Yang Yang, Li Hao, Zhao Haitao, Qu Ruiyang, Zhang Shuo, Hu Wenshuo, Yu Xinning, Zhu Xinbo, Liu Shaojun, Zheng Chenghang, Gao Xiang
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, 310027, China.
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, 310027, China; School of Energy and Power, Jiangsu University of Science and Technology, Zhenjiang, 212003, China.
J Hazard Mater. 2019 Jun 5;371:156-164. doi: 10.1016/j.jhazmat.2019.02.103. Epub 2019 Feb 27.
Efficient removal of chlorinated volatile organic compounds (CVOCs) has received great attention because of the considerable harm that they cause to the environment and to human health. Developing novel catalysts and exploring the catalytic activation and deconstruction mechanism of CVOCs molecule are always the focus in this field. Here, a set of Sn doped TiO catalysts were investigated for the decomposition of dichloromethane (DCM). Rietveld refinement of the XRD patterns showed that Sn ions can uniformly disperse into TiO and induce the crystal transition of anatase. Meanwhile, such decorating can induce an increase in specific surface area and affect the surface oxygen vacancy concentration of these samples, which have been demonstrated by N adsorption and XPS, respectively. Catalytic performance tests indicated that the SnTiO has the best activity for DCM decomposition, and a lower CHCl selectivity than that of pure TiO. Computational results suggested the dominant surface (110) of rutile SnTiO is more beneficial for the adsorption/dissociation of DCM molecule than that of anatase TiO (101). That's because the anchoring of DCM to Sn sites and electron enrichment on the surface bridge oxygen atoms of rutile SnTiO (110) can promote the nucleophilic substitution process for breaking of CCl bonds.
由于氯代挥发性有机化合物(CVOCs)对环境和人类健康造成的巨大危害,其有效去除受到了广泛关注。开发新型催化剂并探索CVOCs分子的催化活化和解构机制一直是该领域的研究重点。在此,研究了一组Sn掺杂的TiO催化剂用于二氯甲烷(DCM)的分解。对XRD图谱的Rietveld精修表明,Sn离子可以均匀地分散到TiO中并诱导锐钛矿的晶体转变。同时,这种修饰可以导致比表面积增加,并分别通过N吸附和XPS证明影响这些样品的表面氧空位浓度。催化性能测试表明,SnTiO对DCM分解具有最佳活性,且CHCl选择性低于纯TiO。计算结果表明,金红石型SnTiO的主要表面(110)比锐钛矿型TiO(101)更有利于DCM分子的吸附/解离。这是因为DCM锚定在Sn位点以及金红石型SnTiO(110)表面桥氧原子上的电子富集可以促进亲核取代过程以断裂C-Cl键。