New Insights into Keggin-Type 12-Tungstophosphoric Acid from P-31 MAS NMR Analysis of Absorbed Trimethylphosphine Oxide and DFT Calculations

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	New Insights into Keggin-Type 12-Tungstophosphoric Acid from P-31 MAS NMR Analysis of Absorbed Trimethylphosphine Oxide and DFT Calculations
	Huang, Shing-Jong 2; Yang, Chih-Yi 3,4; Zheng, Anmin 1; Feng, Ningdong 1; Yu, Ningya 3; Wu, Pei-Hao 3; Chang, Yu-Chi 4; Lin, Ying-Chih 2; Deng, Feng 1; Liu, Shang-Bin 3,5
刊名	CHEMISTRY-AN ASIAN JOURNAL
	2011-01-03
卷号	6 期号:1 页码:137-148
关键词	density functional calculations heterogeneous catalysis polyoxometalates solid-state spectroscopy superacids
英文摘要	The acid and transport properties of the anhydrous Keggin-type 12-tungstophosphoric acid (H3PW12O40; HPW) have been studied by solid-state P-31 magic-angle spinning NMR of absorbed trimethylphosphine oxide (TMPO) in conjunction with DFT calculations. Accordingly, P-31 NMR resonances arising from various protonated complexes, such as TMPOH+ and (TMPO)(2)H+ adducts, could be unambiguously identified. It was found that thermal pretreatment of the sample at elevated temperatures (>= 423 K) is a prerequisite for ensuring complete penetration of the TMPO guest probe molecule into HPW particles. Transport of the TMPO absorbate into the matrix of the HPW adsorbent was found to invoke a desorption/absorption process associated with the ( TMPO)(2)H+ adducts. Consequently, three types of protonic acid sites with distinct superacid strengths, which correspond to P-31 chemical shifts of 92.1, 89.4, and 87.7 ppm, were observed for HPW samples loaded with less than three molecules of TMPO per Keggin unit. Together with detailed DFT calculations, these results support the scenario that the TMPOH+ complexes are associated with protons located at three different terminal oxygen (O-d) sites of the PW12O403- polyanions. Upon increasing the TMPO loading to > 3.0 molecules per Keggin unit, abrupt decreases in acid strength and the corresponding structural variations were attributed to the change in secondary structure of the pseudoliquid phase of HPW in the presence of excessive guest absorbate.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Multidisciplinary
研究领域[WOS]	Chemistry
关键词[WOS]	SOLID-STATE NMR ; QUANTUM-CHEMICAL CALCULATIONS ; LIQUID-PHASE REACTIONS ; HETEROPOLY COMPOUNDS ; PSEUDOLIQUID PHASE ; DODECATUNGSTOPHOSPHORIC ACID ; HETEROGENEOUS CATALYSIS ; WATER-MOLECULES ; H3PW12O40 ; SPECTROSCOPY
收录类别	SCI
语种	英语
WOS记录号	WOS:000285976300013
公开日期	2015-12-01
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/8214]
专题	武汉物理与数学研究所_2011年以前论文发表（包括2011年）
作者单位	1.Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Inst Phys & Math, Wuhan 430071, Peoples R China 2.Natl Taiwan Univ, Dept Chem, Taipei 10617, Taiwan 3.Acad Sinica, Inst Atom & Mol Sci, Taipei 10617, Taiwan 4.Tamkang Univ, Dept Chem & Mat Engn, Tamsui 23157, Taiwan 5.Natl Taiwan Normal Univ, Dept Chem, Taipei 11677, Taiwan
推荐引用方式 GB/T 7714	Huang, Shing-Jong,Yang, Chih-Yi,Zheng, Anmin,et al. New Insights into Keggin-Type 12-Tungstophosphoric Acid from P-31 MAS NMR Analysis of Absorbed Trimethylphosphine Oxide and DFT Calculations[J]. CHEMISTRY-AN ASIAN JOURNAL,2011,6(1):137-148.
APA	Huang, Shing-Jong.,Yang, Chih-Yi.,Zheng, Anmin.,Feng, Ningdong.,Yu, Ningya.,...&Liu, Shang-Bin.(2011).New Insights into Keggin-Type 12-Tungstophosphoric Acid from P-31 MAS NMR Analysis of Absorbed Trimethylphosphine Oxide and DFT Calculations.CHEMISTRY-AN ASIAN JOURNAL,6(1),137-148.
MLA	Huang, Shing-Jong,et al."New Insights into Keggin-Type 12-Tungstophosphoric Acid from P-31 MAS NMR Analysis of Absorbed Trimethylphosphine Oxide and DFT Calculations".CHEMISTRY-AN ASIAN JOURNAL 6.1(2011):137-148.