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用分子模拟方法对6FDA-durene、6FDA-pPDA及其共聚物6FDA-durene/pPDA的链间距及自由体积进行了模拟计算,结果与文献实验值一致;采用巨正则Monte Carlo(GCMC)方法模拟了O2、N2、CH4和CO2在聚酰亚胺中的溶解,计算结果表明:COMPASS力场能较准确地描述O2、N2和CH4在聚酰亚胺中的吸附溶解,O2、N2、CH4的溶解系数模拟结果与实验数据吻合较好。CO2的溶解系数计算值与实验值偏差较大(约50%),主要原因可能在于模拟过程中未考虑体积溶胀效应以及COMPASS力场不能精确描述CO2与—CF3基团的相互作用。同一聚合物中,计算所得气体溶解系数的大小顺序为CO2>CH4>O2>N2,与气体凝聚性趋势一致,同种气体在6FDA型聚酰亚胺中的溶解系数与其自由体积分数变化趋势一致。3种聚合物对CO2/CH4的溶解选择性高于O2/N2,共聚物与均聚物相比,气体溶解选择性没有明显提高。 相似文献
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利用滴管炉研究了O2/N2、O2/CO2和O2/CO2/NO气氛下煤燃烧过程中NOx的排放特性。实验结果表明,在O2/N2和O2/CO2气氛下,高温或高O2浓度均使NO排放量增加。O2/CO2气氛下NO排放量比O2/N2气氛下NO排放量低大约30%~40%。在O2/CO2/NO气氛下,温度不同时,O2浓度变化对NO排放量的影响规律不同,对循环NO降解的影响规律也不同。高温不利于循环NO降解。随停留时间的延长NO排放量出现两个峰值。 相似文献
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甲基丙烯酸二甲氨基乙酯-丙烯腈共聚物膜的制备及其气体渗透性能 总被引:2,自引:0,他引:2
采用水溶液沉淀法合成了甲基丙烯酸二甲氨基乙酯(DM)和丙烯腈(AN)的共聚物,用红外光谱、黏度法和X射线衍射分析了聚合物的结构.实验考察了反应条件对共聚物结构的影响.在此基础上,通过溶液浇注法制备了甲基丙烯酸二甲氨基乙酯(DM)和丙烯腈(AN)的共聚物膜,研究了聚合物膜的CO2、CH4渗透性能.结果表明,由于共聚物中含有能与CO2进行可逆反应的叔胺基,共聚物膜表现出较好的CO2渗透性和CO2/CH4选择性,如在25℃、压力为1140 Pa时,CO2的渗透速率可达 3.53×10-12 cm3(STP)8226;cm-28226;s-18226;Pa-1 , CO2/CH4 的理想分离因子达到104.5.利用膜吸附CO2和CH4后红外光谱的变化,分析了膜对CO2的促进传递机理. 相似文献
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采用共沉淀法制备γ-Al2O3载体和不同Ce添加量的CeO2-Al2O3载体,然后用浸渍法制备Ni负载质量分数10%的Ni/γ-Al2O3和Ni/CeO2-Al2O3催化剂。在固定床微反装置中考察了反应温度、原料气配比和CH4空速等工艺条件对Ni/γ-Al2O3和Ni/Ce30Al70Oδ催化剂在甲烷自热重整制氢反应中催化性能的影响。结果表明,添加Ce的催化剂催化性能有较大提高,在Ni/Ce30Al70Oδ催化剂上,反应温度750 ℃时, CH4转化率94.3%,与Ni/Al2O3催化剂相比,提高20%。Ni/γ-Al2O3和Ni/CeO2-Al2O3催化剂的CH4转化率均随反应温度的升高而增大。原料气中n(O2)∶n(CH4)和n(H2O)∶n(CH4)的增加均能提高各催化剂的CH4转化率。但n(O2)∶n(CH4)和n(H2O)∶n(CH4)的变化对各催化剂的催化性能的影响不同。随着n(O2)∶n(CH4)的增大,产物中n(H2)∶n(CO)降低,n(CO2)∶n(CO+CO2)升高;而n(H2O)∶n(CH4)增大时,产物中n(H2)∶n(CO)和n(CO2)∶n(CO+CO2)均升高。随着CH4空速的增加,Ni/Al2O3催化剂上CH4转化率、n(H2)∶n(CO)和n(CO2)∶n(CO+CO2)均较大程度下降;而在Ni/Ce30Al70Oδ催化剂上,随着CH4空速的增加,CH4转化率、n(H2)∶n(CO)和n(CO2)∶n(CO+CO2)变化不大。 相似文献
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通过溶液共混法制备了聚乙烯基胺(PVAm)/聚乙二醇(PEG)和PVAm/聚N-乙烯基-γ-氨基丁酸钠(PVSA)共混聚合物.分别以这两种共混聚合物为分离层,以聚醚砜超滤膜为支撑层制备了用于分离CO2的固定载体复合膜.研究了共混组成对膜结构和性能的影响,结果表明共混可以改善固定载体膜的透过分离性能.PEG质量含量为10%的PVAm/PEG共混膜具有整体最优的透过分离性能,当温度为25℃、压力为125kPa时,纯CO2渗透速率为4.34×10-9cm3(STP)8226;cm-28226;s-18226;Pa-1,CO2/CH4理想分离因子为63.5;对PVAm/PVSA共混膜,PVSA质量含量为33.3%的膜具有最高的CO2/CH4理想分离因子,而PVSA质量含量为50%的膜具有最高纯CO2渗透速率. 相似文献
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在水平管式炉上研究了O2浓度、CO2浓度、温度及石灰石添加等各参数对O2/CO2气氛下徐州烟煤和龙岩无烟煤燃烧过程中SO2/NO排放特性的影响。结果发现,O2/CO2气氛下,烟煤和无烟煤燃烧SO2/NO的析出规律与空气气氛下不同,同等O2浓度下析出量比空气气氛下小。O2/CO2气氛下,随着O2浓度的提高,烟煤和无烟煤SO2/NO排放量均增大;随着CO2浓度的升高, SO2/NO排放量均减小。O2/CO2气氛下,石灰石添加对SO2排放的抑制作用低于空气气氛下;石灰石添加对NO的排放有一定减排作用。对煤灰的元素分析显示O2/CO2燃烧对SO2的抑制主要是由于煤灰的自固硫能力增强,而对NO的减排作用则是促进燃料N向其他含N气体的转换。 相似文献
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以自由基聚合合成了聚乙烯基吡咯烷酮(PVP),并用其水解产物聚N-乙烯基-γ-氨基丁酸钠(PVSA)和聚砜(PS)超滤膜制备了PVSA/PS复合膜;用红外光谱、X射线衍射等方法研究了PVP及其水解产物PVSA的结构,证实了PVSA含有可作为CO2载体的仲胺基与羧基;测试了复合膜的透气性能及对CO2/CH4的选择性.结果表明,在26℃,压力为1333Pa时,CO2渗透速率可达5.46×10-7 cm3(STP)8226;cm-28226;s-18226;Pa-1,CO2/CH4的理想分离因子达到212.1.随着进料气压力的增大,CO2/CH4的分离因子及CO2的渗透速率均呈下降趋势.依据膜的渗透通量随压力的变化特性以及不同状态下膜的红外光谱,分析了膜对CO2的促进传递机理. 相似文献
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O2/CO2气氛下煤燃烧SO2/NO析出特性 总被引:2,自引:0,他引:2
在水平管式炉上研究了O2浓度、CO2浓度、温度及石灰石添加等各参数对O2/CO2气氛下徐州烟煤和龙岩无烟煤燃烧过程中SO2/NO排放特性的影响。结果发现,O2/CO2气氛下,烟煤和无烟煤燃烧SO2/NO的析出规律与空气气氛下不同,同等O2浓度下析出量比空气气氛下小。O2/CO2气氛下,随着O2浓度的提高,烟煤和无烟煤SO2/NO排放量均增大;随着CO2浓度的升高, SO2/NO排放量均减小。O2/CO2气氛下,石灰石添加对SO2排放的抑制作用低于空气气氛下;石灰石添加对NO的排放有一定减排作用。对煤灰的元素分析显示O2/CO2燃烧对SO2的抑制主要是由于煤灰的自固硫能力增强,而对NO的减排作用则是促进燃料N向其他含N气体的转换。 相似文献
