A polynuclear complex, {[Cu(bpe)2](NO3)},with interpenetrated diamondoid networks:: synthesis, properties and catalytic behavior

被引:41
作者
Parvulescu, AN
Marin, G
Suwinska, K
Kravtsov, VC
Andruh, M
Pârvulescu, V
Pârvulescu, VI
机构
[1] Univ Bucharest, Fac Chem, Inorgan Chem Lab, Bucharest, Romania
[2] Polish Acad Sci, Inst Chem Phys, PL-01224 Warsaw, Poland
[3] Moldavian Acad Sci, Inst Appl Phys, Xray Lab, Kishinev 2028, Moldova
[4] Inst Chem Phys, Bucharest 060021, Romania
[5] Univ Bucharest, Fac Chem, Dept Chem Technol & Catalysis, Bucharest, Romania
关键词
D O I
10.1039/b506786c
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A polynuclear complex {[Cu(bpe)(2)](NO3)} (1), with five-fold interpenetrated diamondoid nets, was synthesized following a hydrothermal procedure, starting from a copper(II) salt, Cu(NO3)(2)(.)2.5H(2)O, and using a molar ratio Cu(NO3)(2) : monoethanolamine : bpe : H2O of 1 : 3 : 1 : 500. The well stirred mixture was introduced into a Teflon-lined stainless steel autoclave, heated at 423 K, and kept at this temperature for 3 days. Red single crystals containing complex 1 were fully characterized by chemical analysis, FTIR, single-crystal X-ray diffraction, powder XRD, DR-UV-Vis, TG-heat flow analysis, sorption isotherms of N-2 at 77 K, and X- ray photoelectron spectroscopy ( XPS). The characterization results indicated that these crystals corresponded to a copper-organic network with a microporous-like structure in which part of the channels are blocked by water molecules and nitrate ions. The synthesis led to a structure in which all the Cu ions were well stabilized as a Cu( I) species, although the precursor was a Cu(II) compound. This structure exhibits remarkable properties: high thermal stability and capacity to totally exchange NO3 2 anions, without causing any damage to the microporous texture. The catalytic behavior was investigated in NO decomposition and NO reduction with hexane in the presence of O-2, revealing very interesting and high catalytic activity. Cu was well preserved in a Cu(I) state after the catalytic tests, which provided new information about the mechanism of NO reaction on copper.
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收藏
页码:4234 / 4240
页数:7
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