构建0D/1D Ag3PO4/TiO2 S型异质结以实现高效光降解和析氧

doi:10.1016/S1872-2067(22)64099-3

催化学报 ›› 2022, Vol. 43 ›› Issue (10): 2558-2568.DOI: 10.1016/S1872-2067(22)64099-3

构建0D/1D Ag₃PO₄/TiO₂ S型异质结以实现高效光降解和析氧

朱玉坤^a^,^†, 庄严^b^,^†, 王乐乐^b, 唐华^a^,^*(), 孟献丰^b, 佘希林^a^,^#()

^a青岛大学环境科学与工程学院, 山东青岛 266071
^b江苏大学材料科学与工程学院, 江苏镇江 212013

收稿日期:2022-01-24 接受日期:2022-03-29 出版日期:2022-10-18 发布日期:2022-09-30
通讯作者: 唐华,佘希林
作者简介:^†共同第一作者.
基金资助:
国家自然科学基金(21975110);山东省泰山青年学者计划

Constructing 0D/1D Ag₃PO₄/TiO₂ S-scheme heterojunction for efficient photodegradation and oxygen evolution

Yukun Zhu^a^,^†, Yan Zhuang^b^,^†, Lele Wang^b, Hua Tang^a^,^*(), Xianfeng Meng^b, Xilin She^a^,^#()

^aSchool of Environmental Science and Engineering, Qingdao University, Qingdao 266071, Shandong, China
^bSchool of Materials Science & Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China

Received:2022-01-24 Accepted:2022-03-29 Online:2022-10-18 Published:2022-09-30
Contact: Hua Tang, Xilin She
About author:^†Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(21975110);Taishan Youth Scholar Program of Shandong Province

摘要/Abstract

摘要：

化石燃料的大量使用使人类面临前所未有的能源枯竭与环境污染问题, 因此, 寻求和发展可持续能源与技术迫在眉睫. 光催化过程利用催化剂捕获光子将太阳能转化成各种能源与化学品, 是一种极具潜力的绿色可持续技术. 理性设计高效的捕光材料与催化体系是实现高效太阳能利用与转化的有效策略. 而光催化剂的效率主要受制于电荷分离效率低、氧化还原能力不足等缺陷. 在众多提高光催化效率的策略中, 异质结光催化剂的构建是解决以上问题的有效途径. 与传统的Ⅱ型异质结光催化剂相比, 阶梯(S)型异质结在氧化型和还原型半导体之间构筑了内建电场, 动力学上加速了光生载流子的分离、迁移并且保留催化剂最高的氧化还原能力, 成为一类极具应用潜力的异质结催化剂.

本文通过简单的水热法将Ag₃PO₄纳米颗粒原位生长在TiO₂纤维表面, 制备了0D/1D Ag₃PO₄/TiO₂ S型异质结. 两者之间通过构筑紧密的界面接触有效降低了光生载流子的传输障碍, 促进了界面电荷转移, 从而在光催化产氧和光分解罗丹明B、苯酚和盐酸四环素方面表现出优异的活性和光稳定性. 催化体系的一系列表征结果均验证了Ag₃PO₄/TiO₂复合材料的成功制备. 物相表征表明, 均匀负载在TiO₂ NFs表面的Ag₃PO₄ NPs颗粒尺寸更小, 这是由于TiO₂ 纳米纤维(NFs)中丰富的羟基使得二氧化钛纤维具备显著的限域效应, 可以有效地防止Ag₃PO₄颗粒的聚集. 此外, Ag₃PO₄/TiO₂的比表面积远大于Ag₃PO₄, 比表面积的增加有利于提供更多的活性位点, 从而提高光催化活性. 光电测试分析表明, Ag₃PO₄/TiO₂具有较高的载流子分离和迁移效率; 功函数的密度泛函理论计算结合XPS数据证实了内建电场的建立及其从TiO₂指向Ag₃PO₄的方向. 上述实验和理论计算结果都确定了Ag₃PO₄/TiO₂在光照下的S型电荷转移路径. 循环试验及反应前后催化剂的XRD表征结果都验证了该S型异质结具有较好的氧化还原能力和光催化稳定性.

总之, 0D/1D Ag₃PO₄/TiO₂ S型异质结具有较高的光催化产氧活性(726 mol/g/h)和稳定性, 对RhB(100%), 苯酚(60%)和TC(100%)等有机污染物具有良好的降解能力. 复合材料活性的提高与Ag₃PO₄ NPs和TiO₂ NFs之间紧密的界面接触以及丰富的活性位点密切相关. 综上, 本文为构建0D/1D S型异质结光催化剂提供了一种有前景的策略.

