VALORIZATION OF BIOGAS THROUGH SIMULTANEOUS CO₂ AND H₂S REMOVAL BY RENEWABLE AQUEOUS AMMONIA SOLUTION IN MEMBRANE CONTACTOR

Highlights

● Simultaneous H₂S and CO₂ removal from biogas is studied.

● Renewable absorbent from biogas slurry is used in membrane contactor.

● More than 98% of H₂S can be removed by membrane absorption.

● The impurities have less influence on H₂S removal efficiency.

Abstract

Upgrading biogas into biomethane not only improves the biogas utilization as vehicle fuel or natural gas substitute, but also reduces the greenhouse gases emissions. Considering the principle of engineering green energy process, the renewable aqueous ammonia (RAA) solution obtained from biogas slurry was used to remove H₂S and CO₂ simultaneously in the hollow fiber membrane contactor. RAA was mimicked in this study using the ammonia aqueous solution mixed with some typical impurities including ethanol, acetic acid, propionic acid, butyric acid and NH₄HCO₃. Compared with the typical physical absorption (i.e., pure water) removing 48% of H₂S from biogas, RAA with 0.1 mol·L⁻¹ NH₃ could remove 97% of H₂S. Increasing the NH₃ concentration from 0.1 to 0.5 mol·L⁻¹ could elevate the CO₂ absorption flux from 0.97 to 1.72 mol·m⁻²·h⁻¹ by 77.3%. Among the impurities contained in RAA, ethanol has a less impact on CO₂ absorption, while other impurities like CO₂ and acetic acid have significant negative impacts on CO₂ absorption. Fortunately, the impurities have a less influence on H₂S removal efficiency, with more than 98% of H₂S could be removed by RAA. Also, the influences of operating parameters on acid gases removal were investigated to provide some engineering suggestions.

Graphical abstract

Keywords

biomethane / biogas purification / CO₂ removal / H₂S removal / membrane absorption

References

[1] Ullah Khan I, Othman M H D, Hashim H, Matsuura T, Ismail A F, Rezaei-DashtArzhandi M, Wan Azelee I. Biogas as a renewable energy fuel—A review of biogas upgrading, utilisation and storage. Energy Conversion and Management, 2017, 150: 277–294

[2] Hakawati R, Smyth B M, McCullough G, De Rosa F, Rooney D. What is the most energy efficient route for biogas utilization: Heat, electricity or transport. Applied Energy, 2017, 206: 1076–1087

[3] Hoo P Y, Hashim H, Ho W S, Yunus N A. Spatial-economic optimisation of biomethane injection into natural gas grid: The case at southern Malaysia. Journal of Environmental Management, 2019, 241: 603–611

[4] Bak C, Lim C J, Kim Y D, Kim W S. Multi-stage adsorptive purification process for improving desulfurization performance of biogas. Separation and Purification Technology, 2019, 227: 115702

[5] Al Mamun M R, Torii S, Rahman M M, Karim M R. Physico-chemical elimination of unwanted CO₂, H₂S and H₂O fractions from biomethane. Sustainable Energy & Fuels, 2019, 3(1): 166–172

[6] Sarker S, Lamb J J, Hjelme D R, Lien K M. Overview of recent progress towards in-situ biogas upgradation techniques. Fuel, 2018, 226: 686–697

[7] Lombardi L, Francini G. Techno-economic and environmental assessment of the main biogas upgrading technologies. Renewable Energy, 2020, 156: 440–458

[8] Von der Assen N, Jung J, Bardow A. Life-cycle assessment of carbon dioxide capture and utilization: avoiding the pitfalls. Energy & Environmental Science, 2013, 6(9): 2721–2734

[9] Miltner M, Makaruk A, Harasek M. Review on available biogas upgrading technologies and innovations towards advanced solutions. Journal of Cleaner Production, 2017, 161: 1329–1337

[10] Sun Q, Li H, Yan J, Liu L, Yu Z, Yu X. Selection of appropriate biogas upgrading technology—A review of biogas cleaning, upgrading and utilisation. Renewable & Sustainable Energy Reviews, 2015, 51: 521–532

[11] Abdeen F R H, Mel M, Jami M S, Ihsan S I, Ismail A F. A review of chemical absorption of carbon dioxide for biogas upgrading. Chinese Journal of Chemical Engineering, 2016, 24(6): 693–702

[12] Ruane A C, Phillips M M, Rosenzweig C. Climate shifts within major agricultural seasons for +1.5 and +2.0 ℃ worlds: HAPPI projections and AgMIP modeling scenarios. Agricultural and Forest Meteorology, 2018, 259: 329–344

[13] He Q, Yu G, Wang W, Yan S, Zhang Y, Zhao S. Once-through CO₂ absorption for simultaneous biogas upgrading and fertilizer production. Fuel Processing Technology, 2017, 166: 50–58

[14] He Q, Shi M, Liang F, Xu L, Ji L, Yan S. Renewable absorbents for CO₂ capture: from biomass to nature. Greenhouse Gases, 2019, 9(4): 637–651

[15] McLeod A, Jefferson B, McAdam E J. Biogas upgrading by chemical absorption using ammonia rich absorbents derived from wastewater. Water Research, 2014, 67: 175–186

