本文選題：丙烷脫氫 + 一鍋水熱合成��； 參考：《催化學(xué)報》2017年04期

【摘要】：丙烷脫氫制丙烯能夠?qū)⒌图壨闊N轉(zhuǎn)變成烯烴,是有效擴(kuò)大丙烯來源的生產(chǎn)工藝.鉑錫催化劑用于丙烷催化脫氫的主要缺點是穩(wěn)定性差、選擇性低,通過穩(wěn)定錫的氧化態(tài)可以大大改善催化劑的脫氫性能及穩(wěn)定性.本文采用一鍋水熱合成法制備了一系列高比表面積具有高度有序介孔結(jié)構(gòu)的Sn摻雜的Sn-SBA-15材料,并作為載體負(fù)載鉑催化劑用于丙烷脫氫反應(yīng).同時利用傳統(tǒng)浸潰法(IM)合成了Sn/SBA-15-IM材料作為對比.結(jié)合X射線衍射(XRD)、BET比表面積和孔體積測試、紅外光譜(FT-IR)、X射線光電子能譜、H_2程序升溫脫附(H_2-TPD)、熱重分析(TGA)、掃描電鏡和透射電鏡等多種物理化學(xué)表征手段研究了Sn-SBA-15材料和催化劑的結(jié)構(gòu)性質(zhì)及其丙烷脫氫反應(yīng)性能.XRD和BET比表面積和孔體積測試結(jié)果表明,水熱合成法原位引入助劑Sn不影響載體SBA-15的有序孔道結(jié)構(gòu),同時能夠保持較大的比表面積.傳統(tǒng)浸潰法引入Sn會堵塞載體孔道,載體比表面積及孔道有序度下降.Sn摻雜進(jìn)入SBA-15骨架能夠增強(qiáng)Sn物種與載體的相互作用,有利于Sn物種在反應(yīng)過程中保持氧化態(tài),提高催化劑丙烷脫氫反應(yīng)的活性及選擇性.當(dāng)Sn摻雜量增至2.0 wt%時,Pt,Sn組分與載體之間的相互作用減弱,催化劑中Sn~0物種所占比例增多,導(dǎo)致催化劑丙烷脫氫性能下降.在丙烷脫氫反應(yīng)過程中,一鍋法引入Sn的催化劑上反應(yīng)活性和穩(wěn)定性明顯優(yōu)于浸潰法引入Sn的催化劑.其中,Pt/0.5Sn-SBA-15催化劑表現(xiàn)出最優(yōu)的丙烷脫氫性能,丙烷轉(zhuǎn)化率為43.8%,丙烯選擇性為98.5%.
[Abstract]:Dehydrogenation of propane to propylene can transform alkanes into alkenes, which is an effective process to expand propene sources. The main disadvantages of Pt-Sn catalyst for catalytic dehydrogenation of propane are poor stability and low selectivity. The dehydrogenation performance and stability of the catalyst can be greatly improved by stabilizing the oxidation state of tin. In this paper, a series of Sn-doped Sn-SBA-15 materials with high specific surface area and highly ordered mesoporous structure have been prepared by one-pot hydrothermal synthesis method and used as supported platinum catalysts for propane dehydrogenation. At the same time, Sn/SBA-15-IM materials were synthesized by traditional leaching method. The specific surface area and pore volume of BET were measured by X-ray diffraction. The structure and properties of Sn-SBA-15 materials and catalysts for dehydrogenation of propane were studied by means of FTIR, FTIR and X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption of H _ (2) T _ (PDN), thermogravimetric analysis (TGA), scanning electron microscope (SEM) and transmission electron microscope (TEM). XRD and BET specific surface area and pore volume test results show that, The in-situ introduction of Sn by hydrothermal synthesis does not affect the ordered pore structure of the carrier SBA-15, and can maintain a large specific surface area at the same time. The introduction of Sn into the carrier by traditional leaching method can block the pore channel of the carrier, and doping Sn into the SBA-15 skeleton can enhance the interaction between Sn species and the carrier, which is helpful for the Sn species to maintain the oxidation state during the reaction. The activity and selectivity of the catalyst for dehydrogenation of propane were improved. When Sn doping content increased to 2.0 wt%, the interaction between the Sn component and the support was weakened, and the proportion of Sn~0 species in the catalyst increased, which resulted in the degradation of the dehydrogenation performance of propane over the catalyst. In the process of dehydrogenation of propane, the catalytic activity and stability of the catalyst on which Sn is introduced by one-pot method is obviously better than that by leaching method. Among them, Pt- / 0.5Sn-SBA-15 catalyst showed the best dehydrogenation performance of propane, the conversion of propane was 43.8 and the selectivity of propylene was 98.5.
【作者單位】： 四川大學(xué)化學(xué)工程學(xué)院;斯特拉斯堡大學(xué)能源環(huán)境與健康化學(xué)過程研究所;
【基金】：supported by the Science & Technology Support Plan Projects of Sichuan Province (2016GZ0371) National Natural Science Foun-dation of China (NNSFC,21476145,21506111)~~
【分類號】：O643.36
，

本文編號：1844738