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基于纤维素的 3-甲基环戊-2-烯酮直接加氢脱氧合成生物基甲基环戊二烯。

Synthesis of bio-based methylcyclopentadiene via direct hydrodeoxygenation of 3-methylcyclopent-2-enone derived from cellulose.

机构信息

CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023, Dalian, China.

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023, Dalian, China.

出版信息

Nat Commun. 2021 Jan 4;12(1):46. doi: 10.1038/s41467-020-20264-3.

DOI:10.1038/s41467-020-20264-3
PMID:33397902
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7782798/
Abstract

The exploration of highly efficient processes to convert renewable biomass to fuels and value-added chemicals is stimulated by the energy and environment problems. Herein, we describe an innovative route for the production of methylcyclopentadiene (MCPD) with cellulose, involving the transformation of cellulose into 3-methylcyclopent-2-enone (MCP) and subsequent selective hydrodeoxygenation to MCPD over a zinc-molybdenum oxide catalyst. The excellent performance of the zinc-molybdenum oxide catalyst is attributed to the formation of ZnMoO species during the reduction of ZnMoO. Experiments reveal that preferential interaction of ZnMoO sites with the C=O bond instead of C=C bond in vapor-phase hydrodeoxygenation of MCP leads to highly selective formations of MCPD (with a carbon yield of 70%).

摘要

高效转化可再生生物质为燃料和高附加值化学品的方法受到能源和环境问题的推动。在此,我们描述了一种利用纤维素生产甲基环戊二烯(MCPD)的创新途径,涉及纤维素转化为 3-甲基环戊-2-烯酮(MCP),以及在锌钼氧化物催化剂上通过选择性加氢脱氧生成 MCPD。锌钼氧化物催化剂的优异性能归因于 ZnMoO 在还原过程中形成 ZnMoO 物种。实验表明,在 MCP 的气相加氢脱氧过程中,ZnMoO 位点与 C=O 键的优先相互作用而不是 C=C 键的相互作用导致 MCPD 的高选择性形成(碳收率为 70%)。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/5cc3b5e256c6/41467_2020_20264_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/e7216c508e28/41467_2020_20264_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/52675f2553f1/41467_2020_20264_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/954fd0be92ad/41467_2020_20264_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/5cc3b5e256c6/41467_2020_20264_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/e7216c508e28/41467_2020_20264_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/52675f2553f1/41467_2020_20264_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/954fd0be92ad/41467_2020_20264_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/acc5/7782798/5cc3b5e256c6/41467_2020_20264_Fig4_HTML.jpg

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