Cellulose hydrolysis by Clostridium thermocellum is agnostic to substrate structural properties in contrast to fungal cellulases

Kothari, Ninad; Bhagia, Samarthya; Zaher, Maher; Pu, Yunqiao; Mittal, Ashutosh; Yoo, Chang Geun; Himmel, Michael E.; Ragauskas, Arthur J.; Kumar, Rajeev; Wyman, Charles E.

doi:10.1039/C9GC00262F

Title: Cellulose hydrolysis by Clostridium thermocellum is agnostic to substrate structural properties in contrast to fungal cellulases

Journal Article · Wed May 01 00:00:00 EDT 2019 · Green Chemistry

DOI:https://doi.org/10.1039/C9GC00262F· OSTI ID:1525764

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Univ. of California, Riverside, CA (United States). Bourns College of Engineering, Dept. of Chemical and Environmental Engineering, Center for Environmental Research and Technology (CE-CERT); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC), and Biosciences Division
Univ. of California, Riverside, CA (United States). Bourns College of Engineering, Dept. of Chemical and Environmental Engineering, Center for Environmental Research and Technology (CE-CERT)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). UT-ORNL Joint Inst. for Biological Sciences; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC)
National Renewable Energy Lab. (NREL), Golden, CO (United States). Biosciences Center
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). UT-ORNL Joint Inst. for Biological Sciences; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI)
National Renewable Energy Lab. (NREL), Golden, CO (United States). Biosciences Center; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC), Center for Bioenergy Innovation (CBI),; Univ. of Tennessee, Knoxville, TN (United States). Inst. of Agriculture, Dept. of Forestry, Wildlife, and Fisheries, Center for Renewable Carbon; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biosciences Division; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Joint Inst. of Biological Sciences, Biosciences Division
Univ. of California, Riverside, CA (United States). Bourns College of Engineering, Center for Environmental Research and Technology (CE-CERT); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI)
Univ. of California, Riverside, CA (United States). Bourns College of Engineering, Dept. of Chemical and Environmental Engineering, Center for Environmental Research and Technology (CE-CERT); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI)

The native recalcitrance of lignocellulosic biomass hinders its effective deconstruction for biological conversion to fuel ethanol. However, once cellulose is physically available to enzymes/microbes, i.e., macro-accessible, cellulose micro-accessibility, i.e., the accessibility as influenced by cellulose properties, further affects cellulose conversion. Here, we performed a comparative study of the effect of cellulose micro-accessibility on cellulose conversion by two biological approaches of potential commercial interest: consolidated bioprocessing (CBP) using Clostridium thermocellum and cell-free saccharification mediated by fungal enzymes. Commercially available cellulosic substrates, Avicel® PH-101, Sigmacell Cellulose Type 50, cotton linters, Whatman™ 1 milled filter paper, and α-cellulose were employed to constitute different cellulose micro-accessibilities. Physiochemical characterization was performed on these substrates to determine key morphological and chemical differences. Biological conversion of these substrates showed that C. was unaffected overall by cellulose structural properties, i.e., micro-accessibility, and achieved similar solids solubilization and metabolite production from these structurally different materials. However, fungal enzymes digested these substrates to different extents. Specifically, glucan conversion of these substrates diminished in the following order: milled filter paper > Avicel > Sigmacell and α-cellulose > cotton linters. Here, we propose that C. thermocellum digestion of lignocellulosic biomass is primarily controlled by the physical availability of cellulose in the lignocellulosic matrix and largely unaffected by cellulose properties once cellulose is made macro-accessible. Finally, in contrast, fungal enzymes require cellulose to be physically accessible, i.e., macro-accessible, as well as have properties amenable to digestion, i.e., micro-accessible.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC36-08GO28308; PS02-06ER64304; AC05- 00OR22725.; AC05-00OR22725

OSTI ID:: 1525764

Alternate ID(s):: OSTI ID: 1511773; OSTI ID: 1511910

Report Number(s):: NREL/JA-2700-74123; GRCHFJ

Journal Information:: Green Chemistry, Vol. 21, Issue 10; ISSN 1463-9262

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 11 works

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Title: Cellulose hydrolysis by Clostridium thermocellum is agnostic to substrate structural properties in contrast to fungal cellulases

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