Elucidation of cellulose accessibility, hydrolysability and reactivity as the major limitations in the enzymatic hydrolysis of cellulose

被引:56
作者
Bansal, Prabuddha [1 ]
Vowell, Bryan J. [1 ]
Hall, Melanie [1 ,2 ]
Realff, Matthew J. [1 ]
Lee, Jay H. [1 ,3 ]
Bommarius, Andreas S. [1 ,4 ]
机构
[1] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA
[2] Graz Univ, Dept Chem Organ & Bioorgan Chem, A-8010 Graz, Austria
[3] Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea
[4] Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USA
关键词
Accessibility; Hydrolysability; Reactivity; Enzymatic cellulose hydrolysis; Kinetic modeling; KINETIC-MODEL; CELLULASES; BIOFUELS; CRYSTALLINITY; PROTEIN; SURFACE;
D O I
10.1016/j.biortech.2011.12.063
中图分类号
S2 [农业工程];
学科分类号
0828 ;
摘要
The precipitous decline in the rates of enzymatic hydrolysis of cellulose with conversion is one of the major limitations to the commercialization of second-generation biofuel. In this work, various rate-limiting factors (fractal kinetics, changes in crystallinity, accessibility, reactivity and hydrolysable fraction, enzyme clogging, and degree of polymerization) were investigated employing experimental as well as computational studies. Model-guided experiments showed cellulose accessibility and the hydrolysable fraction of accessible substrate (a previously undefined and unreported quantity) to decrease steadily until a conversion level of nearly 70%, while cellulose reactivity, defined in terms of hydrolytic activity per amount of actively adsorbed cellulase, remained constant. Substrate depletion, accessibility and hydrolysability decrease accounted for approximately 90% of rate retardation up to 70% conversion. Faster restart rates were observed on partially converted cellulose as compared to uninterrupted hydrolysis rates, supporting an enzyme clogging phenomenon that could possibly be responsible for the additional rate decrease. (C) 2011 Elsevier Ltd. All rights reserved.
引用
收藏
页码:243 / 250
页数:8
相关论文
共 36 条
[1]   Multivariate statistical analysis of X-ray data from cellulose: A new method to determine degree of crystallinity and predict hydrolysis rates [J].
Bansal, Prabuddha ;
Hall, Melanie ;
Realff, Matthew J. ;
Lee, Jay H. ;
Bommarius, Andreas S. .
BIORESOURCE TECHNOLOGY, 2010, 101 (12) :4461-4471
[2]   Modeling cellulase kinetics on lignocellulosic substrates [J].
Bansal, Prabuddha ;
Hall, Melanie ;
Realff, Matthew J. ;
Lee, Jay H. ;
Bommarius, Andreas S. .
BIOTECHNOLOGY ADVANCES, 2009, 27 (06) :833-848
[3]   Cellulase kinetics as a function of cellulose pretreatment [J].
Bommarius, Andreas S. ;
Katona, Adrian ;
Cheben, Sean E. ;
Patel, Arpit S. ;
Ragauskas, Arthur J. ;
Knudson, Kristina ;
Pu, Yunqiao .
METABOLIC ENGINEERING, 2008, 10 (06) :370-381
[4]   PROTEIN MEASUREMENT USING BICINCHONINIC ACID - ELIMINATION OF INTERFERING SUBSTANCES [J].
BROWN, RE ;
JARVIS, KL ;
HYLAND, KJ .
ANALYTICAL BIOCHEMISTRY, 1989, 180 (01) :136-139
[5]   KINETIC MODELING OF THE ENZYMATIC-HYDROLYSIS OF PRETREATED CELLULOSE [J].
CAMINAL, G ;
LOPEZSANTIN, J ;
SOLA, C .
BIOTECHNOLOGY AND BIOENGINEERING, 1985, 27 (09) :1282-1290
[6]   Effect of digestion by pure cellulases on crystallinity and average chain length for bacterial and microcrystalline celluloses [J].
Chen, Yao ;
Stipanovic, Arthur J. ;
Winter, William T. ;
Wilson, David B. ;
Kim, Young-Jun .
CELLULOSE, 2007, 14 (04) :283-293
[7]   THE 3-DIMENSIONAL CRYSTAL-STRUCTURE OF THE CATALYTIC CORE OF CELLOBIOHYDROLASE-I FROM TRICHODERMA-REESEI [J].
DIVNE, C ;
STAHLBERG, J ;
REINIKAINEN, T ;
RUOHONEN, L ;
PETTERSSON, G ;
KNOWLES, JKC ;
TEERI, TT ;
JONES, TA .
SCIENCE, 1994, 265 (5171) :524-528
[8]   The cellulose-binding domain of cellobiohydrolase Cel7A from Trichoderma reesei is also a thermostabilizing domain [J].
Hall, Melanie ;
Rubin, Jonathan ;
Behrens, Sven H. ;
Bommarius, Andreas S. .
JOURNAL OF BIOTECHNOLOGY, 2011, 155 (04) :370-376
[9]   Biological pretreatment of cellulose: Enhancing enzymatic hydrolysis rate using cellulose-binding domains from cellulases [J].
Hall, Melanie ;
Bansal, Prabuddha ;
Lee, Jay H. ;
Realff, Matthew J. ;
Bommarius, Andreas S. .
BIORESOURCE TECHNOLOGY, 2011, 102 (03) :2910-2915
[10]   Cellulose crystallinity - a key predictor of the enzymatic hydrolysis rate [J].
Hall, Melanie ;
Bansal, Prabuddha ;
Lee, Jay H. ;
Realff, Matthew J. ;
Bommarius, Andreas S. .
FEBS JOURNAL, 2010, 277 (06) :1571-1582