【摘要】：CO_2加氫在鐵基催化劑上直接制取高附加值化學(xué)品是實(shí)現(xiàn)其資源化利用的重要途徑。通過(guò)等體積浸漬法制備了不同硅鋁比(25,70,150)的ZSM-5負(fù)載的鐵基催化劑,考察硅鋁比對(duì)鐵基催化劑上CO_2加氫性能的影響。結(jié)果表明,隨著硅鋁比的升高,催化劑活性先升高后降低,最優(yōu)化硅鋁比為70。CO_2-DRIFTS和CO_2-TPD結(jié)果顯示,硅鋁比為70的ZSM-5載體制備的催化劑具有較多且較強(qiáng)的表面堿性位,促進(jìn)CO_2分子的活化解離。通過(guò)H2-TPR、XRD、Raman等表征揭示了催化劑結(jié)構(gòu)的演變過(guò)程。還原后催化劑的活性金屬以單質(zhì)Fe形式存在,反應(yīng)過(guò)程中單質(zhì)Fe向Fe3O4和Fe Cx物種轉(zhuǎn)化。不同硅鋁比配位環(huán)境影響Fe與C的相互作用,影響FeC_x的生成,從而影響CO_2加氫的活性和選擇性。
[Abstract]:It is an important way to make high added value chemicals from CO_2 hydrogenation on iron-based catalysts. Iron based catalysts supported on ZSM-5 with different Si / Al ratios (25 / 70150) were prepared by equal volume impregnation method. The effect of Si / Al ratio on the hydrogenation of CO_2 was investigated. The results showed that with the increase of Si / Al ratio, the activity of the catalyst first increased and then decreased. The optimum ratio of Si to Al was 70.CO_2-DRIFTS and CO_2-TPD. The results showed that the catalyst prepared by ZSM-5 support with Si / Al ratio of 70 had more and stronger surface alkaline sites. Promote the activation and dissociation of CO_2 molecules. The evolution of the catalyst structure was revealed by Raman characterization of the catalyst. The active metal of the catalyst after reduction exists in the form of elemental Fe, and during the reaction, the Fe is transformed into Fe3O4 and FeCx species. The interaction between Fe and C, the formation of FeC_x and the activity and selectivity of CO_2 hydrogenation were affected by the coordination environment of Si / Al ratio.
【作者單位】： 化學(xué)工程聯(lián)合國(guó)家重點(diǎn)實(shí)驗(yàn)室華東理工大學(xué);
【基金】：國(guó)家自然科學(xué)基金項(xiàng)目(21576084,91534127) 科技部國(guó)際合作項(xiàng)目(2015DFG42570)~~
【分類(lèi)號(hào)】：O643.36

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