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基于铜基混合氧化物和磷化镍催化剂组合在超临界乙醇中实现木质素升级的协同作用

Synergy in Lignin Upgrading by a Combination of Cu-Based Mixed Oxide and Ni-Phosphide Catalysts in Supercritical Ethanol.

作者信息

Korányi Tamás I, Huang Xiaoming, Coumans Alessandro E, Hensen Emiel J M

机构信息

Schuit Institute of Catalysis, Inorganic Materials Chemistry, Eindhoven University of Technology , Den Dolech 2, 5612 AZ, Eindhoven, The Netherlands.

出版信息

ACS Sustain Chem Eng. 2017 Apr 3;5(4):3535-3543. doi: 10.1021/acssuschemeng.7b00239. Epub 2017 Mar 1.

Abstract

The depolymerization of lignin to bioaromatics usually requires a hydrodeoxygenation (HDO) step to lower the oxygen content. A mixed Cu-Mg-Al oxide (CuMgAlO ) is an effective catalyst for the depolymerization of lignin in supercritical ethanol. We explored the use of Ni-based cocatalysts, i.e. Ni/SiO, NiP/SiO, and Ni/ASA (ASA = amorphous silica alumina), with the aim of combining lignin depolymerization and HDO in a single reaction step. While the silica-supported catalysts were themselves hardly active in lignin upgrading, Ni/ASA displayed comparable lignin monomer yield as CuMgAlO . A drawback of using an acidic support is extensive dehydration of the ethanol solvent. Instead, combining CuMgAlO with Ni/SiO and especially NiP/SiO proved to be effective in increasing the lignin monomer yield, while at the same time reducing the oxygen content of the products. With NiP/SiO, the lignin monomer yield was 53 wt %, leading to nearly complete deoxygenation of the aromatic products.

摘要

木质素解聚为生物芳烃通常需要一个加氢脱氧(HDO)步骤来降低氧含量。混合铜镁铝氧化物(CuMgAlO )是超临界乙醇中木质素解聚的有效催化剂。我们探索了使用镍基助催化剂,即Ni/SiO、NiP/SiO和Ni/ASA(ASA = 无定形硅铝酸盐),目的是在单个反应步骤中将木质素解聚和HDO结合起来。虽然二氧化硅负载的催化剂本身在木质素升级方面几乎没有活性,但Ni/ASA表现出与CuMgAlO 相当的木质素单体产率。使用酸性载体的一个缺点是乙醇溶剂的大量脱水。相反,将CuMgAlO 与Ni/SiO尤其是NiP/SiO结合起来被证明在提高木质素单体产率的同时有效降低产物的氧含量。使用NiP/SiO时,木质素单体产率为53 wt%,导致芳烃产物几乎完全脱氧。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/62b0/5384481/e97fc24b507f/sc-2017-00239z_0001.jpg

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