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题名: Investigation of the Strong Bronsted Acidity in a Novel SAPO-type Molecular Sieve, DNL-6
作者: Su, Xiong1;  Xu, Shutao1;  Tian, Peng1;  Li, Jinzhe1;  Zheng, Anmin3;  Wang, Qiang3;  Yang, Miao1;  Wei, Yingxu1;  Deng, Feng3;  Liu, Zhongmin1, 2
刊名: JOURNAL OF PHYSICAL CHEMISTRY C
发表日期: 2015-02-05
DOI: 10.1021/jp511670q
卷: 119, 期:5, 页:2589-2596
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Science & Technology - Other Topics ;  Materials Science
英文摘要: By applying analysis of multiple solid-state MAS NMR spectra, the atomic coordination environment and acidity of a novel SAPO-type molecular sieve, DNL-6, are studied. 27Al MQ-MAS NMR and 31P27Al MQ-HETCOR NMR spectra reveal the existence of a SiAlSi region with Al(OSi)n (n = 14) species in the framework of DNL-6, explaining well the high concentration of single Si(OAl)4 species (3 mmol/g) accommodated in the sample. 13C MAS NMR of 2-13C-acetone adsorption indicates that there exist two kinds of strong Bronsted acid sites in DNL-6. One of them has similar strength as those in HZSM-5 and the other is even stronger, which is unusual in SAPO-type molecular sieves. Also, a discrepancy in Bronsted acid concentration between the theoretical and 1H NMR experimental results has been found, revealing the occurrence of a dehydoxylation process during the calcination. The origin of the extremely strong Bronsted acid sites in DNL-6 is investigated by density functional theory calculations, which suggest that the dehydroxylation process may lead to a local structure deformation and remarkably enhance the Bronsted acidity. More importantly, DNL-6 exhibits excellent catalytic activity in the synthesis of methylamines due to its stronger acidity.
关键词[WOS]: SOLID-STATE NMR ;  ANGLE-SPINNING NMR ;  RESOLUTION HETERONUCLEAR CORRELATION ;  DIFFERENT FRAMEWORK TOPOLOGIES ;  HETEROGENEOUS CATALYSIS ;  QUADRUPOLAR NUCLEI ;  ZEOLITES ;  SPECTROSCOPY ;  SILICOALUMINOPHOSPHATES ;  CHEMISTRY
语种: 英语
WOS记录号: WOS:000349136400040
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/145979
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Natl Engn Lab Methanol Olefins, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Sate Key Lab Catalysis, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
3.Chinese Acad Sci, State Key Lab Magnet Resonance and Atom Mol Phys, Wuhan Ctr Magnet Resonance, Inst Phys & Math, Wuhan 430071, Peoples R China

Recommended Citation:
Su, Xiong,Xu, Shutao,Tian, Peng,et al. Investigation of the Strong Bronsted Acidity in a Novel SAPO-type Molecular Sieve, DNL-6[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2015,119(5):2589-2596.
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