梯型BiVO4/Ag3VO4光催化剂的构建及其可见光光催化性能

doi:10.1016/S1872-2067(20)63560-4

催化学报 ›› 2021, Vol. 42 ›› Issue (1): 46-55.DOI: 10.1016/S1872-2067(20)63560-4

梯型BiVO₄/Ag₃VO₄光催化剂的构建及其可见光光催化性能

刘丽忠^a, 胡太平^a, 代凯^a^,^*(), 张金锋^a^,^#(), 梁长浩^b^,^$()

^a淮北师范大学绿色和精准合成化学及应用教育部重点实验室, 物理与电子信息学院, 安徽淮北235000
^b中国科学院固体物理研究所, 材料物理重点实验室和安徽纳米材料和纳米技术重点实验室, 安徽合肥230031

收稿日期:2020-03-03 接受日期:2020-04-15 出版日期:2021-01-18 发布日期:2020-01-03
通讯作者: 代凯,张金锋,梁长浩
作者简介:第一联系人：† 共同第一作者.
基金资助:
国家自然科学基金(51572103);国家自然科学基金(51973078);安徽省杰出青年基金(1808085J14);安徽省教育厅重点项目(KJ2019A0595)

A novel step-scheme BiVO₄/Ag₃VO₄ photocatalyst for enhanced photocatalytic degradation activity under visible light irradiation

Lizhong Liu^a, Taiping Hu^a, Kai Dai^a^,^*(), Jinfeng Zhang^a^,^#(), Changhao Liang^b^,^$()

^aKey Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, College of Physics and Electronic Information, Huaibei Normal University, Huaibei 235000, Anhui, China
^bKey Laboratory of Materials Physics and Anhui Key Laboratory of Nanomaterials and Nanotechnology, Institute of Solid State Physics, Hefei Institute of Physical Science, Chinese Academy of Sciences, Hefei 230031, Anhui, China

Received:2020-03-03 Accepted:2020-04-15 Online:2021-01-18 Published:2020-01-03
Contact: Kai Dai,Jinfeng Zhang,Changhao Liang
About author:^$E-mail: chliang@issp.ac.cn
^#E-mail: jfzhang@chnu.edu.cn;
^*Fax: +86-561-3803256; E-mail: daikai940@chnu.edu.cn;
First author contact:† These authors contributed equally to this work.
Supported by:
National Natural Science Foundation of China(51572103);National Natural Science Foundation of China(51973078);Distinguished Young Scholar of Anhui Province(1808085J14);Key Foundation of Educational Commission of Anhui Province(KJ2019A0595)

摘要/Abstract

摘要：

近年来, 有机污染物的问题变得越来越严重. 为了解决该问题, 人们研究和开发了许多有效的光催化剂. 本工作采用水热法和化学沉积法合成了BiVO₄/Ag₃VO₄梯型半导体材料, 该复合材料在可见光下具有很强的氧化还原能力. 其中40%BiVO₄/Ag₃VO₄具有最佳的光催化降解性能, 其降解速率为0.05588 min^-1, 分别是BiVO₄和Ag₃VO₄的22.76和1.76倍. 并且其性能稳定, 经过四次循环后其降解率仍可保持90%以上. BiVO₄和Ag₃VO₄复合后, 其催化性能得到增强, 归因于形成了新型的梯型光催化机制, 该方法促进了光生电荷的分离并延长了电荷的寿命, 且通过PL测试和瞬态光电流响应证明了电荷的有效转移.
X射线衍射(XRD)可以观察到Ag₃VO₄和BiVO₄物相, 没有其他成分. 用扫描电子显微镜(SEM)和透射电子显微镜(TEM)进一步观察了该催化剂的结构和形貌, 从SEM可以看出, Ag₃VO₄生长在BiVO₄的上面, 能谱分析也证明该催化剂仅包含Ag₃VO₄和BiVO₄的各种元素, 而不含其他杂质, TEM进一步证明了两种物质复合在一起, 而不是机械混合. 通过紫外-可见光漫反射光谱(UV-vis)测试可以得到BiVO₄和Ag₃VO₄的吸收带边, 进一步计算BiVO₄的带隙和导带分别为2.41和0.455 eV, Ag₃VO₄的带隙和导带分别为2.20和0.04 eV, 二者组成的异质结的带隙满足降解的条件. 用荧光光谱(PL)和光电流研究了样品的光电特征, 结果表明BiVO₄/Ag₃VO₄光催化剂具有很高的载流子分离效率和很低的光电流电阻, 这有助于光生载流子的运输.
光催化降解甲基蓝实验表明, BiVO₄/Ag₃VO₄具有很强的光催化降解速率(0.05588 min^-1), 是BiVO₄的22.6倍, Ag₃VO₄的1.76倍, 而且经过四次循环后仍能保持很高的活性. 通过XRD发现使用后的催化剂并没有发生变化, 说明该催化剂具有良好的稳定性. 高分辨X射线光电子能谱(XPS)不仅进一步说明了该催化剂成功复合后没有其他杂质元素, 而且从各元素的结合能变化可以看出构成异质结后电子的流向, 证实了光催化机制为梯型机制. 光照射后, BiVO₄和Ag₃VO₄产生电子空穴对, 当催化剂受光激发后, 电子从价带被激发到导带, 并在价带留下空穴. 当BiVO₄和Ag₃VO₄复合后, 在接触界面形成内电场, 由于库仑相互作用, 能带边缘弯曲等作用加速了Ag₃VO₄价带上某些空穴和BiVO₄导带上电子的复合, 从而阻止了Ag₃VO₄和BiVO₄内部电子空穴对的复合, 这有助于Ag₃VO₄导带上的电子和BiVO₄价带上的空穴参与氧化还原反应. 从捕获实验可以看出, 本实验中空穴在光催化降解中起着最重要的作用, 这与上述结论一致.

