 以保证反应的最佳活性. 其次, Fenton反应中铁离子不断流失并形成固体污泥, 这严重影响了Fenton反应产生•OH的效率. 目前, 将光催化反应与非均相芬顿反应相结合是改善这些问题的有效方案. 非均相光芬顿反应不仅能提高有机物降解的活性, 而且通过光催化剂导带上的电子有效减少Fe³⁺的浸出和铁氢氧化物沉淀的产生.
最近, 作为一种可见光Fenton催化剂, α-Fe₂O₃可以在几乎中性的条件下发生光芬顿反应, 这解决了在反应过程中需要随时调整PH值的问题. 此外, 光照条件下α-Fe₂O₃价带上的电子能跃迁至导带并将Fe ³⁺还原成Fe²⁺, 从而减少铁离子的损耗. 然而, 由于光生载流子复合率较高等问题, 单一α-Fe₂O₃光催化剂的催化活性仍不理想. 构建具有2D/2D结构的S型异质结可以缩短电子在界面间的传输距离, 增大材料的活性位点, 将光生电子-空穴在空间上分离, 从而有效增强光生载流子的分离效率. 因此, 构建2D/2D α-Fe₂O₃/Bi₂WO₆ S型异质结, 并用于光芬顿反应有望进一步提高对有机污染物的降解效率.
本文通过简易的水热法制备了具有2D/2D结构的α-Fe₂O₃/Bi₂WO₆ S型异质结光芬顿催化剂, 并通过XRD、BET、TEM、XPS和UV-Vis等手段对催化剂的晶体结构、元素状态、微观结构、光学性质和化学组分进行了表征. 通过在可见光照射下降解甲基蓝(MB), 考察了α-Fe₂O₃/Bi₂WO₆的光芬顿催化活性. 结果表明, 由于光催化反应与Fenton反应的协同作用, α-Fe₂O₃/Bi₂WO₆表现出了明显增强的光-Fenton催化活性, 最佳比例的α-Fe₂O₃/Bi₂WO₆的活性分别是单一α-Fe₂O₃和Bi₂WO₆的11.06倍和3.29倍. 本文将光催化反应与Fenton反应相结合, 一方面, 光催化反应对Fe³⁺的还原有促进作用,提高了Fe²⁺的浓度, 从而提升羟基自由基的产量; 另一方面, Fenton反应对α-Fe₂O₃/Bi₂WO₆中电子的利用阻止了光生载流子的复合,进一步提高了光催化降解效率. 此外, 由于二维纳米片之间具有更大的接触面积, 2D/2D异质结可以缩短电荷传输时间和距离, 促进了光生电子-空穴的分离. 同时, 具有较大比表面积的2D/2D材料可以在催化剂表面提供大量用于有机物氧化分解的活性位点. 而S型异质结的构建不但促进了界面电荷的转移和分离, 还能维持最佳的电荷氧化还原电位, 这都提升了催化剂的光芬顿催化活性. 总之, 本文为合成可高效降解有机污染物的非均相光-芬顿催化剂提供了新的思路.

关键词: Bi₂WO₆, α-Fe₂O₃, S型异质结, 光芬顿, 2D光催化剂

Abstract:

Although the traditional Fenton reaction is considered an effective strategy for solving problems caused by environmental pollution, construction of an efficient photocatalytic system by coordinating the Fenton reaction is challenging. In this study, 2D/2D step-scheme α-Fe₂O₃/Bi₂WO₆ (FO/BWO) heterostructure photo-Fenton catalysts were successfully fabricated by a facile hydrothermal method. The as-prepared materials were characterized by XRD, FT-IR, TEM, XPS, UV-vis DRS, PL, I-t, EIS, and BET analyses. Under visible light irradiation, FO/BWO exhibited remarkably high and stable photo-Fenton catalytic activity for the degradation of methyl blue (MB) at low concentrations of H₂O₂. It was noted that FO/BWO (0.5) displayed a significantly enhanced photo-Fenton catalytic activity, which was 11.06 and 3.29 times those of FO nanosheets and BWO nanosheets, respectively. The notably improved photo-Fenton catalytic activity of FO/BWO was mainly due to the combination of H₂O₂ and FO under light illumination and the presence of the 2D/2D S-scheme heterostructure, with the large contact surface, abundant active sites, and efficient separation rate of photogenerated carriers playing contributory roles. Additionally, a possible catalytic mechanism for the FO/BWO composite was preliminarily proposed via active species trapping experiments. In summary, this study provided new insights into the synthesis of an effectively heterogeneous 2D/2D S-scheme photo-Fenton catalyst for degradation of organic pollutants in wastewater.