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Ordered mesoporous silica/carbon composite membranes with a high CO2 permeability and selectivity were designed and prepared by incorporating SBA-15 or MCM-48 particles into polymeric precursors followed by heat treatment. The as-made composite membranes were characterized by high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) and N2 adsorption, of which the gas separation performance in terms of gas permeability and selectivity were evaluated using the single gas (CO2, N2, CH4) and gas mixtures (CO2/N2 and CO2/CH4, 50/50 mol.%). In comparison to the pure carbon membranes and microporous zeolite/C composite membranes, the as-made mesoporous silica/C composite membranes, and the MCM-48/C composite membrane in particular, exhibit an outstanding CO2 gas permeability and selectivity for the separation of CO2/CH4 and CO2/N2 gas pairs owing to the smaller gas diffusive resistance through the membrane and additional gas permeation channels created by the incorporation of mesoporous silicas in carbon membrane matrix. The channel shape and dimension of mesoporous silicas are key parameters for governing the gas permeability of the as-made composite membranes. The gas separation mechanism and the functions of porous materials incorporated inside the composite membranes are addressed. 相似文献
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Qingling Liu Tonghua Wang Hongchen Guo Changhai Liang Shili Liu Zhiguo Zhang Yiming Cao Dang Sheng Su Jieshan Qiu 《Microporous and mesoporous materials》2009,120(3):460-466
A simple approach has been developed to synthesize the carbon/zeolite T composite membrane materials with the high gas separation performance. The precursors of the composite membrane are composed of polyimide matrix and dispersed zeolite T particles. The composite membranes prepared by pyrolysis at 973 K show excellent gas (H2, CO2, O2, N2, and CH4) permeability and selectivity (O2/N2, CO2/CH4) for both single gas and mixed-gas. The gas separation performance of the composite membranes can be controlled in a wide range by only changing the zeolite T particle size. The maximum selectivity of O2 over N2 (21/79 mol%) for the composite membranes with the least zeolite T particle (0.5 μm) is 15 with an O2 permeability of 347 Barrers (1 Barrer = 7.5 × 10−18 m2 s−1 Pa−1) and the selectivity of CO2 over CH4 (50/50 mol%) reaches a value of 179 with a CO2 permeability of 1532 Barrers. It is believed that the increase of gas permeability is attributed to the ordered microchannels in the zeolite and the interfacial gaps formed between zeolite and carbon matrix in the composite membranes. And the gas selectivity is tuned by the size of interfacial gaps which are varied with the zeolite particle size. This technique will provide a simple and convenient route to efficiently improve the trade-off relationship between the permeability and the selectivity and enable the construction of carbon-based composite materials with novel functionalities in membrane science. 相似文献
