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In Situ Synthesis of Protic Ionic Liquids for Biomass Pretreatment

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    Research Article

    In Situ Synthesis of Protic Ionic Liquids for Biomass Pretreatment
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    • Ezinne C. Achinivu
      Ezinne C. Achinivu
      Joint BioEnergy Institute, Lawrence Berkeley National Laboratory, 5885 Hollis St, Emeryville, California 94608, United States
      Sandia National Laboratories, 7011 East Ave, Livermore, California 94551, United States
      More by Ezinne C. Achinivu
      Orcidhttps://orcid.org/0000-0002-8140-4503
    • Mica Cabrera
      Mica Cabrera
      Joint BioEnergy Institute, Lawrence Berkeley National Laboratory, 5885 Hollis St, Emeryville, California 94608, United States
      Biological Systems and Engineering Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      More by Mica Cabrera
    • Athiyya Umar
      Athiyya Umar
      Joint BioEnergy Institute, Lawrence Berkeley National Laboratory, 5885 Hollis St, Emeryville, California 94608, United States
      Biological Systems and Engineering Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      More by Athiyya Umar
    • Minliang Yang
      Minliang Yang
      Joint BioEnergy Institute, Lawrence Berkeley National Laboratory, 5885 Hollis St, Emeryville, California 94608, United States
      Biological Systems and Engineering Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      More by Minliang Yang
      Orcidhttps://orcid.org/0000-0002-4670-7947
    • Nawa Raj Baral
      Nawa Raj Baral
      Joint BioEnergy Institute, Lawrence Berkeley National Laboratory, 5885 Hollis St, Emeryville, California 94608, United States
      Biological Systems and Engineering Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      More by Nawa Raj Baral
      Orcidhttps://orcid.org/0000-0002-0942-9183
    • Corinne D. Scown
      Corinne D. Scown
      Joint BioEnergy Institute, Lawrence Berkeley National Laboratory, 5885 Hollis St, Emeryville, California 94608, United States
      Biological Systems and Engineering Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      More by Corinne D. Scown
      Orcidhttps://orcid.org/0000-0003-2078-1126
    • Blake A. Simmons
      Blake A. Simmons
      Joint BioEnergy Institute, Lawrence Berkeley National Laboratory, 5885 Hollis St, Emeryville, California 94608, United States
      Biological Systems and Engineering Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
      More by Blake A. Simmons
      Orcidhttps://orcid.org/0000-0002-1332-1810
    • John M. Gladden*
      John M. Gladden
      Joint BioEnergy Institute, Lawrence Berkeley National Laboratory, 5885 Hollis St, Emeryville, California 94608, United States
      Sandia National Laboratories, 7011 East Ave, Livermore, California 94551, United States
      *Email: [email protected], [email protected]
      More by John M. Gladden
      Orcidhttps://orcid.org/0000-0002-6985-2485
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    ACS Sustainable Chemistry & Engineering

    Cite this: ACS Sustainable Chem. Eng. 2022, 10, 37, 12090–12098
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acssuschemeng.2c01211
    Published September 8, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Ionic liquids (ILs) have emerged as versatile solvents that are facilitating advances in many industries such as energy storage, separations, and bioprocessing. Despite their great promise, the cost of many ILs remains excessively high, thus limiting their scalability and commercialization. Therefore, the aim of this paper was to develop a simple and integrated process for synthesizing protic ionic liquids (PILs) in situ, while utilizing them directly as pretreatment solvents for biomass deconstruction/biorefining. The in situ method eliminates the major steps associated with increased cost and carbon footprint, thereby yielding an economically advantaged and environmentally efficient process. The PIL hydroxyethylammonium acetate ([Eth][OAc]) was utilized in the pretreatment and enzymatic hydrolysis of sorghum biomass with the in situ method, which demonstrated equivalent sugar yields relative to the presynthesized [Eth][OAc]. Techno-economic analysis demonstrated the economic advantage of the in situ synthesis over other PIL synthesis methods, due to its reduction of production costs up to $2.9/kg, while the life-cycle assessment showed the environmental efficiency of the process, yielding >30% reduction of GHG per kilogram of PIL. Therefore, this method demonstrates an improvement in the sustainability impact for the utilization of PILs for biomass pretreatment and other IL-utilizing processes.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssuschemeng.2c01211.

    • In-depth TGA/FTIR/NMR analyses of the protic ionic liquids and biomass (PDF)

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    This article is cited by 12 publications.

