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Microporosity and CO2 Capture Properties of Amorphous Silicon Oxynitride Derived from Novel Polyalkoxysilsesquiazanes

机译:新型聚烷氧基硅倍半氮衍生的非晶态氮氧化硅的微孔性和CO2捕获特性

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摘要

Polyalkoxysilsesquiazanes ([ROSi(NH)1.5]n, ROSZ, R = Et, nPr, iPr, nBu, sBu, nHex, sHex, cHex, decahydronaphthyl (DHNp)) were synthesized by ammonolysis at −78 °C of alkoxytrichlorosilane (ROSiCl3), which was isolated by distillation as a reaction product of SiCl4 and ROH. The simultaneous thermogravimetric and mass spectrometry analyses of the ROSZs under helium revealed a common decomposition reaction, the cleavage of the oxygen–carbon bond of the RO group to evolve alkene as a main gaseous species formed in-situ, leading to the formation of microporous amorphous Si–O–N at 550 °C to 800 °C. The microporosity in terms of the peak of the pore size distribution curve located within the micropore size range (<2 nm) and the total micropore volume, as well as the specific surface area (SSA) of the Si–O–N, increased consistently with the molecular size estimated for the alkene formed in-situ during the pyrolysis. The CO2 capture capacity at 0 °C of the Si–O–N material increased consistently with its SSA, and an excellent CO2 capture capacity of 3.9 mmol·g−1 at 0 °C and CO2 1 atm was achieved for the Si–O–N derived from DHNpOSZ having an SSA of 750 m2·g−1. The CO2 capture properties were further discussed based on their temperature dependency, and a surface functional group of the Si–O–N formed in-situ during the polymer/ceramics thermal conversion.
机译:聚烷氧基硅倍半氮烷([ROSi(NH)1.5] n,ROSZ,R = Et,nPr,iPr,nBu,sBu,nHex,sHex,cHex,十氢萘基(DHNp))是在-78°C的烷氧基三氯硅烷(ROSiCl3)氨解法合成的通过蒸馏将其分离为SiCl 4和ROH的反应产物。氦气下的ROSZ的同时热重分析和质谱分析揭示了一个常见的分解反应,RO基团的氧碳键断裂,以发展烯烃作为原位形成的主要气态物质,导致形成了微孔无定形物。 Si–O–N在550°C至800°C的温度下。就位于微孔尺寸范围(<2 nm)内的孔径分布曲线的峰值而言,微孔性和总的微孔体积以及Si–O–N的比表面积(SSA)一直在增加估计在热解过程中原位形成的烯烃的分子大小。 Si–O–N材料在0°C时的CO2捕集能力与其SSA一致,并且在0°C和1 atm时的出色CO2捕集能力分别为3.9 mmol·g -1 源自DHNpOSZ的SSA为750 m 2 ·g -1 的Si-O-N达到了。根据它们对温度的依赖性以及在聚合物/陶瓷热转化过程中原位形成的Si–O–N的表面官能团,进一步讨论了CO2的捕获特性。

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