Pyrolysis of the Cellulose Fraction of Biomass in the Presence of Solid Acid Catalysts: An Operando Spectroscopy and Theoretical Investigation,ChemSusChem

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Pyrolysis of the Cellulose Fraction of Biomass in the Presence of Solid Acid Catalysts: An Operando Spectroscopy and Theoretical Investigation
ChemSusChem ( IF 7.5 ) Pub Date : 2018-11-19 , DOI: 10.1002/cssc.201802073
Christopher J. Keturakis _{1,

2} , Olga B. Lapina _{3,

4} , Aleksandr A. Shubin _{3,

4} , Victor V. Terskikh ₅ , Evgeniy Papulovskiy ₃ , Ivan V. Yudaev ₃ , Eugenii A. Paukshtis _{3,

4} , Israel E. Wachs ₁

Affiliation

Biomass pyrolysis by solid acid catalysts is one of many promising technologies for sustainable production of hydrocarbon liquid fuels and value‐added chemicals, but these complex chemical transformations are still poorly understood. A series of well‐defined model SiO₂‐supported alumina catalysts were synthesized and molecularly characterized, under dehydrated conditions and during biomass pyrolysis, with the aim of establishing fundamental catalyst structure–activity/selectivity relationships. The nature and corresponding acidity of the supported AlO_x nanostructures on SiO₂ were determined with ²⁷Al/¹H NMR and IR spectroscopy of chemisorbed CO, and DFT calculations. Operando time‐resolved IR–Raman–MS spectroscopy studies revealed the molecular transformations taking place during biomass pyrolysis. The molecular transformations during biomass pyrolysis depended on both the domain size of the AlO_x cluster and molecular nature of the biomass feedstock. These new insights allowed the establishment of fundamental structure–activity/selectivity relationships during biomass pyrolysis.

中文翻译：

固体酸催化剂存在下生物质纤维素馏分的热解：操作光谱和理论研究

固体酸催化剂进行生物质热解是可持续生产烃类液体燃料和增值化学品的许多有前途的技术之一，但是对这些复杂的化学转化仍然知之甚少。合成了一系列定义明确的模型SiO ₂负载的氧化铝催化剂，并在脱水条件下和生物质热解过程中进行了分子表征，旨在建立基本的催化剂结构-活性/选择性关系。用²⁷ Al / ¹确定了SiO ₂上负载的AlO _x纳米结构的性质和相应的酸度化学吸附一氧化碳的1 H NMR和IR光谱，以及DFT计算。Operando时间分辨的IR–Raman–MS光谱研究显示了生物质热解过程中发生的分子转化。生物质热解过程中的分子转化取决于AlO _x团簇的区域大小和生物质原料的分子性质。这些新的见解允许在生物质热解过程中建立基本的结构-活性/选择性关系。

更新日期：2018-11-19

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