Energy-Efficient Microbial Electrochemical Lignin and Alkaline Hydroxide Recovery from DMR Black Liquor

Jiang, Jinyue; Chen, Xi; Chen, Xiaowen; Ren, Zhiyong Jason

doi:10.1016/j.resconrec.2022.106529

Energy-Efficient Microbial Electrochemical Lignin and Alkaline Hydroxide Recovery from DMR Black Liquor

Journal Article · 18 July 2022 · Resources, Conservation and Recycling

DOI:https://doi.org/10.1016/j.resconrec.2022.106529· OSTI ID:1882675

Jiang, Jinyue; Chen, Xi; Chen, Xiaowen; Ren, Zhiyong Jason

Black liquor is a complex waste stream generated from the fast-expanding biorefinery industry, and the high management cost has been known as a major development barrier. In this work, we demonstrated a rationally designed 4-chamber microbial electrolysis process that was capable of recovering the value-added lignin, NaOH, and H2 products while removing waste organics from the Deacetylation and Mechanical Refining (DMR) black liquor, which could potentially reduce the disposal cost by up to 40%. The lab-scale MEC achieved 52% organic removal from a highly concentrated feedstock (28,960 ± 212 mg/L COD) and recovered 83.2 mM NaOH under a small voltage application (1.2 V). Lignin recovery was observed to be as high as 13.98 +/- 0.28 g/L, and 0.35 L/L/day H2 was produced with a faradaic efficiency of 93.5%. This work provided a good example on how complex liquid waste stream can be valorized via multi-functional microbial electrochemical technology, and how the traditionally unfavored pH gradient in an electrochemical reactor can be manipulated for lignin precipitation and alkaline recovery at the same time. The versatility and good performance in concurrent contaminants removal, lignin precipitation, H2 production and NaOH recovery demonstrate a good potential for microbial electrolysis in black liquor treatment.

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office (BETO)

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 1882675

Report Number(s):: NREL/JA-5100-83770; MainId:84543; UUID:fc3482d2-17dd-47e3-befd-b8c8ff575adb; MainAdminID:65132

Journal Information:: Resources, Conservation and Recycling, Vol. 186

Country of Publication:: United States

Language:: English

References (60)