关键词: S型异质结, 0D/1D, Ag₃PO₄/TiO₂, 光催化产氧, 光催化降解

Abstract:

An S-scheme heterojunction photocatalyst is capable of boosting photogenerated carrier separation and transfer, thus maintaining high photooxidation and photoredox ability. Herein, a 0D Ag₃PO₄ nanoparticles (NPs)/1D TiO₂ nanofibers (NFs) S-scheme heterojunction with intimate interfacial contact was designed via the the hydro-thermal method. Benefiting from the abundant hydroxyl groups and size confinement effect of TiO₂ NFs, the average diameter of the Ag₃PO₄ nanoparticles decreased from 100 to 22 nm, which favored the construction of a 0D/1D geometry heterojunction. The multifunctional Ag₃PO₄/TiO₂ sample exhibited excellent photocatalytic activity and stability in photocatalytic oxygen production (726 µmol/g/h) and photocatalytic degradation of various organic contaminants such as rhodamine B (100%), phenol (60%) and tetracycline hydrochloride (100%). The significant improvements in the photocatalytic performance and stability can be attributed to the intimate interfacial contacts and rich active sites of 0D/1D geometry, fast charge carrier migration, and outstanding photoredox properties induced by the S-scheme charge-transfer route. This work offers a promising strategy for constructing 0D/1D S-scheme heterojunction photocatalysts for improved photocatalytic performance.

Key words: S-Scheme heterojunction, 0D/1D, Ag₃PO₄/TiO₂, Oxygen production, Photocatalytic degradation

朱玉坤, 庄严, 王乐乐, 唐华, 孟献丰, 佘希林. 构建0D/1D Ag₃PO₄/TiO₂ S型异质结以实现高效光降解和析氧[J]. 催化学报, 2022, 43(10): 2558-2568.

Yukun Zhu, Yan Zhuang, Lele Wang, Hua Tang, Xianfeng Meng, Xilin She. Constructing 0D/1D Ag₃PO₄/TiO₂ S-scheme heterojunction for efficient photodegradation and oxygen evolution[J]. Chinese Journal of Catalysis, 2022, 43(10): 2558-2568.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(22)64099-3

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图/表 14

Scheme 1. Schematic illustration of the synthesis of the 0D/1D Ag3PO4/TiO2 S-scheme heterostructure by an electrostatic self-assembly approach.

Fig. 1. XRD patterns (a), FTIR spectra (b) and Raman spectra (c) of the samples.

Fig. 2. The SEM images of Ag3PO4 (a) and Ag3PO4/TiO2 NFs (b). (c) The EDS profile of Ag3PO4/TiO2 NFs. The TEM images (d), HRTEM images (e,g) and the corresponding particle size distributions of Ag3PO4 in Ag3PO4/TiO2 NFs (f). (h,i) The SAED image of Ag3PO4/TiO2.

Fig. 3. XPS profiles of the Ag3PO4/TiO2 sample. (a) Survey spectrum; (b) Ag 3d; (c) Ti 2p; (d) P 2p spectrum.

Fig. 4. Time course (a) and comparison of the O2 evolution rates (b) over different samples.

Fig. 5. Photocatalytic degradation of RhB (a), phenol (b) and TC (c) under visible light. The corresponding -ln(C/C0) vs. reaction time plots of RhB (d), phenol (e) and TC (f).

Fig. 6. (a) Photocatalytic degradation of TC in the presence of Ag3PO4/TiO2, mechanical mixing sample, Ag3PO4/P25 and Ag3PO4/TiO2 NPs. (b) the kinetic fit for (a).

Fig. 7. Photocatalytic degradation of RhB (a), phenol (b) and TC (c) under UV-vis light. The corresponding -ln(C/C0) vs. reaction time plots of RhB (d), phenol (e) and TC (f).

Fig. 8. Cycle experiments of Ag3PO4/TiO2 and Ag3PO4 for photocatalytic degradation of RhB with visible light (a) and UV-visible light (b) irradiation. XRD patterns (c) and TEM (up) and HRTEM (down) images (d) of Ag3PO4/TiO2 sample before and after the reaction.

Fig. 9. UV-vis spectra (a), the (αhν)1/2 vs. hν plots (b) of Ag3PO4 and TiO2. (c,d) Mott-Schottky plots of TiO2 NFs and Ag3PO4 particles.

Fig. 10. PL spectra (a), ns-level time-resolved PL decay spectra (b), transient photocurrent responses (c) and EIS Nyquist plots (d) of Ag3PO4/TiO2, Ag3PO4 and TiO2 samples.

Fig. 11. (a) SPV spectra of Ag3PO4/TiO2, Ag3PO4 and TiO2 samples. Work function for the TiO2 (b) and Ag3PO4 (c). (d) EPR spectra.

Fig. 12. Effect of radical scavengers on the degradation efficiency of RhB by Ag3PO4/TiO2 under visible and UV-vis light irradiation.

Fig. 13. (a,b) Band energy alignments of the TiO2 and Ag3PO4 before and after contacting. Possible mechanism for the S-scheme heterojunction electron-hole migration pathway in the degradation (c) and OER (d) reaction over the Ag3PO4/TiO2 heterojunction.

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构建0D/1D Ag₃PO₄/TiO₂ S型异质结以实现高效光降解和析氧

Constructing 0D/1D Ag₃PO₄/TiO₂ S-scheme heterojunction for efficient photodegradation and oxygen evolution

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