High efficiency Al modified mesoporous SBA-15 catalyst for biomass-derived γ-valerolactone decarboxylation to butene
High efficiency Al modified mesoporous SBA-15 catalyst for biomass-derived γ-valerolactone decarboxylation to butene
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DOI：
10.1016/j.micromeso.2021.111432
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发表时间：
2021-11
影响因子：
5.2
通讯作者：
Haibiao Yu;Xiu Jia;Peng Wang;Y. Xiong;W. Shan;Congge Zhang;Zhimeng Song
中科院分区：
文献类型：
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作者：
Haibiao Yu;Xiu Jia;Peng Wang;Y. Xiong;W. Shan;Congge Zhang;Zhimeng Song
采用改进的浸渍法制备了xwt %的Al-SBA-15系列催化剂，考察了其在γ-戊内酯（GVL）脱羧制丁烯反应中的催化性能。结果表明，Al物种的浸渍不仅保持了SBA-15的有序介孔结构，而且在催化剂表面产生了大量的Brønsted和刘易斯酸中心。2.23wt%的Al-SBA-15催化剂具有较高的固体酸中心含量和合适的Brønsted/刘易斯酸比，具有较好的催化性能。在优化条件下，在320 °C时，GVL转化率和丁烯收率分别达到99.8%和96.6%。反应机理研究表明，γ-质子化PEA的脱羧反应控制了整个反应的速率。再生后的2. 23 wt%Al-SBA-15催化剂在8次循环后仍具有良好的催化活性，丁烯收率可达92.2%。
A series ofxwt%Al-SBA-15 catalysts prepared by modified wetness impregnation was investigated for γ-valerolactone (GVL) decarboxylation to butene. It was found that the impregnation of Al species not only remained the ordered mesoporous structure of parent SBA-15, but also created large amounts of Brønsted and Lewis acid sites on the surface of catalyst. The considerable amount of solid acid sites and the suitable Brønsted/Lewis acid ratio endowed 2.23 wt%Al-SBA-15 catalyst an excellent catalytic performance. Under the optimized conditions, the GVL conversion and butene yield can reach 99.8% and 96.6% at 320 °C, respectively. Mechanism studies indicated that the decarboxylation of γ-protonated PEA controlled speed of the whole reaction. Moreover, the catalytic activity of regenerated 2.23 wt%Al-SBA-15 catalyst was satisfactory after eight cycle tests, and the butene yield could still reach 92.2%.