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Investigation of the Strong Bronsted Acidity in a Novel SAPO-type Molecular Sieve, DNL-6
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
2015-02-05
DOI10.1021/jp511670q
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
关键词[WOS]SOLID-STATE NMR ; ANGLE-SPINNING NMR ; RESOLUTION HETERONUCLEAR CORRELATION ; DIFFERENT FRAMEWORK TOPOLOGIES ; HETEROGENEOUS CATALYSIS ; QUADRUPOLAR NUCLEI ; ZEOLITES ; SPECTROSCOPY ; SILICOALUMINOPHOSPHATES ; CHEMISTRY
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.
语种英语
WOS记录号WOS:000349136400040
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/145979
专题中国科学院大连化学物理研究所
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
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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.
APA Su, Xiong.,Xu, Shutao.,Tian, Peng.,Li, Jinzhe.,Zheng, Anmin.,...&Liu, Zhongmin.(2015).Investigation of the Strong Bronsted Acidity in a Novel SAPO-type Molecular Sieve, DNL-6.JOURNAL OF PHYSICAL CHEMISTRY C,119(5),2589-2596.
MLA Su, Xiong,et al."Investigation of the Strong Bronsted Acidity in a Novel SAPO-type Molecular Sieve, DNL-6".JOURNAL OF PHYSICAL CHEMISTRY C 119.5(2015):2589-2596.
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