title: In situ template generation via N-alkylation in the syntheses of open-framework zinc phosphites and phosphate.
abstract: 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][Zn3(HPO3)4] I (pmpip = N,N,N',N'-tetramethyl-2-methylpiperazinium), [dmdabco][Zn3(HPO3)4] II (dmdabco = N,N'-dimethyl-1,4-diazabicyclo[2,2,2]octane) and [Hmampy][Zn2(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.
authors.affiliation: Teachers College, College of Chemistry, Chemical Engineering and Environment of Qingdao University, Shandong 266071, P. R. China. gmwang_pub@163.com.
authors.forename: Guoming
authors.initials: G
authors.lastname: Wang
authors.forename: Jinhua
authors.initials: J
authors.lastname: Li
authors.forename: Xiao
authors.initials: X
authors.lastname: Zhang
authors.forename: Pei
authors.initials: P
authors.lastname: Wang
authors.forename: BeiBei
authors.initials: B
authors.lastname: Pang
authors.forename: Zonghua
authors.initials: Z
authors.lastname: Wang
authors.forename: Yingxia
authors.initials: Y
authors.lastname: Wang
authors.forename: Jianhua
authors.initials: J
authors.lastname: Lin
authors.forename: Chunyang
authors.initials: C
authors.lastname: Pan