Low-temperature hydrodeoxygenation of phenol using modified TiO2(B) nanosheets supported highly dispersed Pt catalyst
Low-temperature hydrodeoxygenation of phenol using modified TiO2(B) nanosheets supported highly dispersed Pt catalyst
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DOI：
10.1016/j.fuel.2022.127314
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发表时间：
2023-04
期刊：
影响因子：
7.4
通讯作者：
Xu Li;Long Yan;Zi-Tong Liu;Y. Liao;Longlong Ma
中科院分区：
文献类型：
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作者：
Xu Li;Long Yan;Zi-Tong Liu;Y. Liao;Longlong Ma
含氧化合物的催化加氢脱氧（HDO）是化学精炼的关键，通常在高温、氢压或/和强酸条件下进行。在此，我们开发了一种新型的Pt/TiO 2（B）催化剂用于常压HDO工艺。有机功能化TiO 2（B）纳米片的改性显著提高了Pt/TiO 2（B）催化剂的催化活性。通过高分散的Pt物种和TiO 2（B）载体的协同效应，在50 °C和常压氢气下，苯酚被有效地转化为环己烷和伴随的环己醇，而不需要额外的酸。对催化剂的表征表明，有机官能团的引入不仅有利于形成高分散的Pt物种，而且有利于生成关键的HDO中间体。由于烯醇中间体的C单键O键能较低，因此可以在温和的条件下通过可实现的烯醇中间体的C单键O键断裂来进行苯酚的HDO反应。本研究为绿色加氢脱硫工艺提供了新的认识，为加氢脱硫催化剂的开发提供了新的思路。
Catalytic hydrodeoxygenation (HDO) of oxygenated compounds is essential for chemical refining, which is always carried out under high temperature, hydrogen pressure or/and strong acids. Herein, we developed a novel Pt/TiO2(B) catalyst for the ambient HDO process. With the modified organic functional TiO2(B) nanosheets, the catalytic activity of Pt/TiO2(B) was significantly improved. Through the synergistic effect of highly dispersed Pt species and TiO2(B) supports, phenol was efficiently converted into cyclohexane and concomitant cyclohexanol under 50 °C and atmospheric hydrogen without extra acid. The characterizations of catalysts showed that the introduction of organic functional groups not only led to the formation of highly dispersed Pt species, but was also conducive to the yielding of key HDO intermediates. Due to the low Csingle bondO bond energy of enol intermediates, the HDO of phenol could be carried out at mild conditions through the implementable Csingle bondO bond cleavage of enol intermediates. This study provides a new understanding of the green HDO process and a novel approach for HDO catalyst development.