Electrochemical Treatment of Black Liquor from Straw Pulping Blanco, M. A.; Negro, C.; Tijero, J. Separation Science and Technology, Vol. 31, Issue 19 https://doi.org/10.1080/01496399608000821	journal	November 1996
Supply Chain Sustainability Analysis of Renewable Hydrocarbon Fuels via Indirect Liquefaction, Ex Situ Catalytic Fast Pyrolysis, Hydrothermal Liquefaction, Combined Algal Processing, and Biochemical Conversion: Update of the 2019 State-of-Technology Cases Cai, Hao; Ou, Longwen; Wang, Michael https://doi.org/10.2172/1616516	report	March 2020
Hydrogen Production in a Single Chamber Microbial Electrolysis Cell Lacking a Membrane Call, Douglas; Logan, Bruce E. Environmental Science & Technology, Vol. 42, Issue 9, p. 3401-3406 https://doi.org/10.1021/es8001822	journal	May 2008
Rapid and near-complete dissolution of wood lignin at ≤80°C by a recyclable acid hydrotrope Chen, Liheng; Dou, Jinze; Ma, Qianli Science Advances, Vol. 3, Issue 9 https://doi.org/10.1126/sciadv.1701735	journal	September 2017
Development of the Microbial Electrolysis Desalination and Chemical-Production Cell for Desalination as Well as Acid and Alkali Productions Chen, Shanshan; Liu, Guangli; Zhang, Renduo Environmental Science & Technology, Vol. 46, Issue 4 https://doi.org/10.1021/es203332g	journal	January 2012
The Microbial Electrochemical Current Accelerates Urea Hydrolysis for Recovery of Nutrients from Source-Separated Urine Chen, Xi; Gao, Yifan; Hou, Dianxun Environmental Science & Technology Letters, Vol. 4, Issue 7 https://doi.org/10.1021/acs.estlett.7b00168	journal	May 2017
DMR (deacetylation and mechanical refining) processing of corn stover achieves high monomeric sugar concentrations (230 g L ⁻¹ ) during enzymatic hydrolysis and high ethanol concentrations (>10% v/v) during fermentation without hydrolysate purification or concentration Chen, Xiaowen; Kuhn, Erik; Jennings, Edward W. Energy & Environmental Science, Vol. 9, Issue 4 https://doi.org/10.1039/C5EE03718B	journal	January 2016
Recycling of Dilute Deacetylation Black Liquor to Enable Efficient Recovery and Reuse of Spent Chemicals and Biomass Pretreatment Waste Chen, Xiaowen; Kuhn, Erik; Nagle, Nick Frontiers in Energy Research, Vol. 6 https://doi.org/10.3389/fenrg.2018.00051	journal	June 2018
Microbial electrochemical treatment of biorefinery black liquor and resource recovery Chen, Xi; Katahira, Rui; Ge, Zheng Green Chemistry, Vol. 21, Issue 6 https://doi.org/10.1039/C8GC02909A	journal	January 2019
Electrolysis of weak black liquor Part II: Effect of process parameters on the energy efficiency of the electrolytic cell Cloutier, J. -N.; Azarniouch, M. K.; Callender, D. Journal of Applied Electrochemistry, Vol. 25, Issue 5 https://doi.org/10.1007/BF00260690	journal	May 1995
Performance of a pilot-scale continuous flow microbial electrolysis cell fed winery wastewater Cusick, Roland D.; Bryan, Bill; Parker, Denny S. Applied Microbiology and Biotechnology, Vol. 89, Issue 6 https://doi.org/10.1007/s00253-011-3130-9	journal	February 2011
Impact of applied voltage on methane generation and microbial activities in an anaerobic microbial electrolysis cell (MEC) Ding, Aqiang; Yang, Yu; Sun, Guodong Chemical Engineering Journal, Vol. 283 https://doi.org/10.1016/j.cej.2015.07.054	journal	January 2016
Scaling-up of membraneless microbial electrolysis cells (MECs) for domestic wastewater treatment: Bottlenecks and limitations Escapa, A.; San-Martín, M. I.; Mateos, R. Bioresource Technology, Vol. 180 https://doi.org/10.1016/j.biortech.2014.12.096	journal	March 2015
Electrochemical acidification of Kraft black liquor: Impacts of pulsed electric field application on bipolar membrane colloidal fouling and process intensification Haddad, Maryam; Bazinet, Laurent; Savadogo, Oumarou Journal of Membrane Science, Vol. 524 https://doi.org/10.1016/j.memsci.2016.10.043	journal	February 2017
