Z-机制磷酸银/钨酸铋复合物的构建及其可见光催化降解有机污染物

引用本文: 王中辽, 胡太平, 代凯, 张金锋, 梁长浩. Z-机制磷酸银/钨酸铋复合物的构建及其可见光催化降解有机污染物[J]. 催化学报, 2017, 38(12): 2021-2029. doi: 10.1016/S1872-2067(17)62942-5 shu

Citation: Zhongliao Wang, Taiping Hu, Kai Dai, Jinfeng Zhang, Changhao Liang. Construction of Z-scheme Ag₃PO₄/Bi₂WO₆ composite with excellent visible-light photodegradation activity for removal of organic contaminants[J]. Chinese Journal of Catalysis, 2017, 38(12): 2021-2029. doi: 10.1016/S1872-2067(17)62942-5 shu

Z-机制磷酸银/钨酸铋复合物的构建及其可见光催化降解有机污染物

a 淮北师范大学物理与电子信息学院, 安徽能源材料重点实验室, 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
基金项目:
国家自然科学基金（51572103，51502106）；安徽省高等学校省级优秀青年人才基金（gxyqZD201751）.

摘要: 环境危害不仅对人类健康构成巨大威胁，而且也阻碍了经济社会的快速发展.光催化剂通过利用太阳能来降解污染物为环境问题提供一条理想的途径.光催化剂的制备应该考虑以下几点：（1）对可见光响应；（2）高量子效率和稳定性；（3）安全、廉价、无毒的原材料.早期的一些催化剂如二氧化钛、氧化锌、硫化锌、锗酸锌和磷酸铋等在紫外线照射下表现出优秀的光催化活性.但是紫外光是稀有的，而且对人体健康有害.近年来，对宽带隙半导体的改性如掺杂、贵金属沉积、构建异质结或固溶体催化剂取得了有效进展.遗憾的是，受限于材料的固有属性，有限的改进仍然不能满足实际应用的需求.因此，探索高效稳定的可见光驱动的光催化剂依然是十分有意义的.环境危害不仅对人类健康构成巨大威胁，而且也阻碍了经济社会的快速发展.光催化剂通过利用太阳能来降解污染物为环境问题提供一条理想的途径.光催化剂的制备应该考虑以下几点：（1）对可见光响应；（2）高量子效率和稳定性；（3）安全、廉价、无毒的原材料.早期的一些催化剂如二氧化钛、氧化锌、硫化锌、锗酸锌和磷酸铋等在紫外线照射下表现出优秀的光催化活性.但是紫外光是稀有的，而且对人体健康有害.近年来，对宽带隙半导体的改性如掺杂、贵金属沉积、构建异质结或固溶体催化剂取得了有效进展.遗憾的是，受限于材料的固有属性，有限的改进仍然不能满足实际应用的需求.因此，探索高效稳定的可见光驱动的光催化剂依然是十分有意义的.
磷酸银在可见光下表现出超强的光催化降解有机污染物和产氧的能力，但是磷酸银容易受到光腐蚀，光催化活性和稳定性很难维持.另外，磷酸银导带上的电子电势较正，这将导致其很难在光催化过程中被利用.而磷酸银导带上电子的积累会抑制其内部电子空穴对的分离，从而对磷酸银的光催化活性和稳定性造成不利影响.
本文选择钨酸铋纳米片与磷酸银复合去抑制电子空穴对的复合和进一步提高磷酸银的活性和稳定性.样品的粉末X射线衍射、能谱和X光电子能谱的分析证实了磷酸银/钨酸铋复合物已经被成功合成.稳态荧光光谱证实了磷酸银/钨酸铋复合物的构建可以作为一种有效抑制电子和空穴对复合的手段.通过对样品进行光催化降解次甲基蓝的实验，我们发现磷酸银/钨酸铋复合材料展现出比磷酸银和钨酸铋更强的光催化活性.其中，磷酸银/钨酸铋光催化降解次甲基蓝的速率为0.61385 min^-1，这是磷酸银（0.47179 min^-1）和钨酸铋（0.10270 min^-1）活性的1.3和6.0倍.同时，磷酸银/钨酸铋表现出耐久的稳定性，在连续五次光降解过程中几乎没有明显的活性损失.进一步通过对磷酸银/钨酸铋复合材料进行光催化活性成分的捕获实验，我们发现空穴、超氧负离子自由基和羟基自由基都发挥了一定的作用.最后，我们讨论了光催化机制，Z-机制光催化机制被认为是合理的.

关键词:

English

Construction of Z-scheme Ag₃PO₄/Bi₂WO₆ composite with excellent visible-light photodegradation activity for removal of organic contaminants

a College of Physics and Electronic Information, Anhui Key Laboratory of Energetic Materials, Huaibei Normal University, Huaibei 235000, Anhui, China;
b Key Laboratory of Materials Physics and Anhui Key Laboratory of Nanomaterials and Nanotechnology, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, Anhui, China
Received Date: 19 September 2017
Revised Date: 12 October 2017
Fund Project:
This work was supported by the National Natural Science Foundation of China (51572103, 51502106) and the Foundation for Young Talents in College of Anhui Province (gxyqZD201751).

Abstract: Ag₃PO₄ has good potential for use in photocatalytic degradation of organic contaminants. However, the activity and stability of Ag₃PO₄ is hard to sustain because of photocorrosion and the positive potential of the conduction band of Ag₃PO₄. In this study, A composite consisting of Bi₂WO₆ nanosheets and Ag₃PO₄ was developed to curb recombination of charge carriers and enhance the activity and stability of the catalyst. Formation of a Ag₃PO₄/Bi₂WO₆ composite was confirmed using X-ray diffraction, energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. Photoluminescence spectroscopy provided convincing evidence that compositing Bi₂WO₆ with Ag₃PO₄ effectively reduced photocorrosion of Ag₃PO₄. The Ag₃PO₄/Bi₂WO₆ composite gave a high photocatalytic performance in photodegradation of methylene blue. A degradation rate of 0.61 min^-1 was achieved; this is 1.3 and 6.0 times higher than those achieved using Ag₃PO₄ (0.47 min^-1) and Bi₂WO₆ (0.10 min^-1), respectively. Reactive species trapping experiments using the Ag₃PO₄/Bi₂WO₆ composite showed that holes, ·OH, and ·O₂^-all played specific roles in the photodegradation process. The photocatalytic mechanism was investigated and a Z-scheme was proposed as a plausible mechanism.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

Z-机制磷酸银/钨酸铋复合物的构建及其可见光催化降解有机污染物

English

Construction of Z-scheme Ag₃PO₄/Bi₂WO₆ composite with excellent visible-light photodegradation activity for removal of organic contaminants

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Z-机制磷酸银/钨酸铋复合物的构建及其可见光催化降解有机污染物

English

Construction of Z-scheme Ag3PO4/Bi2WO6 composite with excellent visible-light photodegradation activity for removal of organic contaminants

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Construction of Z-scheme Ag₃PO₄/Bi₂WO₆ composite with excellent visible-light photodegradation activity for removal of organic contaminants

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs