高性能气体分离炭膜的设计与制备
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- 英文论文题名：Design and preparation of carbon membranes with high performance for gas separation
- 论文作者：徐瑞松 ; 李琳 ; 宋晶 ; 金鑫 ; 王春雷 ; 鲁云华 ; 王同华
- 英文论文作者：XU Ruisong ; LI Lin ; SONG Jing ; JIN Xin ; WANG Chunlei ; LU Yunhua ; WANG Tonghua ; State Key Laboratory of Fine Chemicals ; Carbon research Laboratory ; R&D Center of Membrane Science ; School of Chemical Engineering ; Dalian University of Technology
- 年：2016
- 作者机构：大连理工大学化工学院精细化工国家重点实验室碳素材料研究室膜科学与技术研究开发中心;
- 论文关键词：气体分离 ; 炭膜 ; 高性能 ; 刚性 ; 高自由体积
- 英文论文关键词：gas separation ; carbon membrane ; high performance ; rigidity ; high free volume
- 会议召开时间：2016-11-25
- 会议录名称：第五届全国膜分离技术在冶金工业中应用研讨会论文集
- 语种：中文
- 分类号：TQ051.893
- 学会代码：LXJT
- 会议名称：第五届全国膜分离技术在冶金工业中应用研讨会
- 会议地点：中国湖南长沙
- 主办单位：中国膜工业协会、中南大学
- 学会名称：中国蓝星(集团)总公司膜科学与技术编辑部
- 页数：5
- 文件大小：332k
- 原文格式：O
- 会议级别：全国
摘要
炭膜是由有机聚合物经高温热解炭化制备而成的一种新型炭基膜材料.从炭膜前驱体的化学结构设计出发,选择开发和自主合成了2种新型的刚性、高自由体积的聚合物-含有Cardo侧基的酚酞型聚芳醚酮(PEK-C)和含芴基共聚聚酰亚胺(BAF:BAHF(1:1)-6FDA),经过高温热解炭化制得炭膜.两种炭膜对小分子气体都具有较高的气体渗透性能,其中CO_2的渗透系数分别最高可达8 111 Barrer和24 770 Barrer(1 Barrer=1×10~(-10)cm~3(STP)cm/cm~2 s cmHg),对CO_2/CH_4、CO_2/N_2和O_2/N_2混合气体的分离性能远超过聚合物膜的Robeson上限,在天然气的提纯、空气的分离和冶金工业用气体的处理等方面具有很大工业化应用的潜力.
Carbon membrane is the novel porous carbon-based membrane material,which prepared by the pyrolysis of the polymeric precursors.In this paper,two novel polymers of high rigidity and high free volume were developed and synthesized for the preparation of carbon membranes,including phenolphthalein-based poly(arylene ether ketone)(PEK-C) with cardo groups and copolyimide(BAF:BAHF(1:1)-6FDA) with fluorenyl groups.Carbon membranes prepared by two types of polymeric precursors show high gas permeability for small-molecule gases,especially for CO_2 which was up to 8 111 Barrer and 24 770 Barrer(1 Barrer =1×10~(-10) cm~3(STP) cm/cm~2 s cmHg),respectively.Moreover,the gas separation properties of these carbon membranes for mixed gases of CO_2/CH_4,CO_2/N_2 and O_2/N_2surpassed Robeson upper bound of polymer membranes,which possess great potential for industrial application such as purification of natural gases,air separation,processing of metallurgical industrial gases.
Carbon membrane is the novel porous carbon-based membrane material,which prepared by the pyrolysis of the polymeric precursors.In this paper,two novel polymers of high rigidity and high free volume were developed and synthesized for the preparation of carbon membranes,including phenolphthalein-based poly(arylene ether ketone)(PEK-C) with cardo groups and copolyimide(BAF:BAHF(1:1)-6FDA) with fluorenyl groups.Carbon membranes prepared by two types of polymeric precursors show high gas permeability for small-molecule gases,especially for CO_2 which was up to 8 111 Barrer and 24 770 Barrer(1 Barrer =1×10~(-10) cm~3(STP) cm/cm~2 s cmHg),respectively.Moreover,the gas separation properties of these carbon membranes for mixed gases of CO_2/CH_4,CO_2/N_2 and O_2/N_2surpassed Robeson upper bound of polymer membranes,which possess great potential for industrial application such as purification of natural gases,air separation,processing of metallurgical industrial gases.