A feasibility study of a novel electro-membrane based process to acidify Kraft black liquor and extract lignin Haddad, Maryam; Bazinet, Laurent; Savadogo, Oumarou Process Safety and Environmental Protection, Vol. 106 https://doi.org/10.1016/j.psep.2016.10.003	journal	February 2017
Effect of electrolyte pH on the rate of the anodic and cathodic reactions in an air-cathode microbial fuel cell He, Zhen; Huang, Yuelong; Manohar, Aswin K. Bioelectrochemistry, Vol. 74, Issue 1 https://doi.org/10.1016/j.bioelechem.2008.07.007	journal	November 2008
Exploring the use of electrochemical impedance spectroscopy (EIS) in microbial fuel cell studies He, Zhen; Mansfeld, Florian Energy Environ. Sci., Vol. 2, Issue 2 https://doi.org/10.1039/B814914C	journal	January 2009
Production of hydrogen from domestic wastewater in a pilot-scale microbial electrolysis cell Heidrich, E. S.; Dolfing, J.; Scott, K. Applied Microbiology and Biotechnology, Vol. 97, Issue 15 https://doi.org/10.1007/s00253-012-4456-7	journal	October 2012
Performance of a pilot scale microbial electrolysis cell fed on domestic wastewater at ambient temperatures for a 12 month period Heidrich, Elizabeth S.; Edwards, Stephen R.; Dolfing, Jan Bioresource Technology, Vol. 173 https://doi.org/10.1016/j.biortech.2014.09.083	journal	December 2014
Hydrogen production using single-chamber membrane-free microbial electrolysis cells Hu, Hongqiang; Fan, Yanzhen; Liu, Hong Water Research, Vol. 42, Issue 15 https://doi.org/10.1016/j.watres.2008.06.015	journal	September 2008
Efficient extraction of lignin from black liquor via a novel membrane-assisted electrochemical approach Jin, Wei; Tolba, Rasha; Wen, Jiali Electrochimica Acta, Vol. 107 https://doi.org/10.1016/j.electacta.2013.06.031	journal	September 2013
Base-Catalyzed Depolymerization of Biorefinery Lignins Katahira, Rui; Mittal, Ashutosh; McKinney, Kellene ACS Sustainable Chemistry & Engineering, Vol. 4, Issue 3 https://doi.org/10.1021/acssuschemeng.5b01451	journal	December 2015
Influence of catholyte pH and temperature on hydrogen production from acetate using a two chamber concentric tubular microbial electrolysis cell Kyazze, Godfrey; Popov, Arseniy; Dinsdale, Richard International Journal of Hydrogen Energy, Vol. 35, Issue 15 https://doi.org/10.1016/j.ijhydene.2010.05.036	journal	August 2010
Impact of applied cell voltage on the performance of a microbial electrolysis cell fully catalysed by microorganisms Lim, Swee Su; Fontmorin, Jean-Marie; Izadi, Paniz International Journal of Hydrogen Energy, Vol. 45, Issue 4 https://doi.org/10.1016/j.ijhydene.2019.11.142	journal	January 2020
Bioanode as a limiting factor to biocathode performance in microbial electrolysis cells Lim, Swee Su; Yu, Eileen Hao; Daud, Wan Ramli Wan Bioresource Technology, Vol. 238 https://doi.org/10.1016/j.biortech.2017.03.127	journal	August 2017
Electrochemically Assisted Microbial Production of Hydrogen from Acetate Liu, Hong; Grot, Stephen; Logan, Bruce E. Environmental Science & Technology, Vol. 39, Issue 11 https://doi.org/10.1021/es050244p	journal	June 2005
Microbial Electrolysis Cells for High Yield Hydrogen Gas Production from Organic Matter Logan, Bruce E.; Call, Douglas; Cheng, Shaoan Environmental Science & Technology, Vol. 42, Issue 23 https://doi.org/10.1021/es801553z	journal	December 2008
Active H ₂ Harvesting Prevents Methanogenesis in Microbial Electrolysis Cells Lu, Lu; Hou, Dianxun; Wang, Xin Environmental Science & Technology Letters, Vol. 3, Issue 8 https://doi.org/10.1021/acs.estlett.6b00209	journal	July 2016
Spontaneous Solar Syngas Production from CO2 Driven by Energetically Favorable Wastewater Microbial Anodes Lu, Lu; Li, Zhida; Chen, Xi Joule, Vol. 4, Issue 10 https://doi.org/10.1016/j.joule.2020.08.014	journal	October 2020
