原位制备SnO2/SnS2异质结促进光催化污染物降解

doi:10.1016/S1872-2067(19)63498-4

催化学报 ›› 2020, Vol. 41 ›› Issue (10): 1554-1563.DOI: 10.1016/S1872-2067(19)63498-4

原位制备SnO₂/SnS₂异质结促进光催化污染物降解

刘媖^a, 潘东来^a, 熊明文^b, 陶英^a, 陈晓峰^a, 张蝶青^a, 黄宇^c, 李贵生^a

a 上海师范大学资源化学教育部重点实验室, 稀土功能材料上海市重点实验室, 上海 200234;
b 蚌埠学院材料与化学工程学院, 安徽蚌埠 233030;
c 中国科学院地球环境研究所, 中国科学院气溶胶化学与物理重点实验室, 陕西西安 710075

收稿日期:2020-02-23 修回日期:2020-03-21 出版日期:2020-10-18 发布日期:2020-08-15
通讯作者: 李贵生, 熊明文
基金资助:
国家自然科学基金（21677099，21876113）；安徽省自然科学基金（KJ2018A0571）；蚌埠学院启动基金BBXY2018KYQD21）；资源化学重点实验室开放基金（00007908）；上海绿色化学工程中心；气溶胶重点实验室开放基金（KLACP1901）.

In-situ fabrication SnO₂/SnS₂ heterostructure for boosting the photocatalytic degradation of pollutants

Ying Liu^a, Donglai Pan^a, Mingwen Xiong^b, Ying Tao^a, Xiaofeng Chen^a, Dieqing Zhang^a, Yu Huang^c, Guisheng Li^a

a The Education Ministry Key Lab of Resource Chemistry, Shanghai Key Laboratory of Rare Earth Functional Materials, Shanghai Normal University, Shanghai 200234, China;
b School of Materials and Chemical Engineering, Bengbu University, Bengbu 233030, Anhui, China;
c Key Laboratory of Aerosol Chemistry and Physics of CAS, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710075, Shaanxi, China

Received:2020-02-23 Revised:2020-03-21 Online:2020-10-18 Published:2020-08-15
Supported by:
This work was supported by the National Natural Science Foundation of China (21677099, 21876113), Anhui Province (KJ2018A0571), Bengbu University (BBXY2018KYQD21), The Education Ministry Key Lab of Resource Chemistry (00007908), Shanghai Engineering Research Center of Green Energy Chemical Engineering, and Key Laboratory of Aerosol Chemistry and Physics (KLACP1901).

摘要/Abstract

摘要： 光催化技术作为一种新兴的绿色催化技术，在解决环境污染、缓解能源短缺等方面得到了广泛的研究，但光生载流子易复合的问题极大限制了该技术的应用.构建光催化剂内建电场的方法可有效提高异质结光催化剂的光生载流子分离效率，进而提高光催化效率.然而如何在两种半导体界面形成紧密接触的异质结结构仍然存在一定的挑战.
本文通过在含硫前驱液中加入SnO₂纳米颗粒，在水热条件下利用原位离子交换的方法合成了SnO₂/SnS₂异质结光催化剂。形貌表征发现此法所制备催化剂是一种复合有纳米颗粒的六边形结构纳米片异质结光催化剂，透射电子显微镜（TEM）以及X射线光电子能谱（XPS）表征证实其具有紧密连接的异质结结构.高倍TEM图显示SnO₂颗粒均紧密负载在SnS₂纳米片上.同时，XPS测试结果表明，在SnO₂/SnS₂异质结构中Sn 3d_5/2的结合能为486.43eV，介于SnS₂与SnO₂的结合能之间，这一结果可归结为SnO₂与SnS₂形成了紧密结合的异质结.此外，紫外-可见漫反射光谱（UV-vis DRS）测试结果表明，由于SnS₂的存在拓宽了单纯SnO₂光催化剂的光吸收范围，样品的光吸收范围成功地从紫外光波长范围扩展到可见光波长范围，进而提高了其对太阳光的利用率.
本文进一步采用有机染料的光催化降解作为探针反应，对所制备催化剂进行了光催化性能评价。光催化降解亚甲基蓝（MB）的实验结果显示，SnO₂/SnS₂异质结样品相比纯相的SnO₂和SnS₂以及SnO₂&SnS₂的机械混合样品均表现出更高的降解效率，验证了该紧密连接的异质结光催化剂具有更优的光催化性能.为了进一步探究SnO₂/SnS₂异质结光催化剂的光降解机理和光生载流子迁移过程，通过活性物种捕获实验探索了光降解过程中的活性物种.实验结果显示，在SnO₂/SnS₂异质结光催化剂降解有机物的过程，超氧自由基是污染物光降解过程中的主要活性物种.光生载流子迁移过程探究表明作为电子传输体的SnO₂能够快速传导光生电子并使得光生电子与水体中溶解氧发生反应产生超氧自由基.此外，光电化学测试结果证实该紧密连接的异质结结构可有效提高光生电子空穴对的分离效率。电化学阻抗谱Bode图结果证明，原位制备的SnO₂/SnS₂异质结具有最长的光生载流子寿命（41.6μs），进一步验证了具有紧密连接的异质结结构光催化剂可以有效提高对有机污染物光催化降解效率.
综上所述，通过离子交换原位转化SnO₂制备的SnO₂/SnS₂异质结构光催化剂所形成的紧密异质结结构能有效地提高光催化处理有机污染物的性能。

关键词: 原位制备, SnO₂/SnS₂异质结, 光催化降解, 光生载流子分离

Abstract: Heterostructure photocatalysts with a built-in electric field have become one of the most promising strategies to enhance photogenerated electron-hole pair separation. However, close contact between the two active components of heterogeneous photocatalysts remains a problem. Herein, the in-situ fabrication of an SnO₂/SnS₂ heterostructure photocatalyst was performed; the structure showed enhanced photocatalytic performance resulting from the tight-contact heterostructures. The results of photoelectrochemical measurements further verified that a tight-contact heterostructure improved the separation of photogenerated electron-hole pairs. The results of EIS Bode plots also demonstrated that such in-situ fabricated SnO₂/SnS₂ samples exhibited the longest carrier lifetime (41.6 μs) owing to the intimate interface of SnO₂/SnS₂ heterostructures.

Key words: in-situ fabrication, SnO₂/SnS₂ heterostructure, Photo-degradation, Photogenerated carrier separation

刘媖, 潘东来, 熊明文, 陶英, 陈晓峰, 张蝶青, 黄宇, 李贵生. 原位制备SnO₂/SnS₂异质结促进光催化污染物降解[J]. 催化学报, 2020, 41(10): 1554-1563.

Ying Liu, Donglai Pan, Mingwen Xiong, Ying Tao, Xiaofeng Chen, Dieqing Zhang, Yu Huang, Guisheng Li. In-situ fabrication SnO₂/SnS₂ heterostructure for boosting the photocatalytic degradation of pollutants[J]. Chinese Journal of Catalysis, 2020, 41(10): 1554-1563.

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https://www.cjcatal.com/CN/Y2020/V41/I10/1554

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原位制备SnO₂/SnS₂异质结促进光催化污染物降解

In-situ fabrication SnO₂/SnS₂ heterostructure for boosting the photocatalytic degradation of pollutants

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