Location, acid strength, and mobility of the acidic protons in Keggin 12-H3PW12O40: A combined solid-state NMR spectroscopy and DFT quantum chemical calculation study

CORC > 武汉物理与数学研究所 > 中国科学院武汉物理与数学研究所 > 2011年以前论文发表（包括2011年）

	Location, acid strength, and mobility of the acidic protons in Keggin 12-H3PW12O40: A combined solid-state NMR spectroscopy and DFT quantum chemical calculation study
	Yang, J ; Janik, MJ ; Ma, D ; Zheng, AM ; Zhang, MJ ; Neurock, M ; Davis, RJ ; Ye, CH ; Deng, F
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2005-12-28
卷号	127 期号:51 页码:18274-18280
英文摘要	Solid-state C-13 NMR experiments and quantum chemical Density Functional Theory (DFT) calculations of acetone adsorption were used to study the location of protons in anhydrous 12-tungstophosphoric acid (HPW), the mobility of the isolated and hydrated acidic protons, and the acid strength heterogeneity of the anhydrous hydroxyl groups. This study presents the first direct NMR experimental evidence that there are two types of isolated protons with different acid strengths in the anhydrous Keggin HPW. Rotational Echo DOuble Resonance (REDOR) NMR experiments combined with quantum chemical DFT calculations demonstrated that acidic protons in anhydrous HPW are localized on both bridging (O-c) and terminal (O-d) atoms of the Keggin unit. The CP/MAS NMR experiments revealed that the isolated acidic protons are immobile, but hydrated acidic protons are highly mobile at room temperature. The isotropic chemical shift of the adsorbed acetone suggested that the acid strength of the H(H2O)(n)(+) species in partially hydrated HPW is comparable to that of a zeolite, while the acidity of an isolated proton is much stronger than that of a zeolite. Isolated protons on the bridging oxygen atoms of anhydrous HPW are nearly superacidic.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Multidisciplinary
研究领域[WOS]	Chemistry
关键词[WOS]	DOUBLE-RESONANCE NMR ; TOTAL-ENERGY CALCULATIONS ; WAVE BASIS-SET ; IN-SITU NMR ; H-1 MAS NMR ; HETEROPOLY COMPOUNDS ; DODECATUNGSTOPHOSPHORIC ACID ; 12-TUNGSTOPHOSPHORIC ACID ; PHOSPHOTUNGSTIC ACID ; ISOBUTANE/BUTENE ALKYLATION
收录类别	SCI
语种	英语
WOS记录号	WOS:000234258700060
公开日期	2015-07-28
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/4477]
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.Univ Virginia, Dept Chem Engn, Charlottesville, VA 22904 USA 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Yang, J,Janik, MJ,Ma, D,et al. Location, acid strength, and mobility of the acidic protons in Keggin 12-H3PW12O40: A combined solid-state NMR spectroscopy and DFT quantum chemical calculation study[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2005,127(51):18274-18280.
APA	Yang, J.,Janik, MJ.,Ma, D.,Zheng, AM.,Zhang, MJ.,...&Deng, F.(2005).Location, acid strength, and mobility of the acidic protons in Keggin 12-H3PW12O40: A combined solid-state NMR spectroscopy and DFT quantum chemical calculation study.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,127(51),18274-18280.
MLA	Yang, J,et al."Location, acid strength, and mobility of the acidic protons in Keggin 12-H3PW12O40: A combined solid-state NMR spectroscopy and DFT quantum chemical calculation study".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 127.51(2005):18274-18280.