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Summary Physical and gas transport properties of novel hyperbranched polyimide – silica hybrid membranes were investigated. Hyperbranched polyamic acid as a precursor was prepared by polycondensation of a triamine monomer, 1,3,5-tris(4-aminophenoxy)benzene (TAPOB), and a dianhydride monomer, 4,4-(hexafluoro-isopropylidene)diphthalic anhydride (6FDA), and subsequently modified the end groups by 3-aminopropyltrimethoxysilane (APTrMOS). The hyperbranched polyimide – silica hybrid membranes were prepared using the polyamic acid, water, and tetramethoxysilane (TMOS) via a sol-gel technique. 5 % weight-loss temperature and glass transition temperature of the hyperbranched polyimide – silica hybrid membranes determined by TG-DTA measurement considerably increased with increasing silica content, indicating effective cross-linking at polymer – silica interface mediated by APTrMOS moiety. CO2, O2, and N2 permeability coefficients of the hybrid membranes increased with increasing silica content. It was pointed out that the increased gas permeabilities are mainly attributed to increase in the gas solubilities. On the contrary, CH4 permeability of the hybrid membranes decreased with increasing silica content because of decrease in the CH4 diffusivity and, as a result, CO2/CH4 selectivity of the hybrid membranes remarkably increased. It was concluded that the 6FDA-TAPOB hyperbranched polyimide – silica hybrid membranes have high thermal stability and excellent gas selectivity, and are expected to apply to a high-performance gas separation membrane. 相似文献
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Physical and gas transport properties of hyperbranched polyimide-silica hybrid membranes were investigated. Hyperbranched polyamic acid as a precursor was prepared by polycondensation of a triamine, 1,3,5-tris(4-aminophenoxy) benzene (TAPOB), and a dianhydride, 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA), and subsequently modified a part of end groups by 3-aminopropyltrimethoxysilane (APTrMOS). The hyperbranched polyimide-silica hybrid membranes were prepared by sol–gel reaction using the polyamic acid, water, and alkoxysilanes. 5% weight-loss temperature of the hybrid membranes increased with increasing silica content, indicating effective crosslinking at polymer-silica interface mediated by APTrMOS moiety. On the other hand, glass transition temperature of the hybrid membranes prepared with methyltrimethoxysilane (MTMS) showed a minimum value at low silica content region, suggesting insufficient formation of three-dimensional Si O Si network compared to the hybrid membranes prepared with tetramethoxysilane (TMOS). CO2, O2, N2, and CH4 permeability coefficients of the hybrid membranes increased with increasing silica content. Especially for TMOS/MTMS combined system, the hybrid membranes showed simultaneous enhancements of gas permeability and CO2/CH4 separation ability. It was concluded that the 6FDA-TAPOB hyperbranched polyimide-silica hybrid membranes have high thermal stability and excellent CO2/CH4 selectivity and are expected to apply to high-performance gas separation membranes. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008 相似文献
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Seyed Farzad Soleymanipour Amir Hossein Saeedi Dehaghani Vahid Pirouzfar Afahar Alihosseini 《应用聚合物科学杂志》2016,133(34)
