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Tailoring a Thermally Stable Amorphous SiOC Structure for the Separation of Large Molecules: The Effect of Calcination Temperature on SiOC Structures and Gas Permeation Properties
ACS Omega ( IF 4.1 ) Pub Date : 2018-06-13 00:00:00 , DOI: 10.1021/acsomega.8b00632
Hiroki Inde , Masakoto Kanezashi , Hiroki Nagasawa , Toshimi Nakaya , Toshinori Tsuru

A SiOC membrane with high oxidative stability for gas separation was tailored by utilizing vinyltrimethoxysilane, triethoxysilane, and 1,1,3,3-tetramethyldisiloxane as Si precursors. Amorphous SiOC networks were formed via the condensation of Si–OH groups, the hydrosilylation of Si–H and Si–CH═CH2 groups, and a crosslinking reaction of Si–CH3 groups, respectively. The crosslinking of Si–CH3 groups at temperatures ranging from 600 to 700 °C under a N2 atmosphere was quite effective in constructing a Si–CH2–Si unit without the formation of mesopores, which was confirmed by the results of N2 adsorption and by the gas permeation properties. The network pore size of the SiOC membrane calcined at 700 °C under N2 showed high oxidative stability at 500 °C and was appropriate for the separation of large molecules (H2/CF4 selectivity: 640, H2/SF6: 2900, N2/CF4: 98). A SiOC membrane calcined at 800 °C showed H2/N2 selectivity of 62, which was approximately 10 times higher than that calcined at 700 °C because the SiOC networks were densified by the cleavage and redistribution reactions of Si–C and Si–O groups.

中文翻译:

量身定制用于分离大分子的热稳定非晶SiOC结构:煅烧温度对SiOC结构和气体渗透性能的影响

通过使用乙烯基三甲氧基硅烷,三乙氧基硅烷和1,1,3,3-四甲基二硅氧烷作为Si前体,定制出具有高氧化稳定性的气体分离SiOC膜。分别通过Si–OH基团的缩合,Si–H和Si–CH═CH 2基团的氢化硅烷化以及Si–CH 3基团的交联反应形成非晶SiOC网络。N 2气氛下,在600至700°C的温度范围内,Si-CH 3基团的交联非常有效地构建了Si-CH 2 -Si单元,而没有形成中孔,这一点已由N 2的结果证实吸附和受气体渗透的特性。N 2下在700°C下煅烧的SiOC膜的网络孔径在500°C下显示出高氧化稳定性,适合分离大分子(H 2 / CF 4选择性:640,H 2 / SF 6:2900 ,N 2 / CF 4:98)。在800°C煅烧的SiOC膜显示H 2 / N 2选择性为62,比在7​​00°C煅烧的SiOC膜高约10倍,因为SiOC网络通过Si–C和Si–2的裂解和再分布反应而致密化O组。
更新日期:2018-06-13
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