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聚芳撑乙炔微孔骨架材料的合成及其气体吸附
  • ISSN号:0567-7351
  • 期刊名称:《化学学报》
  • 时间:0
  • 分类:O626[理学—有机化学;理学—化学]
  • 作者机构:[1]武汉工程大学化工与制药学院,武汉430073, [2]陕西师范大学材料科学与工程学院,西安710062
  • 相关基金:项目受国家自然科学基金(No.51103111)和教育部新世纪优秀人才支持计划(No.NCET-12-0714)资助.
中文摘要:

有机微孔聚合物(MOPs)在气体存储、吸附分离和非均相催化等领域具有优良性质而广受关注.近年来,聚芳撑乙炔微孔骨架材料的研究成为MOPs领域中的热点.分别以三(4-乙炔基)苯胺、甲基三(4-乙炔基苯基)Ni烷、苯基三(4-乙炔基苯基)硅烷为基本构筑单元,通过端炔基氧化均聚的方法,制备了三种聚芳撑乙炔微孔骨架材料,研究了结构组成对制备聚合物孔道性能和气体吸附性能的影响.氮气吸附测试结果表明,聚合物的Brunauer-Emmett—Teller(BET)比表面积的范围在602-715m2·g^-1.由于骨架中含有富氮基团(三苯胺)以及具有较大的比表面积,在1.13bar/273K条件下,聚三(4-乙炔基)苯胺(TEPA—MOP)的C02吸附能力为1.59mmol·g^-1.此外,TEPA—MOP和聚苯基三(4-乙炔基苯基)硅烷(TEPP.MOP)具有优良的选择性吸附性能,对C02/N2的选择性吸附分别是69.9和73.2.聚合物TEPA-MOP具有优异的CO2/N2的选择吸附性和适中的C02吸附能力,因此将在气体吸附与分离方面具有潜在的应用前景.

英文摘要:

Microporous organic polymers (MOPs) have drawn much attention because of their potential applications such as gas storage, separation and heterogeneous catalysis. There is great interest in the design, synthesis and property evaluation of poly(arylene ethynylenes) (PAEs) with intrinsic microporosity. In addition to Sonogashira Coupling reaction between terminal alkynes and halides, the oxidative dimerization of terminal alkynes is an alternating strategy for the buildup of the mi- croporous PAE frameworks. In this paper, a series of MOPs were synthesized by the oxidative dimerization of terminal al- kynes using triethynyl monomers such as tris(4-ethynylphenyl)amine, tris(4-ethynylphenyl)methylsilane and poly- tris(4-ethynylphenyl)phenylsilane. The resulting MOPs were characterized by FT-IR spectra, thermogravimetric analysis (TGA), scanning electron microscopy (SEM), transmission electron microscopy (TEM), powder X-ray diffraction (PXRD) measurements. FT-IR spectra indicate the success of the homocoupling reaction for constructing the dialkyne-bridged poly- mer frameworks. These polymer frameworks exhibit high thermal stability with onset of decomposition temperature above 350 ℃ at 5% mass loss under nitrogen flow. PXRD and TEM measurements revealed that alt the polymer frameworks are amorphous solid in nature. These dialkyne-bridged MOPs exhibit moderate surface areas ranging from 602 to 715 m2·g^-1. The incorporation of triphenylamine moieties into the polymer skeleton increases the number of electron donating basic ni- trogen sites in the porous frameworks. Thus, the triphenylamine-based polymer polytris(4-ethynylphenyl)amine (TE- PA-MOP) with the highest Brunauer-Emmett-Teller (BET) surface area shows the highest CO2 uptake capacity of 1.59 mmol·g^-1 at 273 K and 1.13 bar among the resulting polymer frameworks. In addition, TEPA-MOP showed the highest 1-12 adsorption up to 1.04 wt% at 1.13 bar and 77 K and polytris(4-ethynylphenyl)phenylsilane (TEP

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期刊信息
  • 《化学学报》
  • 北大核心期刊(2014版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院上海有机化学研究所
  • 主编:周其林
  • 地址:上海市零陵路345号
  • 邮编:200032
  • 邮箱:hxxb@sioc.ac.cn
  • 电话:021-54925085
  • 国际标准刊号:ISSN:0567-7351
  • 国内统一刊号:ISSN:31-1320/O6
  • 邮发代号:4-209
  • 获奖情况:
  • 首届国家期刊奖,第二届国家期刊奖提名奖,中国期刊方阵“双高期刊”
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国科学引文索引(扩展库),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:28694