Efficient dehydration of bio-based 2,3-butanediol to butanone over boric acid modified HZSM-5 zeolites
Efficient dehydration of bio-based 2,3-butanediol to butanone over boric acid modified HZSM-5 zeolites
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硼酸改性 HZSM-5 沸石上生物基 2,3-丁二醇高效脱水生成丁酮
DOI：
10.1039/c2gc36324k
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发表时间：
2012-11
期刊：
影响因子：
9.8
通讯作者：
Wengui Zhang , Dinghua Yu , Xiaojun Ji, He Huang
中科院分区：
文献类型：
--
作者：
Wengui Zhang , Dinghua Yu , Xiaojun Ji, He Huang
生物基2，3-丁二醇的脱水为丁酮的生产提供了一条可供选择的绿色途径。本文研究了HZSM-5分子筛（Si/Al = 38-360）骨架硅铝比对2，3-丁二醇脱水反应的影响。用硼酸对HZSM-5（360）进行了进一步改性，研究了硼酸负载量对脱水性能的影响。结果表明，高硅铝比有利于2，3-丁二醇的低温活化和甲基向2-甲基丙醛的迁移。1.0%B/HZSM-5（360）不仅在180 °C下表现出最好的性能，而且在180-300 °C之间保持稳定的活性，具有2.4 h-1的高LHSV。根据表征结果，相对于HZSM-5（360）的优异性能是由于归因于H-键合的羟基基团（通常为硅烷醇）的最高量的强酸位点（1.1674 mmol g−1）。在1.0%B/HZSM-5（360）上，更有效的骨架外B-OH物种和保留的硅醇的共存是催化剂性能提高的原因。
The dehydration of bio-based 2,3-butanediol provides an alternative green way to produce butanone, which is mainly produced through the dehydrogenation of butanol in industry. In this research, the effect of the framework Si/Al ratio on 2,3-butanediol dehydration over HZSM-5 zeolites (Si/Al = 38–360) was investigated. HZSM-5(360) was further modified with boric acid, and the influence of the loading amount of boric acid on the dehydration performance was studied. The results showed that high Si/Al ratio was beneficial to low-temperature activation of 2,3-butanediol and the methyl migration to 2-methyl propanal. 1.0%B/HZSM-5(360) not only showed best performance at 180 °C but also kept stable activities between 180–300 °C with a high LHSV 2.4 h−1. According to the characterization results, excellent performance over HZSM-5(360) was due to the highest amount of strong acidic sites (1.1674 mmol g−1) attributed to H-bonded hydroxyl groups, normally silanols. Coexistence of more effective extraframework B–OH species and retained silanols were responsible for the promotion of catalytic performance over 1.0%B/HZSM-5(360).
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