Flowthrough Reductive Catalytic Fractionation of Biomass

被引:227
作者
Anderson, Eric M. [1 ]
Stone, Michael L. [1 ]
Katahira, Rui [2 ]
Reed, Michelle [2 ]
Beckham, Gregg T. [2 ]
Roman-Leshkov, Yuriy [1 ]
机构
[1] MIT, Chem Engn, 25 Ames St, Cambridge, MA 02142 USA
[2] Natl Renewable Energy Lab, 15013 Denver W Pkwy, Golden, CO 80401 USA
基金
美国国家科学基金会;
关键词
LIGNIN MONOMER PRODUCTION; LIGNOCELLULOSE FRACTIONATION; LIQUID FUELS; CONVERSION; DEPOLYMERIZATION; VALORIZATION; CLEAVAGE; HYDRODEOXYGENATION; CHEMICALS; DIMERS;
D O I
10.1016/j.joule.2017.10.004
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Reductive catalytic fractionation (RCF) has emerged as a leading biomass fractionation and lignin valorization strategy. Here, flowthrough reactors were used to investigate RCF of poplar. Most RCF studies to date have been conducted in batch, but a flow-based process enables the acquisition of intrinsic kinetic and mechanistic data essential to accelerate the design, optimization, and scale-up of RCF processes. Time-resolved product distributions and yields obtained from experiments with different catalyst loadings were used to identify and deconvolute events during solvolysis and hydrogenolysis. Multi-bed RCF experiments provided unique insights into catalyst deactivation, showing that leaching, sintering, and surface poisoning are causes for decreased catalyst performance. The onset of catalyst deactivation resulted in higher concentrations of unsaturated lignin intermediates and increased occurrence of repolymerization reactions, producing high-molecular-weight species. Overall, this study demonstrates the concept of flowthrough RCF, which will be vital for realistic scale-up of this promising approach.
引用
收藏
页码:613 / 622
页数:10
相关论文
共 62 条
[51]   Strategies for the Conversion of Lignin to High-Value Polymeric Materials: Review and Perspective [J].
Upton, Brianna M. ;
Kasko, Andrea M. .
CHEMICAL REVIEWS, 2016, 116 (04) :2275-2306
[52]   Integrating lignin valorization and bio-ethanol production: on the role of Ni-Al2O3 catalyst pellets during lignin-first fractionation [J].
Van den Bosch, S. ;
Renders, T. ;
Kennis, S. ;
Koelewijn, S. -F. ;
Van den Bossche, G. ;
Vangeel, T. ;
Deneyer, A. ;
Depuydt, D. ;
Courtin, C. M. ;
Thevelein, J. M. ;
Schutyser, W. ;
Sels, B. F. .
GREEN CHEMISTRY, 2017, 19 (14) :3313-3326
[53]   Tuning the lignin oil OH-content with Ru and Pd catalysts during lignin hydrogenolysis on birch wood [J].
Van den Bosch, S. ;
Schutyser, W. ;
Koelewijn, S. -F. ;
Renders, T. ;
Courtin, C. M. ;
Sels, B. F. .
CHEMICAL COMMUNICATIONS, 2015, 51 (67) :13158-13161
[54]   Reductive lignocellulose fractionation into soluble lignin-derived phenolic monomers and dimers and processable carbohydrate pulps [J].
Van den Bosch, S. ;
Schutyser, W. ;
Vanholme, R. ;
Driessen, T. ;
Koelewijn, S. -F. ;
Renders, T. ;
De Meester, B. ;
Huijgen, W. J. J. ;
Dehaen, W. ;
Courtin, C. M. ;
Lagrain, B. ;
Boerjan, W. ;
Sels, B. F. .
ENERGY & ENVIRONMENTAL SCIENCE, 2015, 8 (06) :1748-1763
[55]   Bifunctional Ni catalysts for the one-pot conversion of Organosolv lignin into cycloalkanes [J].
Wang, Xingyu ;
Rinaldi, Roberto .
CATALYSIS TODAY, 2016, 269 :48-55
[56]  
Weider P. R., 2016, US patent, Patent No. 9382593B2
[57]   Selective Degradation of Wood Lignin over Noble-Metal Catalysts in a Two-Step Process [J].
Yan, Ning ;
Zhao, Chen ;
Dyson, Paul J. ;
Wang, Chen ;
Liu, Ling-tao ;
Kou, Yuan .
CHEMSUSCHEM, 2008, 1 (07) :626-629
[58]   Reavisitng the mechanism of β-O-4 bond cleavage during acidolysis of lignin.: Part 1:: Kinetics of the formation of enol ether from non-phenolic C6-C2 type model compounds [J].
Yokoyama, Tomoya ;
Matsumoto, Yuji .
HOLZFORSCHUNG, 2008, 62 (02) :164-168
[59]   Lignin-Derived Thioacidolysis Dimers: Reevaluation, New Products, Authentication, and Quantification [J].
Yue, Fengxia ;
Lu, Fachuang ;
Regner, Matt ;
Sun, Runcang ;
Ralph, John .
CHEMSUSCHEM, 2017, 10 (05) :830-835
[60]   The Catalytic Valorization of Lignin for the Production of Renewable Chemicals [J].
Zakzeski, Joseph ;
Bruijnincx, Pieter C. A. ;
Jongerius, Anna L. ;
Weckhuysen, Bert M. .
CHEMICAL REVIEWS, 2010, 110 (06) :3552-3599