Unbiased solar H ₂ production with current density up to 23 mA cm ⁻² by Swiss-cheese black Si coupled with wastewater bioanode Lu, Lu; Vakki, Waltteri; Aguiar, Jeffery A. Energy & Environmental Science, Vol. 12, Issue 3 https://doi.org/10.1039/C8EE03673J	journal	January 2019
Microbial community structure accompanied with electricity production in a constructed wetland plant microbial fuel cell Lu, Lu; Xing, Defeng; Ren, Zhiyong Jason Bioresource Technology, Vol. 195 https://doi.org/10.1016/j.biortech.2015.05.098	journal	November 2015
Enhanced bioremediation of hydrocarbon-contaminated soil using pilot-scale bioelectrochemical systems Lu, Lu; Yazdi, Hadi; Jin, Song Journal of Hazardous Materials, Vol. 274 https://doi.org/10.1016/j.jhazmat.2014.03.060	journal	June 2014
Microbial desalination cells for improved performance in wastewater treatment, electricity production, and desalination Luo, Haiping; Xu, Pei; Roane, Timberley M. Bioresource Technology, Vol. 105 https://doi.org/10.1016/j.biortech.2011.11.098	journal	February 2012
Methane Production in Microbial Reverse-Electrodialysis Methanogenesis Cells (MRMCs) Using Thermolytic Solutions Luo, Xi; Zhang, Fang; Liu, Jia Environmental Science & Technology, Vol. 48, Issue 15 https://doi.org/10.1021/es501979z	journal	July 2014
An Evaluation of the Acid-Soluble Lignin Determination in Analyses of Lignin by the Sulfuric Acid Method Maekawa, Eiichi; Ichizawa, Taizo; Koshijima, Testuo Journal of Wood Chemistry and Technology, Vol. 9, Issue 4 https://doi.org/10.1080/02773818908050315	journal	December 1989
Bioelectrochemical treatment of table olive brine processing wastewater for biogas production and phenolic compounds removal Marone, A.; Carmona-Martínez, A. A.; Sire, Y. Water Research, Vol. 100 https://doi.org/10.1016/j.watres.2016.05.008	journal	September 2016
Microbial Electrodialysis Cell for Simultaneous Water Desalination and Hydrogen Gas Production Mehanna, Maha; Kiely, Patrick D.; Call, Douglas F. Environmental Science & Technology, Vol. 44, Issue 24 https://doi.org/10.1021/es1025646	journal	November 2010
Trends in bioconversion of lignocellulose: Biofuels, platform chemicals & biorefinery concept Menon, Vishnu; Rao, Mala Progress in Energy and Combustion Science, Vol. 38, Issue 4 https://doi.org/10.1016/j.pecs.2012.02.002	journal	August 2012
Alkaline black liquor treatment by continuous electrodialysis Mishra, A. K.; Bhattacharya, P. K. Journal of Membrane Science, Vol. 33, Issue 1 https://doi.org/10.1016/S0376-7388(00)80053-8	journal	August 1987
Generation of Hydrogen, Lignin and Sodium Hydroxide from Pulping Black Liquor by Electrolysis Nong, Guangzai; Zhou, Zongwen; Wang, Shuangfei Energies, Vol. 9, Issue 1 https://doi.org/10.3390/en9010013	journal	December 2015
Physico-Chemical Characterization of a Fractionated Kraft Lignin Norgren, Magnus; Lindström, Birger Holzforschung, Vol. 54, Issue 5 https://doi.org/10.1515/HF.2000.089	journal	September 2000
Bipolar membranes: A review on principles, latest developments, and applications Pärnamäe, R.; Mareev, S.; Nikonenko, V. Journal of Membrane Science, Vol. 617 https://doi.org/10.1016/j.memsci.2020.118538	journal	January 2021
Electroactive mixed culture derived biofilms in microbial bioelectrochemical systems: The role of pH on biofilm formation, performance and composition Patil, Sunil A.; Harnisch, Falk; Koch, Christin Bioresource Technology, Vol. 102, Issue 20 https://doi.org/10.1016/j.biortech.2011.07.087	journal	October 2011
Formation of uniform colloidal spheres from lignin, a renewable resource recovered from pulping spent liquor Qian, Yong; Deng, Yonghong; Qiu, Xueqing Green Chemistry, Vol. 16, Issue 4 https://doi.org/10.1039/c3gc42131g	journal	January 2014
pK _a -Values of Guaiacyl and Syringyl Phenols Related to Lignin Ragnar, Martin; Lindgren, Christofer T.; Nilvebrant, Nils-Olof Journal of Wood Chemistry and Technology, Vol. 20, Issue 3 https://doi.org/10.1080/02773810009349637	journal	August 2000
