Journal
GREEN CHEMISTRY
Volume 22, Issue 1, Pages 204-218Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9gc03524a
Keywords
-
Funding
- ORAU 2016 Ralph E. Powe Award
- ORNL Neutron Sciences User Facility
- US National Science Foundation CBET awards [1604421, 1846797]
- Rutgers Global Grant, Rutgers Division of Continuing Studies, Rutgers School of Engineering
- Great Lakes Bioenergy Research Center (DOE BER Office of Science) [DE-FC02-07ER64494]
- Office of Biological and Environmental Research (OBER) [FWP ERKP291, FWP ERKP752]
- Office of Basic Energy Sciences (BES), U.S. Department of Energy (DOE)
- University Grants Commission of India (Raman Fellowship Program)
- China Scholarship Council
- U.S. Department of Energy [DE-AC05-00OR22725]
- Department of Energy
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1604421] Funding Source: National Science Foundation
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1846797] Funding Source: National Science Foundation
Ask authors/readers for more resources
Here, we report a novel ammonia : ammonium salt solvent based pretreatment process that can rapidly dissolve crystalline cellulose into solution and eventually produce highly amorphous cellulose under near-ambient conditions. Pre-activating the cellulose I allomorph to its ammonia-cellulose swollen complex (or cellulose III allomorph) at ambient temperatures facilitated rapid dissolution of the pre-activated cellulose in the ammonia-salt solvent (i.e., ammonium thiocyanate salt dissolved in liquid ammonia) at ambient pressures. For the first time in reported literature, we used time-resolved in situ neutron scattering methods to characterize the cellulose polymorphs structural modification and understand the mechanism of crystalline cellulose dissolution into a 'molecular' solution in real-time using ammonia-salt solvents. We also used molecular dynamics simulations to provide insight into solvent interactions that non-covalently disrupted the cellulose hydrogen-bonding network and understand how such solvents are able to rapidly and fully dissolve pre-activated cellulose III. Importantly, the regenerated amorphous cellulose recovered after pretreatment was shown to require nearly similar to 50-fold lesser cellulolytic enzyme usage compared to native crystalline cellulose I allomorph for achieving near-complete hydrolytic conversion into soluble sugars. Lastly, we provide proof-of-concept results to further showcase how such ammonia-salt solvents can pretreat and fractionate lignocellulosic biomass like corn stover under ambient processing conditions, while selectively co-extracting similar to 80-85% of total lignin, to produce a highly digestible polysaccharide-enriched feedstock for biorefinery applications. Unlike conventional ammonia-based pretreatment processes (e.g., Ammonia Fiber Expansion or Extractive Ammonia pretreatments), the proposed ammonia-salt process can operate at near-ambient conditions to greatly reduce the pressure/temperature severity necessary for conducting effective ammonia-based pretreatments on lignocellulose.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available