The development of desirable chemical structures and properties in nanocomposite membranes involve steps that need to be carefully designed and controlled. This study investigates the effect of adding multiwalled nanotubes (MWNT) on a Kapton–polysulfone composite membrane on the separation of various gas pairs. Data from Fourier transform infrared spectroscopy and scanning electron microscopy confirm that some studies on the Kapton–polysulfone blends are miscible on the molecular level. In fact, the results indicate that the chemical structure of the blend components, the Kapton–polysulfone blend compositions, and the carbon nanotubes play important roles in the transport properties of the resulting membranes. The results of gas permeability tests for the synthesized membranes specify that using a higher percentage of polysulfone (PSF) in blends resulted in membranes with higher ideal selectivity and permeability. Although the addition of nanotubes can increase the permeability of gases, it decreases gas pair selectivity. Furthermore, these outcomes suggest that Kapton–PSF membranes with higher PSF are special candidates for CO2/CH4 separation compared to CO2/N2 and O2/N2 separation. High CH4, CO2, N2, and O2 permeabilities of 0.35, 6.2, 0.34, and 1.15 bar, respectively, are obtained for the developed Kapton–PSF membranes (25/75%) with the highest percentage of carbon nanotubes (8%), whose values are the highest among all the resultant membranes. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43839. 相似文献
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S.S. Madaeni M. Mohammadi Sarab Badieh V. Vatanpour 《Polymer Engineering and Science》2013,53(9):1878-1885
In this study, polydimethylsiloxane (PDMS)‐coated polyethersulfone (PES) composite membrane was prepared for gas separation. “Film casting” and “dip‐coating” techniques were used for producing selective PDMS layer on the surface of the PES support. The effects of coating technique and conditions including coating solution concentration and curing temperature on permselectivity of CO2, CH4, and N2 were investigated. The prepared PES support did not provide any selectivity to the gases. When the concentration of PDMS coating solution was increased, initially permeability of CO2 was rapidly dropped and then gradually reached to an almost constant value. The optimum concentration of coating solution was 5 wt%. Curing temperature showed no pronounced effect on the CO2 permeability and selectivity. In “film casting” method, double coating showed superior permeability and selectivity. However, triple “dip‐coating” was promising. The selectivity of composite membrane prepared by “dip‐coating” was higher than “film casting” method. CO2/N2 and CO2/CH4 selectivity of five sequential dip‐coated composite membranes was 45.5 and 9.3, respectively. POLYM. ENG. SCI., 2013. © 2013 Society of Plastics Engineers 相似文献
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CO2-selective cross-linked poly (ethylene oxide) (PEO) membranes were prepared by the UV irradiation of high molecular weight PEO in the presence of benzophenone as photo-initiator, which act as a hydrogen-abstracting agent. The main goal was to study the effects of the cross-linking process on the structural properties of hydrogel films intended for the gas separation applications. It was found that the gel fraction, and cross-link density enhanced, and the crystallinity, and the size of spherulites decreased by the cross-linking process. Moreover, the permeation performances for N2, O2, CH4, and CO2 and the relationship between the gas permeation performances and physical properties were investigated. The results indicated that the degree of cross-linking and crystallinity could be controlled by changing the initiator concentration, as by increasing the initiator content, the crystallinity percent and gas permeability of the membranes decreased, and the gas pair ideal selectivity of CO2/N2, CO2/CH4, CH4/N2, and O2/N2 increased. 相似文献