Key words: Bi₂WO₆, α-Fe₂O₃, S-scheme, Photo-Fenton, 2D photocatalyst

王文亮, 赵稳立, 张灏纯, 窦新城, 史海峰. 具有高效电荷分离的2D/2D α-Fe₂O₃/Bi₂WO₆ S型异质结增强光-芬顿催化活性[J]. 催化学报, 2021, 42(1): 97-106.

Wenliang Wang, Wenli Zhao, Haochun Zhang, Xincheng Dou, Haifeng Shi. 2D/2D step-scheme α-Fe₂O₃/Bi₂WO₆ photocatalyst with efficient charge transfer for enhanced photo-Fenton catalytic activity[J]. Chinese Journal of Catalysis, 2021, 42(1): 97-106.

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图/表 12

Fig. 1. X-ray diffraction patterns of BWO, FO, FO/BWO (1), FO/BWO (0.5) and FO/BWO (0.3) photocatalysts.

Fig. 2. TEM images of (a-b) FO, (c-d) BWO, (e) FO/BWO (0.5) composite and (f) HRTEM image of FO/BWO (0.5) composite.

Fig. 3. XPS spectra of BWO, FO and FO/BWO (0.5) samples: (a) survey, (b) O 1s, (c) W 4f, (d) Bi 4f and (e) Fe 2p.

Fig. 4. UV-vis spectra of BWO, FO, FO/BWO (0.5), FO/BWO (0.3) and FO/BWO (1) photocatalysts.

Fig. 5. FT-IR spectra of BWO, FO, FO/BWO (1), FO/BWO (0.3) and FO/BWO (0.5) photocatalysts.

Fig. 6. (a) Dynamic curves of photodegradation for MB solution over different samples, (b) kinetic fitting of the photodegradation for MB solution over different samples, (c) degradation rate of the MB solution after 25 min. (d) degradation of MB under different reaction conditions.

Fig. 7. (a) XRD patterns of FO/BWO (0.5) photocatalyst before and after photodegradation experiment. (b) The recyclability of FO/BWO (0.5) for photocatalytic degradation of MB.

Fig. 8. Photoluminescence emission spectra for FO, BWO and FO/BWO (0.5) photocatalysts. The wavelength of excitation light for fluorescence emission spectra was 327 nm.

Fig. 9. Transient photocurrent responses for the FO, BWO and FO/BWO (0.5) composite.

Fig. 10. EIS Nyquist plots of FO, BWO and FO/BWO (0.5) composite.

Fig. 11. Comparison of the effect of different radical scavengers during photocatalytic degradation of MB over FO/BWO (0.5) composite under visible light irradiation (λ ≥ 400 nm).

Fig. 12. Schematic diagram of the photocatalytic oxidation of MB over FO/BWO (0.5) under visible-light irradiation (λ ≥ 400 nm).

