Toward a Unified Identification of Ti Location in the MFI Framework of High-Ti-Loaded TS-1: Combined EXAFS, XANES, and DFT Study

doi:10.1021/acs.jpcc.6b05087

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	Toward a Unified Identification of Ti Location in the MFI Framework of High-Ti-Loaded TS-1: Combined EXAFS, XANES, and DFT Study
	Dong JC(董俊才); Zhu HL(朱海亮); Wang Y(王研); An PF(安鹏飞); Liang YX(梁雅翔); Guo ZY(郭志英); Chen DL(陈栋梁); Doug, JC; Zhu, HL; Xiang, YJ; Wang, Y; An, PF; Gong, Y; Lang, YX; Qiu, LM; Zheng, AG; Peng, XX; Lin, M; Xu, GT; Guo, ZY; Chen, DL
	2016
发表期刊	JOURNAL OF PHYSICAL CHEMISTRY C (IF:4.536[JCR-2016],4.796[5-Year])
ISSN	1932-7447
EISSN	1932-7455
卷号	120 期号:36 页码:20114-20124
通讯作者	郭志英 ; 陈栋梁
文章类型	Article
摘要	Titanium silicalite-1 (TS-1) has been shown to be a heterogeneous catalyst with remarkable efficiency and selectivity; however, the nature of the active Ti site in the MFI framework remains elusive. Here we report combined experimental and theoretical research on Ti distribution in the 12 crystallographically distinct T sites of the MFI framework in high-Ti-loaded TS-1 (2.7 wt % in TiO2). Using a multishell fit to extended X-ray absorption fine structure, we show that T4 is the most populated site, in marked contrast to the preferential substitution sites and the definitely excluded sites assumed hitherto by diffraction studies. The identification is supported by a good agreement between calculated and experimental X-ray absorption near-edge structure studies and by full periodic density functional theory (DFT) computation. In spite of having the identical most favored site, the preference order for the remaining sites predicted by DFT does not fully match the experimental results. This suggests that Ti distribution in the resulting TS-1 framework is positively correlated with the thermodynamic stability of pure material but can be affected by other factors such as interdefects. These new insights may facilitate the bottom-up design of new zeolites with tailored catalytic performance and studies on mechanisms of various oxidation reactions.
DOI	10.1021/acs.jpcc.6b05087
关键词[WOS]	RAY-ABSORPTION SPECTROSCOPY ; POWDER NEUTRON-DIFFRACTION ; HYDROGEN-PEROXIDE ; SILICALITE CHARACTERIZATION ; DEFECTIVE SILICALITES ; TITANIUM SILICALITE-1 ; TITANOSILICATE TS-1 ; IR SPECTROSCOPY ; FINE-STRUCTURE ; ZEOLITE TS-1
收录类别	SCI
语种	英语
WOS类目	Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:000383641700024
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://ir.ihep.ac.cn/handle/311005/260337
专题	多学科研究中心
作者单位	中国科学院高能物理研究所
推荐引用方式 GB/T 7714	Dong JC,Zhu HL,Wang Y,et al. Toward a Unified Identification of Ti Location in the MFI Framework of High-Ti-Loaded TS-1: Combined EXAFS, XANES, and DFT Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2016,120(36):20114-20124.
APA	董俊才.,朱海亮.,王研.,安鹏飞.,梁雅翔.,...&Chen, DL.(2016).Toward a Unified Identification of Ti Location in the MFI Framework of High-Ti-Loaded TS-1: Combined EXAFS, XANES, and DFT Study.JOURNAL OF PHYSICAL CHEMISTRY C,120(36),20114-20124.
MLA	董俊才,et al."Toward a Unified Identification of Ti Location in the MFI Framework of High-Ti-Loaded TS-1: Combined EXAFS, XANES, and DFT Study".JOURNAL OF PHYSICAL CHEMISTRY C 120.36(2016):20114-20124.