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高比表面积介孔硅铝酸盐上木质素的催化快速热解:孔隙率和酸度的影响

Catalytic Fast Pyrolysis of Lignin over High-Surface-Area Mesoporous Aluminosilicates: Effect of Porosity and Acidity.

作者信息

Custodis Victoria B F, Karakoulia Stamatia A, Triantafyllidis Kostas S, van Bokhoven Jeroen A

机构信息

Department of Chemistry and Applied Biosciences, ETH Zürich, 8093, Zürich, Switzerland.

Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232, Villigen, Switzerland.

出版信息

ChemSusChem. 2016 May 23;9(10):1134-45. doi: 10.1002/cssc.201600105. Epub 2016 Apr 15.

DOI:10.1002/cssc.201600105
PMID:27079742
Abstract

Catalytic fast pyrolysis (CFP) of lignin with amorphous mesoporous aluminosilicates catalysts yields a high fraction of aromatics and a relatively low amount of char/coke. The relationship between the acidity and porosity of Al-MCM-41, Al-SBA-15, and Al-MSU-J with product selectivity during lignin CFP is determined. The acid sites (mild Brønsted and stronger Lewis) are able to catalyze pyrolysis intermediates towards fewer oxygenated phenols and aromatic hydrocarbons. A generalized correlation of the product selectivity and yield with the aluminum content and acidity of the mesoporous aluminosilicates is hard to establish. Zeolitic strong acid sites are not required to achieve high conversion and selectivity to aromatic hydrocarbon because nanosized MCM-41 produces a high liquid yield and selectivity. The two most essential parameters are diffusion, which is influenced by pore and grain size, and the active site, which may be mildly acidic, but is dominated by Lewis acid sites. Nanosized grains and mild acidity are essential ingredients for a good lignin CFP catalyst.

摘要

木质素与无定形介孔铝硅酸盐催化剂进行催化快速热解(CFP)可产生高比例的芳烃和相对少量的焦炭。确定了Al-MCM-41、Al-SBA-15和Al-MSU-J的酸度和孔隙率与木质素CFP过程中产物选择性之间的关系。酸性位点(温和的布朗斯台德酸和较强的路易斯酸)能够将热解中间体催化生成更少的含氧酚和芳烃。很难建立产物选择性和产率与介孔铝硅酸盐的铝含量和酸度之间的普遍关联。实现高转化率和对芳烃的选择性并不需要沸石强酸位点,因为纳米尺寸的MCM-41可产生高液体产率和选择性。两个最重要的参数是受孔径和颗粒尺寸影响的扩散以及活性位点,活性位点可能是弱酸性的,但以路易斯酸位点为主。纳米尺寸颗粒和弱酸度是良好木质素CFP催化剂的基本要素。

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