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

Keturakis Christopher J.; Lapina Olga B.; Shubin Aleksandr A.; Terskikh Victor V.; Papulovskiy Evgeniy; Yudaev Ivan V; Paukshtis Eugenii A.; Wachs Israel E.

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

机译：固体酸催化剂存在下生物质纤维素分数的热解：透明度光谱和理论研究

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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 AlOx nanostructures on SiO2 were determined with Al-27/(HNMR)-H-1 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 AlOx cluster and molecular nature of the biomass feed-stock. These new insights allowed the establishment of fundamental structure-activity/selectivity relationships during biomass pyrolysis.

机译：通过固体酸催化剂的生物质热解是可持续生产烃液体燃料和增值化学品的有希望的技术之一，但这些复杂的化学转化仍然明白。在脱水条件下合成了一系列良好的定义模型SiO 2支持的氧化铝催化剂和分子地表征在脱水条件下，在生物质热解中，目的是建立基本催化剂结构 - 活性/选择性关系。用CheAlboLed CO和DFT计算的Al-27 /（HNMR）-H-1和IR光谱法测定SiO 2上负载的Alox纳米结构的性质和相应的酸度。 Operando时间分辨的IR-Raman-MS光谱研究显示在生物质热解期间发生的分子转化。生物质热解期间的分子转化依赖于Alox簇的畴尺寸和生物质饲料储备的分子性质。这些新的见解允许在生物质热解期间建立基本结构 - 活性/选择性关系。

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来源
《ChemSusChem》 |2018年第23期|共16页
作者
Keturakis Christopher J.; Lapina Olga B.; Shubin Aleksandr A.; Terskikh Victor V.; Papulovskiy Evgeniy; Yudaev Ivan V; Paukshtis Eugenii A.; Wachs Israel E.;
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作者单位

Lehigh Univ Dept Chem Engn Operando Mol Spect &

Catalysis Res Lab Bethlehem PA 18015 USA;

Boreskov Inst Catalysis Pr Lavrentieva 5 Novosibirsk 630090 Russia;

Boreskov Inst Catalysis Pr Lavrentieva 5 Novosibirsk 630090 Russia;

Univ Ottawa Dept Chem Ottawa ON K1N 6N5 Canada;

Boreskov Inst Catalysis Pr Lavrentieva 5 Novosibirsk 630090 Russia;

Boreskov Inst Catalysis Pr Lavrentieva 5 Novosibirsk 630090 Russia;

Boreskov Inst Catalysis Pr Lavrentieva 5 Novosibirsk 630090 Russia;

Lehigh Univ Dept Chem Engn Operando Mol Spect &

Catalysis Res Lab Bethlehem PA 18015 USA;

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正文语种 eng
中图分类化学;
关键词
biomass; catalysts; operando spectroscopy; solid acid; supported Al2O3/SiO2;

机译：生物量;催化剂;操作性谱;固体酸;支持的Al2O3 / SiO2;

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1. Pyrolysis of the Cellulose Fraction of Biomass in the Presence of Solid Acid Catalysts: An Operando Spectroscopy and Theoretical Investigation... [J] . The Catalyst Review Newsletter group The Catalyst Review Newsletter . 2019,第1期

机译：固体酸催化剂存在下生物质的纤维素级分的热解：透明度光谱和理论研究......
2. Study on Pyrolysis of Pine Sawdust with Solid Base and Acid Mixed Catalysts by Thermogravimetry-Fourier Transform Infrared Spectroscopy and Pyrolysis-Gas Chromatography/Mass Spectrometry [J] . Huiyan Zhang, Jian Zheng, Rui Xiao, Energy & fuels . 2014,第julaaauga期

机译：热重-傅里叶变换红外光谱和热解-气相色谱/质谱法研究松木屑与固体碱和酸混合催化剂的热解
3. Electrochemical biomass valorization on gold-metal oxide nanoscale heterojunctions enables investigation of both catalyst and reaction dynamics with operando surface-enhanced Raman spectroscopy [J] . Nina Heidary, Nikolay Kornienko Chemical science . 2020,第7期

机译：金属氧化物纳米级异质结上的电化学生物质载物能够通过Operando表面增强的拉曼光谱进行催化剂和反应动力学的研究
4. INFLUENCE OF THE PREVIOUS PYROLYSIS STEP (BIOMASS SOURCE, PYROLYSIS TEMPERATURE,AND TECHNOLOGY) ON THE CATALYTIC STEAM REFORMING PROCESS OF BIOMASS PYROLYSIS AQUEOUS FRACTIONS USING A Ni-Co/Al-Mg CATALYST [C] . Remón J., Broust F., Valette J., European biomass conference and exhibition . 2012

机译：Ni-Co / Al-Mg催化剂对上一步热解步骤（生物质，热解温度和工艺）对生物质热解级分的催化蒸汽重整过程的影响
5. Conversion of Biomass-Derived Oxygenated Compounds to Hydrocarbon Fuels and Commodity Chemicals using Solid Acid Catalysts. [D] . Wang, Dong. 2013

机译：使用固体酸催化剂将生物质衍生的氧化化合物转化为烃类燃料和日用化学品。
6. Electrochemical biomass valorization on gold-metal oxide nanoscale heterojunctions enables investigation of both catalyst and reaction dynamics with operando surface-enhanced Raman spectroscopy [O] . Nina Heidary, Nikolay Kornienko 2020

机译：金-金属氧化物纳米级异质结上的电化学生物量平衡可通过操作性表面增强拉曼光谱研究催化剂和反应动力学
7. The Effect of Mechanical Activation and Lignin Impurities on the Hydrolysis-Dehydration of Cellulose in the Presence of Sibunit-4 Solid Acidic Carbon Catalysts [O] . Nikolay V. Gromov, Marina N. Denisova, Tatiana B. Medvedeva, 2019

机译：机械活化和木质素杂质对纤维素 - 4固体酸性碳催化剂存在下纤维素水解脱水的影响
8. Conversion of Cellulosic Wastes to Liquid Hydrocarbon Fuels: Vol. 4, Slurry Phase Synthesis of Liquid Hydrocarbon Fuels from Biomass Pyrolysis Gas Using Iron Catalysts: Final Report [R] . Kuester, J. L. 1986

机译：纤维素废物转化为液态烃燃料：Vol。 4，利用铁催化剂从生物质裂解气体中分离合成液态烃燃料：最终报告

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

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