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木质纤维素两步催化转化为烷烃。

Two-step catalytic conversion of lignocellulose to alkanes.

作者信息

Sun Zhuohua, Buwalda Daniel, Barta Katalin

机构信息

Stratingh Institute for Chemistry, University of Groningen Nijenborgh 4 9747 AG Groningen The Netherlands

出版信息

RSC Adv. 2019 Jul 30;9(41):23727-23734. doi: 10.1039/c9ra03174j. eCollection 2019 Jul 29.

DOI:10.1039/c9ra03174j
PMID:35530606
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9069466/
Abstract

Direct conversion of lignocellulose to alkanes is challenged by the complex and recalcitrant nature of the starting material. Generally, alkanes are obtained from one of the main lignocellulose constituents (cellulose, hemicellulose or lignin) after their separation, and platform chemicals derived therein. Here we describe a two-step methodology, which uses unprocessed lignocellulose directly, targeting a mixture of alkanes. The first step involves the near-complete conversion of lignocellulose to alcohols, using a copper doped porous metal oxide (Cu-PMO) catalyst in supercritical methanol. The second step comprises a novel solvent exchange procedure and the exhaustive hydrodeoxygenation (HDO) of the complex mixture of aliphatic alcohols, obtained upon depolymerization, to C-C alkanes by either HZSM-5 or Nafion at 180 °C in conjunction with Pd/C in dodecane. This describes an unprecedented two-step process from lignocellulose to hydrocarbons, with an overall carbon yield of 50%.

摘要

木质纤维素向烷烃的直接转化受到起始原料复杂且难降解性质的挑战。一般来说,烷烃是从木质纤维素的主要成分之一(纤维素、半纤维素或木质素)分离后获得的,并由此衍生出平台化学品。在此,我们描述了一种两步法,该方法直接使用未经处理的木质纤维素,目标产物为烷烃混合物。第一步涉及在超临界甲醇中使用铜掺杂多孔金属氧化物(Cu-PMO)催化剂将木质纤维素近乎完全转化为醇类。第二步包括一种新型的溶剂交换程序,以及将解聚后得到的脂肪醇复杂混合物在180℃下通过HZSM-5或Nafion与十二烷中的Pd/C结合进行彻底的加氢脱氧(HDO)反应,转化为碳-碳烷烃。这描述了一个前所未有的从木质纤维素到碳氢化合物的两步过程,总碳产率为50%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/640dbebafa48/c9ra03174j-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/aa7120bb2237/c9ra03174j-f1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/9988a3e75483/c9ra03174j-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/662332e24b38/c9ra03174j-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/a4c47485c197/c9ra03174j-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/5494f2c5a7e2/c9ra03174j-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/640dbebafa48/c9ra03174j-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/aa7120bb2237/c9ra03174j-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/9639532ac452/c9ra03174j-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/9988a3e75483/c9ra03174j-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/662332e24b38/c9ra03174j-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/a4c47485c197/c9ra03174j-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/5494f2c5a7e2/c9ra03174j-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b3d2/9069466/640dbebafa48/c9ra03174j-f7.jpg

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