In situ template generation via N-alkylation in the syntheses of open-framework zinc phosphites and phosphate

被引:23
作者
Wang, Guoming [1 ]
Li, Jinhua [1 ]
Zhang, Xiao [1 ]
Wang, Pei [1 ]
Pang, BeiBei [1 ]
Wang, Zonghua [1 ]
Wang, Yingxia [2 ]
Lin, Jianhua [2 ]
Pan, Chunyang [3 ]
机构
[1] Qingdao Univ, Coll Chem Chem Engn & Environm, Teachers Coll, Qingdao 266071, Shandong, Peoples R China
[2] Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
[3] Guangdong Univ Technol, Sch Chem Engn & Light Ind, Guangzhou 510006, Guangdong, Peoples R China
关键词
HYDROTHERMAL SYNTHESIS; NICKEL(II) PHOSPHATE; BERYLLIUM PHOSPHITE; GALLIUM PHOSPHATE; 24-RING CHANNELS; MOLECULAR-SIEVE; ZINCOPHOSPHATE; RING; ZEOLITES; COMPLEX;
D O I
10.1039/c3dt51434j
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
In methanol-aqueous solutions, three novel structure-directing agents (SDAs) were generated in situ and presented. These in situ reactions feature N-methylation transformations between CH3OH solvent and organic cyclic aliphatic and aromatic amines, i.e. 2-methylpiperazine, 1,4-diazabicyclo[2,2,2]octane (dabco) and 3-(aminomethyl)pyridine. Distinct from conventional Eschweiler-Clarke methylation containing excess formic acid and formaldehyde, such a direct methylation transformation from methanol molecules is unique. In the presence of new SDAs, three organically templated zinc phosphites/phosphates, [pmpip][Zn-3(HPO3)(4)] I (pmpip = N,N,N',N'-tetramethyl-2-methylpiperazinium),[dmdabco][Zn-3(HPO3)(4)] II (dmdabco = N,N'-dimethyl-1,4-diazabicyclo[2,2,2]octane) and [Hmampy][Zn-2(HPO4)(3)] III (mampy = N-methyl-3-(aminomethyl) pyridine), have been prepared and structurally characterized by elemental analysis, IR, thermogravimetric analysis, powder and single-crystal X-ray diffraction. Compound I exhibits a 2D layer with eight-membered apertures, compounds II and III possess a 3D interrupted framework with intersecting 8-, 10- and 12-ring channels (for II), and 8-, 10-ring channels (for III), respectively.
引用
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页码:13084 / 13091
页数:8
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NATURE, 2005, 437 (7059) :716-719