[16] He Q, Yu G, Tu T, Yan S, Zhang Y, Zhao S. Closing CO₂ loop in biogas production: recycling ammonia as fertilizer. Environmental Science & Technology, 2017, 51(15): 8841–8850

[17] Bavarella S, Hermassi M, Brookes A, Moore A, Vale P, Moon I S, Pidou M, McAdam E J. Recovery and concentration of ammonia from return liquor to promote enhanced CO₂ absorption and simultaneous ammonium bicarbonate crystallisation during biogas upgrading in a hollow fibre membrane contactor. Separation and Purification Technology, 2020, 241: 116631

[18] Liang F, Tu T, Yu G, Wang W, He Q, Yan S, Ran Y. Ecological treatment of MEA aqueous solution using hydroponic method. International Journal of Energy for a Clean Environment, 2018, 19(3−4): 143−155

[19] Bonet-Ruiz A E, Plesu V, Bonet J, Iancu P, Llorens J. Preliminary technical feasibility analysis of carbon dioxide absorption by ecological residual solvents rich in ammonia to be used in fertigation. Clean Technologies and Environmental Policy, 2015, 17(5): 1313–1321

[20] He Q Y, Yu G, Yan S P, Dumee L F, Zhang Y L, Strezov V, Zhao S F. Renewable CO₂ absorbent for carbon capture and biogas upgrading by membrane contactor. Separation and Purification Technology, 2018, 194: 207–215

[21] He Q, Tu T, Yan S, Yang X, Duke M, Zhang Y, Zhao S. Relating water vapor transfer to ammonia recovery from biogas slurry by vacuum membrane distillation. Separation and Purification Technology, 2018, 191: 182–191

[22] Jin P, Huang C, Shen Y, Zhan X, Hu X, Wang L, Wang L. Simultaneous separation of H₂S and CO₂ from biogas by gas–liquid membrane contactor using single and mixed absorbents. Energy & Fuels, 2017, 31(10): 11117–11126

[23] Pan Z, Zhang N, Zhang W, Zhang Z. Simultaneous removal of CO₂ and H₂S from coalbed methane in a membrane contactor. Journal of Cleaner Production, 2020, 273: 123107

[24] Gusnawan P J, Zha S, Zou L, Zhang G, Yu J. Soybean and moringa based green biosolvents for low-concentration CO₂ capture via a hollow fiber membrane contactor. Chemical Engineering Journal, 2018, 335: 631–637

[25] Bavarella S, Brookes A, Moore A, Vale P, Di Profio G, Curcio E, Hart P, Pidou M, McAdam E J. Chemically reactive membrane crystallisation reactor for CO₂–NH₃ absorption and ammonium bicarbonate crystallisation: kinetics of heterogeneous crystal growth. Journal of Membrane Science, 2020, 599: 117682

[26] He Q, Ji L, Yu B, Yan S, Zhang Y, Zhao S. Renewable aqueous ammonia from biogas slurry for carbon capture: chemical composition and CO₂ absorption rate. International Journal of Greenhouse Gas Control, 2018, 77: 46–54

[27] Yan S P, Fang M X, Zhang W F, Wang S Y, Xu Z K, Luo Z Y, Cen K F. Experimental study on the separation of CO₂ from flue gas using hollow fiber membrane contactors without wetting. Fuel Processing Technology, 2007, 88(5): 501–511

[28] Puxty G, Rowland R, Attalla M. Comparison of the rate of CO₂ absorption into aqueous ammonia and monoethanolamine. Chemical Engineering Science, 2010, 65(2): 915–922

[29] Sander R. Compilation of Henry’s law constants (version 4.0) for water as solvent. Atmospheric Chemistry and Physics, 2015, 15(8): 4399–4981

[30] Atzori F, Barzagli F, Varone A, Cao G, Concas A. CO₂ absorption in aqueous NH₃ solutions: novel dynamic modeling of experimental outcomes. Chemical Engineering Journal, 2023, 451(Part4): 138999

[31] Qin F, Wang S, Hartono A, Svendsen H F, Chen C. Kinetics of CO₂ absorption in aqueous ammonia solution. International Journal of Greenhouse Gas Control, 2010, 4(5): 729–738

[32] Gondal S, Asif N, Svendsen H F, Knuutila H. Density and N₂O solubility of aqueous hydroxide and carbonate solutions in the temperature range from 25 to 80 °C. Chemical Engineering Science, 2015, 122: 307–320

Supplementary materials

The online version of this article at https://doi.org/10.15302/J-FASE-2022473 contains supplementary materials (Tables S1 and others).

Acknowledgements

The authors thank the financial supports from the Natural Science Foundation of Hubei Province of China (2020CFA107, 2020CFB209), the National Natural Science Foundation of China (32002222, 52076101), and the Fundamental Research Funds for the Central Universities (2662021JC004).

Compliance with ethics guidelines

Tao Sun, Wenlong Li, Jiandong Wei, Long Ji, Qingyao He, and Shuiping Yan declare that they have no conflicts of interest or financial conflicts to disclose. This article does not contain any studies with human or animal subjects performed by any of the authors.

RIGHTS & PERMISSIONS

The Author(s) 2022. Published by Higher Education Press. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0)