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具有高效电荷分离的2D/2D α-Fe₂O₃/Bi₂WO₆ S型异质结增强光-芬顿催化活性

2D/2D step-scheme α-Fe₂O₃/Bi₂WO₆ photocatalyst with efficient charge transfer for enhanced photo-Fenton catalytic activity

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[1]	蔡铭洁, 刘艳萍, 董珂欣, 陈晓波, 李世杰. 漂浮型Bi₂WO₆/C₃N₄/碳布S型异质结光催化材料用于高效净化水体环境[J]. 催化学报, 2023, 52(9): 239-251.
[2]	孙丽娟, 于晓慧, 唐丽永, 王伟康, 刘芹芹. 构建K₃PW₁₂O₄₀/CdS核壳S型异质结实现同步太阳能光催化分解水和选择性苯甲醇氧化反应[J]. 催化学报, 2023, 52(9): 164-175.
[3]	宋明明, 宋相海, 刘鑫, 周伟强, 霍鹏伟. ZnIn₂S₄/MOF-808微球结构S型异质结光催化剂的制备及其光还原CO₂性能研究[J]. 催化学报, 2023, 51(8): 180-192.
[4]	李世杰, 王春春, 董珂欣, 张鹏, 陈晓波, 李鑫. 新型MIL-101(Fe)/BiOBr S型异质催化剂用于高效光催化降解抗生素和还原六价铬: 光催化性能分析和光催化机理研究[J]. 催化学报, 2023, 51(8): 101-112.
[5]	何厚伟, 王中辽, 代凯, 李素文, 张金锋. LSPR效应增强碳包覆In₂O₃/W₁₈O₄₉ S型异质结用于高效CO₂光还原[J]. 催化学报, 2023, 48(5): 267-278.
[6]	李瀚, 陶善仁, 万思杰, 邱国根, 龙庆, 余家国, 曹少文. ZnCdS纳米球和二苯并噻吩修饰的g-C₃N₄构成的S型异质结用于增强光催化产氢[J]. 催化学报, 2023, 46(3): 167-176.
[7]	张志洁, 王雪盛, 唐慧玲, 李德本, 徐家跃. 调控Cs₃Bi₂Br₉@V_O-In₂O₃ S型异质结的费米能级和内建电场促进光生电荷分离和二氧化碳还原[J]. 催化学报, 2023, 55(12): 227-240.
[8]	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(10): 123-133.
[9]	赵振龙, 边辑, 赵丽娜, 吴红君, 徐帅, 孙磊, 李志君, 张紫晴, 井立强. 2D ZnMOF/BiVO₄ S型异质结的构建及其可见光催化还原CO₂性能[J]. 催化学报, 2022, 43(5): 1331-1340.
[10]	徐阳锐, 朱晓蝶, 颜欢, 王盼盼, 宋旼珊, 马长畅, 陈自然, 储金宇, 刘馨琳, 逯子扬. 盐酸介导策略合成的具有优异光催化能力的ZnFe₂O₄小颗粒点缀一维苝二酰亚胺S型异质结[J]. 催化学报, 2022, 43(4): 1111-1122.
[11]	S. Wageh, Ahmed A. Al-Ghamdi, Omar A. Al-Hartomy, Maged F. Alotaibi, 王临曦. CdS/聚合物梯形产氢光催化剂及其原位光照电子转移机制[J]. 催化学报, 2022, 43(3): 586-588.
[12]	薛文华, 孙红莉, 胡晓云, 白雪, 樊君, 刘恩周. 等离子体共振协同S-scheme电荷转移促进W₁₈O₄₉/Cd_0.5Zn_0.5S高效光催化产氢[J]. 催化学报, 2022, 43(2): 234-245.
[13]	贾雪梅, 沈紫晨, 韩巧凤, 毕慧平. 相转移有机前驱体BiOAc_0.6Br_0.2I_0.2固溶体合成表面富有氧空位的棒状S型Bi₄O₅I₂/Bi₄O₅Br₂异质结[J]. 催化学报, 2022, 43(2): 288-302.
[14]	靳治良, 李红英, 李俊柯. 硫化钴改性石墨炔构建S型异质结高效光催化产氢[J]. 催化学报, 2022, 43(2): 303-315.
[15]	郭伟琦, 罗皓霖, 江治, 上官文峰. 压力诱导相变原位构建BiVO₄/Bi_0.6Y_0.4VO₄ S型异质结增强光催化全解水性能[J]. 催化学报, 2022, 43(2): 316-328.