Chinese Journal of Magnetic Resonance ›› 2021, Vol. 38 ›› Issue (4): 571-584.doi: 10.11938/cjmr20212926
Yao XIAO1,2,Chang-jiu XIA3,Xian-feng YI1,*(
),Feng-qing LIU1,2,Shang-bin LIU4,An-min ZHENG1,*()
Received:2021-06-28
Online:2021-12-05
Published:2021-08-14
Contact:
Xian-feng YI,An-min ZHENG
E-mail:yxf@wipm.ac.cn;zhenganm@wipm.ac.cn
CLC Number:
Yao XIAO,Chang-jiu XIA,Xian-feng YI,Feng-qing LIU,Shang-bin LIU,An-min ZHENG. Progress in the Studies on Sn-Zeolites by Solid-State Nuclear Magnetic Resonance[J]. Chinese Journal of Magnetic Resonance, 2021, 38(4): 571-584.
Fig.1
(A) 119Sn MAS NMR spectra of Sn-Beta after different treatments: (a) Calcined; (b) Dehydrated after calcination; (c) Rehydrated after step (b). (B) (a) 119Sn MAS and (b~d) 1H-119Sn CP MAS NMR spectra of dehydrated Sn-Beta. The CP contact times from 1H to 119Sn were varied: (b) 0.2 ms, (c) 1.0 ms, (d) 2.0 ms. (C) 1H-119Sn CP-CPMG MAS NMR spectra of 119Sn-Beta sample dehydrated under vacuum conditions at different temperatures. (D) 119Sn DP-CPMG MAS NMR spectra of (a) dehydrated and (b) hydrated Sn-Beta. The spinning sidebands are marked as asterisks (Reproduced from Refs. [6] and [26])
Fig.2
(a) Variation of 119Sn DP-CPMG MAS NMR spectra of 119Sn-Beta with time after exposure to water (H2O/Sn=4); (b) Variation of the normalized integrated intensity of 119Sn MAS NMR signals at ca. ?581, ?689, and ?703 ppm with time of exposure to water; (c) Dissociative adsorption scheme of water over tin sites in Sn-Beta (Reproduced from Ref. [26])
Fig.3
(a) 1H MAS NMR spectra of dehydrated Sn-Beta before and after exposure to water vapors for 70 h; (b) Time-resolved 1H MAS NMR spectra acquired during the hydration of Sn-Beta; (c) Normalized intensities of 1H and 119Sn MAS NMR signals vs. hydration time; (d, e) Two different hydration mechanism in dehydrated Sn-Beta (Reproduced from Ref. [27])
Fig.4
Two-dimensional 1H-119Sn HMQC MAS NMR spectra of Sn-Beta. (a) Without dehydration; (b) Dehydrated at 298 K; (c) Dehydrated at 393 K without 119Sn decoupling; (d) Dehydrated at 393 K with 119Sn decoupling (Reproduced from Ref. [36])
Fig.5
(a) 31P-TMP NMR spectra of Sn-MFI zeolite under different methanol pressure; (b) The Lewis and Brønsted acid amounts of Sn-MFI zeolite under different methanol pressure (Reproduced from Ref. [13])
Fig.6
(a) 31P MAS NMR spectra of TMPO dosed on Sn-Beta at different loading levels; (b) 119Sn and 31P MAS NMR spectra of 119Sn-Beta with different TMPO loadings (Reproduced from Ref. [45])
Fig.7
Site time yield (STY) for (a) glucose isomerization in water and (b) aldol condensation of benzaldehyde and acetone in toluene catalyzed by different Sn-Beta catalysts plotted against the percent integrated 31P peak area normalized by P and Sn content at (a) δiso = 55.8 and 54.9 ppm and (b) δiso = 58.6 and 57.2 ppm (Reproduced from Ref. [45])
Fig.8
(a) 31P MAS and (b) 13C CP MAS NMR spectra of Si-Beta and Sn-containing Beta zeolites recorded after adsorption of TMPO and 2-13C-acetone, respectively. (c) 1H MAS NMR or difference spectra of various dehydrated Sn-containing Beta zeolites recorded before and after adsorption of ammonia (Reproduced from Ref. [46])
Fig.9
Catalytic performance of the Sn-containing catalysts in the (a) BV oxidation of cyclohexanone and (b) cyclohexene oxide hydration, as well as the plots of reaction rates as a function of the number of accessible LAS (Reproduced from Ref. [46])
Fig.10
15N CP MAS NMR of pyridine adsorbed on metal-substituted zeolites (Reproduced from Ref. [48])
Fig.11
(A) 13C MAS NMR of (a) glucose adsorbed into Si-Beta, (b) fructose adsorbed into Si-Beta, (c) glucose adsorbed into Sn-Beta, (d) fructose adsorbed into Sn-Beta. (B) Spectra from fructose adsorbed into Sn-Beta: (a) CP contact time of 0.1 ms; (b) CP contact time of 1.0 ms; and (c) no CP (Reproduced from Ref. [6])
Fig.12
(A) 13C CP MAS NMR spectra of (a) 30 μmol⋅g?1 and (b) 100 μmol⋅g?1 of 2-13C-acetone adsorbed on Sn-Beta zeolite dehydrated at 393 K, (c) 30 μmol⋅g?1 and (d) 100 μmol⋅g?1 of 2-13C-acetone adsorbed on Sn-Beta zeolite dehydrated at 673 K. (B) Proposed catalytic cycle for the reaction between acetone and cyclohexanol on Sn-Beta zeolite. (Reproduced from Ref. [50])
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