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Utilization of biogas from wastewater treatment plants (WWTPs) as a kind of renewable energy can effectively alleviate the escalating energy crisis. However, volatile methylsiloxanes (VMS) exist in biogas as impurities and hinder its efficient use. Adsorption is the main technology to achieve high-efficiency purification of VMS currently, yet studies on the adsorption processes and mechanisms are quite insufficient. Here, we use the static vapor adsorption method to investigate the adsorption performances and mechanisms of four typical