关键词: 梯型光催化剂, BiVO₄, Ag₃VO₄, 光催化活性, 亚甲基蓝

Abstract:

Over the past few years, the emission of organic pollutants into the environment has increased tremendously. Therefore, various photocatalysts have been developed for the degradation of organic pollutants. In this study, a step-scheme BiVO₄/Ag₃VO₄ composite was synthesized via a hydrothermal and chemical deposition process for the degradation of methylene blue.The composite showed strong redox ability under visible light. The 40%BiVO₄/Ag₃VO₄ composite showed excellent photocatalytic degradation properties with a K_app of 0.05588 min^-1, which is 22.76 and 1.76 times higher than those of BiVO₄ (0.00247 min^-1) and Ag₃VO₄ (0.03167 min^-1), respectively. The composite showed a stable performance and could retain 90% of its photocatalytic activity even after four cycles. The improved catalytic performance of the composite as compared to BiVO₄ and Ag₃VO₄ can be attributed to its novel step-scheme mechanism, which facilitated the separation of the photogenerated charges and increased their lifetime. The photoluminescence measurement results and transient photocurrent response revealed that the composite showed efficient extraction of charge carriers.

Key words: Step-scheme photocatalyst, BiVO4, Ag3VO4, Photocatalytic activity, Methylene blue

刘丽忠, 胡太平, 代凯, 张金锋, 梁长浩. 梯型BiVO₄/Ag₃VO₄光催化剂的构建及其可见光光催化性能[J]. 催化学报, 2021, 42(1): 46-55.

Lizhong Liu, Taiping Hu, Kai Dai, Jinfeng Zhang, Changhao Liang. A novel step-scheme BiVO₄/Ag₃VO₄ photocatalyst for enhanced photocatalytic degradation activity under visible light irradiation[J]. Chinese Journal of Catalysis, 2021, 42(1): 46-55.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(20)63560-4

https://www.cjcatal.com/CN/Y2021/V42/I1/46

图/表 14

Fig. 1. Schematic of the synthesis of the X%BiVO4/Ag3VO4 composites.

Fig. 2. XRD patterns of BiVO4, Ag3VO4, and the X%BiVO4/Ag3VO4 composites.

Fig. 3. SEM images of (a) BiVO4, (b) Ag3VO4, and (c) 40%BiVO4/Ag3VO4; (d) EDS spectra of 40%BiVO4/Ag3VO4 and (e-i) elemental mapping of 40%BiVO4/Ag3VO4.

Fig. 4. (a, b) TEM images and (c, d) HRTEM images of 40%BiVO4/Ag3VO4.

Fig. 5. XPS survey spectra of (a) BiVO4, 40%BiVO4/Ag3VO4, and Ag3VO4 and their high-resolution (b) Bi 4f, (c) Ag 3d, (d) V 2p, and (e) O 1s spectra.

Fig. 6. (a) N2 adsorption-desorption isotherms and (b) SBET values of the BiVO4, Ag3VO4, and X%BiVO4/Ag3VO4 catalysts.

Fig. 7. (a) UV-Vis DRS spectra of Ag3VO4, X%BiVO4/Ag3VO4, and BiVO4; (b) Eg values for Ag3VO4 and BiVO4.

Fig. 8. PL spectra of the BiVO4, Ag3VO4, and X%BiVO4/Ag3VO4 catalysts.

Fig. 9. (a) Transient photocurrent responses and (b) EIS results of Ag3VO4, BiVO4, and X%BiVO4/Ag3VO4.

Fig. 10. (a) Photocatalytic degradation of MB; (b) Linear transform ln(C0/C) of the kinetic curves for MB degradation using the catalysts; (c) The apparent pseudo-first-order rate constants (kapp) of the catalysts.

Table 1 Degradation rates and Kapp values of the catalysts (degradation time: 50 min).

Sample	Degradation rate (%)	K_app(min^-1)
Ag₃VO₄	83.77	0.03167
BiVO₄	16.31	0.00247
20%BiVO₄/Ag₃VO₄	84.89	0.03377
40%BiVO₄/Ag₃VO₄	93.48	0.05588
60%BiVO₄/Ag₃VO₄	84.46	0.03012
BiVO₄+Ag₃VO₄	87.00	0.03511

Fig. 11. (a) MB degradation activities of the photocatalysts after four cycles; (b) XRD patterns of the fresh and used 40%BiVO4/Ag3VO4 catalysts.

Fig. 12. MB degradation rate of 40%BiVO4/Ag3VO4 in the presence of different capture agents.

Fig. 13. Step-scheme charge carrier flow for the composite.

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梯型BiVO₄/Ag₃VO₄光催化剂的构建及其可见光光催化性能

A novel step-scheme BiVO₄/Ag₃VO₄ photocatalyst for enhanced photocatalytic degradation activity under visible light irradiation

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