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of the entering biogas. Nevertheless, it is important to remark that such a stable performance could not be achieved with- out a drying and desulfurization system. Indeed, water and hydrogen sulfide can dramatically affect the adsorption prop- erties of natural zeolites. A direct comparison with other alternative adsorbents such as mudrocks, silicalite, and sepiolite could not be per- formed since these materials have only been tested with dry, synthetic gas mixtures [11–13]. Within the group of natural zeolites, chabazite resulted to be less sensitive to interferents than clinoptilolite. Indeed, no variations in CO2 adsorption efficiency were observed during all the experimental period (90 days) in the presence of up of H2S higher than 12 mg m23 similar tests performed on clinoptilolite [18] resulted in an efficiency reduction. As a future prospect for the development of a large scale application of this technology, the main difficulties to be overcomed are related to the local availability of natural zeo- lites and the final use of adsorbents. With regard to the final use, natural zeolites can be added to digestate with a slow release effect of nitrogen and water [15,29]. Great amounts of natural zeolites are available in several regions where biome- thane economy is growing rapidly, such as China, Latin America, and Mediterranean Europe [30]. CONCLUSIONS The feasibility of biogas upgrading to biomethane with natural zeolites was demonstrated by developing and moni- toring a prototype VSA plant based on these materials. The regeneration conditions were optimized and pressure was confirmed to be the most important parameter, rather than time and flow rate (Table 3). The VSA was fed for 3 months with a stable source of biogas: an ABR followed by a dehu- midification/desulfurization unit. In the experimental condi- tions, VSA with natural zeolites allows to obtain a biomethane average purity > 8%, with methane recovery >95%. These results are in compliance with national standards and legislations, and make natural zeolites a com- petitive solution for biomethane industry, thanks to their low costs. During all the experimentations, no significant changes were observed in the performances of the VSA unit: this sat- isfactory result is mainly due to the good regenerability of natural zeolites towards CO2 adsorption. Another significant contribute to the stability in biomethane composition was also given by the constant composition of the entering bio- gas, together with the removal of H2O and H2S upstream the VSA. Desulfurization efficiency and VSA off-gas were also monitored, and no critical issues were observed. In conclusion, VSA on natural zeolites was demonstrated to be a mature technology for the industrial production of a high quality biomethane, suitable for injection in natural gas grids and/or for use in automotive vehicles. ACKNOWLEDGMENTS The research is part of the project BioGAME, funded by Regione Lazio (FILAS-CR-2011-1148). The authors express their gratitude to Consorzio Colli Sabini for their kind cooperation. CONFLICTS OF INTEREST The authors declare no conflict of interest. The founding sponsors had no role in the design of the study, in the col- lection, analyses, or interpretation of data, in the writing of the manuscript, and in the decision to publish the results. Literature Cited 1. Liotta, F., d’Antonio, G., Esposito, G., Fabbricino, M., Frunzo, L., van Hullebusch, E.D., Lens, P.N.L., & Pirozzi, F. (2013). Effect of moisture on disintegration kinetics during anaerobic digestion of complex organic substrates, Waste Management & Research, 32, 40–48. 2. Liotta, F., d’Antonio, G., Esposito, G., Fabbricino, M., Van Hullebusch, E.D., Lens, P.N.L., Pirozzi, F., & Pontoni, L. (2014). Effect of total solids content on methane and vol- atile fatty acid production in anaerobic digestion of food waste, Waste Management & Research, 32, 947–953. 3. Cecchi, F., & Cavinato, C. (2015). Anaerobic digestion of bio-waste: A mini-review focusing on territorial and envi- ronmental aspects, Waste Management & Research, 33, 429–438. 4. Andriani, D., Wresta, A., Atmaja, T.D., & Saepudin, A. (2014). A Review on Optimization Production and Upgrading Biogas Through CO2 Removal Using Various Techniques, Applied Biochemistry and Biotechnology, 172, 1909–1928. 5. Rasi, S., L€antel€a, J., & Rintala, J. (2011). Trace compounds affecting biogas energy utilisation - a review, Energy Conversion and Management, 52, 3369–3375. 6. Rychelbosch, E., Drouillon, M., & Vervaeren, H. (2011). Techniques for transformation of biogas to biome thane, Biomass and Bioenergy, 35, 1633–1645. 7. Ling, J., Ntiamoah, A., Xiao, P., Xu, D., Webley, P.A., & Zhai, Y. (2014). Overview of CO2 Capture from Flue Gas Streams by Vacuum Pressure Swing Adsorption Technolo- gy, Austin Chemical Engineering, 1, 1–7. 8. Cavenati, S., Grande, C.A., & Rodrigues, A.E. (2004). Adsorption Equilibrium of Methane, Carbon Dioxide, and Nitrogen on Zeolite 13X at High Pressures, Journal of Chemical & Engineering Data, 49, 1095–1101. 9. Cavenati, S., Grande, C.A., & Rodrigues, A.E. (2005). Upgrade of Methane from Landfill Gas by Pressure Swing Adsorption, Energy & Fuels, 19, 2545–2555. 10. Grande, C.A., & Rodrigues, A.R. (2007). Layered Vacuum Pressure-Swing Adsorption for Biogas Upgrading, Indus- trial & Engineering Chemistry Research, 46, 7844–7848. 11. Delgado, J.A., Uguina, M.A., Sotelo, J.L., Ruız, B., & Rosario, M. (2007). Carbon Dioxide/Methane Separation by Adsorption on Sepiolite, Journal of Natural Gas Chem- istry, 16, 235–243. 12. Delgado, J.A., Uguina, M.A., Sotelo, J.L., Ruız, B., & Gomez, J.M. (2006). Fixed-bed adsorption of carbon dioxide/methane mixtures on silicalite pellets, Adsorp- tion, 12, 5–18. 13. Pini, R. (2014). Assessing the adsorption properties of mudrocks for CO2 sequestration, Energy Procedia, 63, 5556–5561. 14. Ackley, M.W., Rege, S.U., & Saxena, H. (2003). Applica- tion of natural zeolites in the purification and separation of gases, Microporous and Mesoporous Materials, 61, 25– 42. 15. Misaelides, P. (2011). Application of natural zeolites in environmental remediation: A short review, Microporous and Mesoporous Materials, 144, 15–18. 16. Pande, D.R., & Fabiani, C. (1989). Feasibility study on the use of a naturally occurring molecular sieve for methane enrichment from biogas, Gas Separation & Purification, 3, 143–147. 17. Yasyerli, S., Ar, I., Dogu, G., & Dogu, T. (2002). Removal of hydrogen sulphide by clinoptilolite in a fixed bed adsorber, Chemical Engineering and Processing, 41, 785– 792. 18. Alonso-Vicario, A., Ochoa-Gomez, J., Gil-Rıo, S., Gomez- Jimenez-Aberasturi, O., Ramırez-Lopez, C.A., Torrecilla- Soria, J., & Domınguez, A. (2010). Purification and upgrading of biogas by pressure swing adsorption on synthetic and natural zeolites, Microporous and Mesopo- rous Materials, 134, 100–107. Environmental Progress & Sustainable Energy (Vol.00, No.00) DOI 10.1002/ep Month 2017 7PDF Image | Vacuum swing adsorption on natural zeolites
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