A Two-Stage Microbial Fuel Cell and Anaerobic Fluidized Bed Membrane Bioreactor (MFC-AFMBR) System for Effective Domestic Wastewater Treatment Ren, Lijiao; Ahn, Yongtae; Logan, Bruce E. Environmental Science & Technology, Vol. 48, Issue 7 https://doi.org/10.1021/es500737m	journal	March 2014
Microbial electrolysis cell (MEC): Strengths, weaknesses and research needs from electrochemical engineering standpoint Rousseau, Raphaël; Etcheverry, Luc; Roubaud, Emma Applied Energy, Vol. 257 https://doi.org/10.1016/j.apenergy.2019.113938	journal	January 2020
Effects of Membrane Cation Transport on pH and Microbial Fuel Cell Performance ^† Rozendal, René A.; Hamelers, Hubertus V. M.; Buisman, Cees J. N. Environmental Science & Technology, Vol. 40, Issue 17 https://doi.org/10.1021/es060387r	journal	September 2006
Microbial electrolysis treatment of post-hydrothermal liquefaction wastewater with hydrogen generation Shen, Ruixia; Jiang, Yong; Ge, Zheng Applied Energy, Vol. 212 https://doi.org/10.1016/j.apenergy.2017.12.065	journal	February 2018
Separation of Lignin from Corn Stover Hydrolysate with Quantitative Recovery of Ionic Liquid Underkofler, Kaylee A.; Teixeira, Rodrigo E.; Pietsch, Stephen A. ACS Sustainable Chemistry & Engineering, Vol. 3, Issue 4 https://doi.org/10.1021/sc500731c	journal	March 2015
Recycled tire crumb rubber anodes for sustainable power production in microbial fuel cells Wang, Heming; Davidson, Matthew; Zuo, Yi Journal of Power Sources, Vol. 196, Issue 14 https://doi.org/10.1016/j.jpowsour.2011.01.082	journal	July 2011
Practical Energy Harvesting for Microbial Fuel Cells: A Review Wang, Heming; Park, Jae-Do; Ren, Zhiyong Jason Environmental Science & Technology, Vol. 49, Issue 6 https://doi.org/10.1021/es5047765	journal	February 2015
A comprehensive review of microbial electrochemical systems as a platform technology Wang, Heming; Ren, Zhiyong Jason Biotechnology Advances, Vol. 31, Issue 8 https://doi.org/10.1016/j.biotechadv.2013.10.001	journal	December 2013
Impact of applied current on sulfate-rich wastewater treatment and microbial biodiversity in the cathode chamber of microbial electrolysis cell (MEC) reactor Wang, Kai; Sheng, Yuxing; Cao, Hongbin Chemical Engineering Journal, Vol. 307 https://doi.org/10.1016/j.cej.2016.07.106	journal	January 2017
Characterization and Deconstruction of Oligosaccharides in Black Liquor From Deacetylation Process of Corn Stover Wang, Wei; Chen, Xiaowen; Katahira, Rui Frontiers in Energy Research, Vol. 7 https://doi.org/10.3389/fenrg.2019.00054	journal	June 2019
Formation and chemical structures of acid-soluble lignin I: sulfuric acid treatment time and acid-soluble lignin content of hardwood Yasuda, Seiichi; Fukushima, Kazuhiko; Kakehi, Akihiro Journal of Wood Science, Vol. 47, Issue 1 https://doi.org/10.1007/BF00776648	journal	February 2001
COD removal characteristics in air-cathode microbial fuel cells Zhang, Xiaoyuan; He, Weihua; Ren, Lijiao Bioresource Technology, Vol. 176 https://doi.org/10.1016/j.biortech.2014.11.001	journal	January 2015
Recent advances in microbial fuel cells (MFCs) and microbial electrolysis cells (MECs) for wastewater treatment, bioenergy and bioproducts Zhou, Minghua; Wang, Hongyu; Hassett, Daniel J. Journal of Chemical Technology & Biotechnology, Vol. 88, Issue 4 https://doi.org/10.1002/jctb.4004	journal	January 2013
Lightweight, conductive hollow fibers from nature as sustainable electrode materials for microbial energy harvesting Zhu, Hongli; Wang, Heming; Li, Yuanyuan Nano Energy, Vol. 10 https://doi.org/10.1016/j.nanoen.2014.08.014	journal	November 2014
Self-Driven Desalination and Advanced Treatment of Wastewater in a Modularized Filtration Air Cathode Microbial Desalination Cell Zuo, Kuichang; Wang, Zhen; Chen, Xi Environmental Science & Technology, Vol. 50, Issue 13 https://doi.org/10.1021/acs.est.6b00520	journal	June 2016

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