引文
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[9]费明月.含羟基聚酰亚胺的合成及性能研究[D].辽宁:辽宁科技大学,2013.
[10]鲁云华,雷蕾,肖国勇.双胺芴基共聚聚酰亚胺的合成与性能研究[J].绝缘材料,2016,49:11-14.
[11]Park H B,Jung C H,Lee Y M Polymers with cavities tuned for fast selective transport of small molecules and ions[J].Science,2007,318:254-258.
[12]Sanders D F,Smith Z P,Freeman B D.Gas permeability,diffusivity,and free volume of thermally rearranged polymers based on 3,3-dihydroxy-4,4-diamino-biphenyl(HAB)and 2,2'-bis-(3,4-dicarboxyphenyl)hexafluoropropane dianhydride(6FDA)[J].J Membr Sci,2012,409-410:232-241.
[13]Rungta M H,Xu L R,KorosWJ.Structure-performance characterization for carbon molecular sieve membranes using molecular scale gas probes[J].Carbon,2015,85:429-442.
[14]Robeson L M The upper bound revisited[J].J Membr Sci,2008,320:390-400.
[15]Swaidan R,Ma X H,Pinnau L High pressure pureand mixed-gas separation of CO_2/CH_4 by thermally-rearranged and carbon molecular sieve membranes derived from a polyimide of intrinsic microporosity[J].J Membr Sci,2013,447:387-394.
[2]Salleh W N W,Ismail A F,Matsuura T.Precursor selection and process conditions in the preparation of carbon membrane for gas separation:A review[J].Sep Purif Rev,2011,40:261-311.
[3]王同华,李琳,曹义鸣.气体分离炭膜的结构设计、制备及功能化[J].膜科学与技术,2008:48-54.
[4]Song C W,Wang T H,Jiang H W.Gas separation performance of C/CMS membranes derived from poly(furfuryl alcohol)(PFA)with different chemical structure[J].J Membr Sci,2010,361:22-27.
[5]Zhang B,Wang T H,Liu S L.Structure and morphology of microporous carbon membrane materials derived from poly(phthalazinone ether sulfone ketone)[J].Microp Mesop Mater,2006,96:79-83.
[6]Zhang B,Wang T H,Wu Y H.Preparation and gas permeation of composite carbon membranes from poly(phthalazinone ether sulfone ketone)[J].Sep Purif Technol,2008,60:259-263.
[7]Qiu W L,Zhang K,Koros W J.Gas separation performance of carbon molecular sieve membranes based on6FDA-mPDA/DABA(3:2)Polyimide[J].Chem Sus Chem,2014,7:1186-1194.
[8]Li L,Wang T H,Liu Q L.A high CO_2 permselective mesoporous silica/carbon composite membrane for CO_2separation[J].Carbon,2012,50:5186-5195.
[9]费明月.含羟基聚酰亚胺的合成及性能研究[D].辽宁:辽宁科技大学,2013.
[10]鲁云华,雷蕾,肖国勇.双胺芴基共聚聚酰亚胺的合成与性能研究[J].绝缘材料,2016,49:11-14.
[11]Park H B,Jung C H,Lee Y M Polymers with cavities tuned for fast selective transport of small molecules and ions[J].Science,2007,318:254-258.
[12]Sanders D F,Smith Z P,Freeman B D.Gas permeability,diffusivity,and free volume of thermally rearranged polymers based on 3,3-dihydroxy-4,4-diamino-biphenyl(HAB)and 2,2'-bis-(3,4-dicarboxyphenyl)hexafluoropropane dianhydride(6FDA)[J].J Membr Sci,2012,409-410:232-241.
[13]Rungta M H,Xu L R,KorosWJ.Structure-performance characterization for carbon molecular sieve membranes using molecular scale gas probes[J].Carbon,2015,85:429-442.
[14]Robeson L M The upper bound revisited[J].J Membr Sci,2008,320:390-400.
[15]Swaidan R,Ma X H,Pinnau L High pressure pureand mixed-gas separation of CO_2/CH_4 by thermally-rearranged and carbon molecular sieve membranes derived from a polyimide of intrinsic microporosity[J].J Membr Sci,2013,447:387-394.