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PVAm/PAN复合膜的制备及其对CO2/CH4的分离性能 总被引:1,自引:0,他引:1
New polymeric membrane materials——polyvinyl amine (PVAm) with different primary amine contents were synthesized.By covering polyacrylonitrile(PAN) ultrafiltration membranes with PVAm, the PVAm/PAN composite membranes for CO2/CH4 separation were prepared. The composite membranes containing more primary amino groups have higher selectivity for CO2/CH4.The cross-linking of acid or glutaradehyde could improve the gas permselectivity of the composite membranes. With decreasing CO2 content in the feed gas, the CO2/CH4 separation factor increased.When the feed gas was 25%(vol) CO2 and 75%(vol) CH4, the CO2 permeation rate was 4.1×10-9cm3(STP) 8226;cm-28226;Pa-18226;s-1, and the CO2/CH4 separation factor was 180. 相似文献
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Graphene oxide (GO) nanosheets stacked in parallel with subnanometer channels can exhibit an excellent size-sieving ability for membrane-based gas separation. However, gas molecules have to diffuse through the tortuous nanochannels, leading to low permeability. Herein we demonstrate two versatile approaches to modify the GO (before membrane fabrication by vacuum-filtration) to collectively increase gas permeability, etching using hydrogen peroxide to generate in-plane nanopores and acidifying using hydrochloric acid. For example, a membrane prepared at a pH of 5.0 using the 4-h-etched GO (HGO-4h) shows He permeability of 5.3 Barrer and He/CH4 selectivity of 800, which are 5 times and 1.5 times those of the GO membranes, respectively. Decreasing the pH from 5.0 to 2.0 for HGO-4h enhances He permeability to 57 Barrer and He/CH4 selectivity to 1,800. The HGO-4h prepared at the pH of 2.0 exhibits separation properties of H2/CO2, H2/N2, He/N2, and He/CH4 surpassing their corresponding upper bounds. 相似文献
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《Journal of Industrial and Engineering Chemistry》2014,20(3):1050-1060
[Cellulose acetate (CA)-blend-multi walled carbon nano tubes (MWCNTs)] mixed matrix membranes (MMMs), [CA/polyethylene glycol (PEG)/MWCNTs] and [CA/styrene butadiene rubber (SBR)/MWCNTs] blend MMMs were prepared by solution casting method for gas separation applications using Tetrahydrofuran (THF) as solvent. Both raw-MWCNTs (R-MWCNTs) and functionalized carboxylic-MWCNTs (C-MWCNTs) were used in membrane preparation. The MWCNTs loading ratio and pressure effects on the gas separation performance of prepared membranes were investigated for pure He, N2, CH4 and CO2 gases. Results indicated that utilizing C-MWCNT instead of R-MWCNTs in membrane fabrication has better performance and (CO2/CH4) and (CO2/N2) selectivity reached to 21.81 and 13.74 from 13.41 and 9.33 at 0.65 wt% of MWCNTs loading respectively. The effects of PEG and SBR on the gas transport performance and mechanical properties were also investigated. The highest CO2/CH4 selectivity at 2 bar pressure was reached to 53.98 for [CA/PEG/C-MWCNT] and 43.91 for [CA/SBR/C-MWCNT] blend MMMs at 0.5 wt% and 2 wt% MWCNTs loading ratio respectively. Moreover, increase of feed pressure led to membrane gas permeability and gas pair selectivity improvement for almost all prepared membranes. The mechanical properties analysis exhibited tensile modules improvement with increasing MWCNTs loading ratio and utilizing polymer blending. 相似文献