    1. Salauddin Al Azad, Meysam Madadi, Ashfaque Rahman, Chihe Sun, Ezhen Zhang, Fubao Sun. Quantum Mechanical Insights into Lignocellulosic Biomass Fractionation through an NaOH-Catalyzed Triton-X 100 System: In Vitro and In Silico Approaches. ACS Sustainable Chemistry & Engineering 2025, 13 (15) , 5516-5530. https://doi.org/10.1021/acssuschemeng.4c09654
    2. Fariba Ghaffari, Hemayat Shekaari, Firouzeh Mousavi. Thermodynamic and Transport Properties of Lithium Bromide in Aqueous Solutions of Protic Ionic Liquids Based on 2-Hydroxyethylammonium Propionate at Different Temperatures. Journal of Chemical & Engineering Data 2025, 70 (2) , 878-889. https://doi.org/10.1021/acs.jced.4c00599
    3. Firouzeh Mousavi, Hemayat Shekaari, Fariba Ghaffari, Behrang Golmohammadi. Effect of Lactate-Based Protic Ionic Liquids on the Thermodynamic and Transport Properties of Aqueous Lithium Bromide Solutions at Different Temperatures. Journal of Chemical & Engineering Data 2023, 68 (12) , 3242-3256. https://doi.org/10.1021/acs.jced.3c00546
    4. Nazife Isik Haykir, Yavuz Gokce, Taner Sar, Jörn Viell. Utilizing N,N-dimethylbutylammonium hydrogen sulfate for the pretreatment of lignin-rich waste, argan nut shells. Biomass Conversion and Biorefinery 2025, 12 https://doi.org/10.1007/s13399-025-06678-3
    5. Le Zhou, Yuxin Liu, Jintong Zhang, Qiongguang Li, Menglei Yuan, Zhaoqing Kang. Ionic liquid screening for lignocellulosic biomass fractionation: COSMO–RS prediction and experimental verification. Journal of Molecular Liquids 2024, 407 , 125214. https://doi.org/10.1016/j.molliq.2024.125214
    6. Sabahat Sardar, Erum Jabeen, Hira Karim, Asad Mumtaz. Enhanced antioxidant activity in Imidazolium-based protic organic salts: An insight into structure activity relationship via experimental and modelling approaches. Journal of Molecular Liquids 2024, 404 , 124964. https://doi.org/10.1016/j.molliq.2024.124964
    7. Ahmed Bahaa, Ayoob Alhammadi, Kallidanthiyil Chellappan Lethesh, Rahmat Agung Susantyoko, Musbaudeen O. Bamgbopa. Ionic liquid electrolyte selection for high voltage supercapacitors in high-temperature applications. Frontiers in Chemistry 2024, 12 https://doi.org/10.3389/fchem.2024.1349864
    8. Mohammad Bagheri, Hemayat Shekaari, Fariba Ghaffari, Firouzeh Mousavi. Solute- solvent interactions between ethanolamine-based protic ionic liquids and lithium bromide in aqueous media using volumetric, acoustic and transport properties. Journal of Molecular Liquids 2024, 397 , 124125. https://doi.org/10.1016/j.molliq.2024.124125
    9. Małgorzata Smuga-Kogut, Bartosz Walendzik, Katarzyna Lewicka-Rataj, Tomasz Kogut, Leszek Bychto, Piotr Jachimowicz, Agnieszka Cydzik-Kwiatkowska. Application of Proton Ionic Liquid in the Process of Obtaining Bioethanol from Hemp Stalks. Energies 2024, 17 (4) , 972. https://doi.org/10.3390/en17040972
    10. Ezinne C. Achinivu, Brian W. Blankenship, Nawa Raj Baral, Hemant Choudhary, Ramu Kakumanu, Mood Mohan, Edward E.K. Baidoo, Corinne D. Scown, Anthe George, Blake A. Simmons, John Gladden. Biomass pretreatment with distillable ionic liquids for an effective recycling and recovery approach. Chemical Engineering Journal 2024, 479 , 147824. https://doi.org/10.1016/j.cej.2023.147824
    11. Paul Wolski, Brian W. Blankenship, Athiyya Umar, Mica Cabrera, Blake A. Simmons, Kenneth L. Sale, Ezinne C. Achinivu. Factors that influence the activity of biomass-degrading enzymes in the presence of ionic liquids—a review. Frontiers in Energy Research 2023, 11 https://doi.org/10.3389/fenrg.2023.1212719
    12. Roger Arthur Sheldon. The E factor at 30: a passion for pollution prevention. Green Chemistry 2023, 25 (5) , 1704-1728. https://doi.org/10.1039/D2GC04747K
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    ACS Sustainable Chemistry & Engineering

    Cite this: ACS Sustainable Chem. Eng. 2022, 10, 37, 12090–12098
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acssuschemeng.2c01211
    Published September 8, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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