Controlling the bidirectional chemical environments for high-performance Y@silicalite-1 core-shell composites in shape selective desulfurization

[Display omitted] •Alkali and Cu2+ are used to tune the structure and increase active sites of Y zeolite.•Resin layer and EDA can provide stable external environment for silicalite-1 shell.•Selective-adsorption achieved 75.58 mg/g, double of 37.1 reported previously.•Extraction before calcination kept 92% desulfurization rate after 6 regeneration cycles. A high-performance Y@silicalite-1 core–shell composite for shape- selective adsorption desulfurization was synthesized by controlling the bidirectional chemical environments via a resin interlayer between Y zeolite core and silicalite-1 shell. In this process, the alkali treatment, Cu2+ ion-exchange, Cu2+ equal volume impregnation, resin coating and ethylenediamine modification were applied to work collaboratively for a high shape selectivity and high sulfur adsorption capacity. Results showed that alkali treatment for 2 h, TEOS:Y = 4, Y:3-aminophenol = 1:1, Y: EDA = 1:1 and 550 °C calcination could endow the synthesized core–shell structured composite with a high-performance in shape-selective adsorption desulfurization of DMDS from MTBE solution with a maximum sulfur adsorption capacity of 75.58 mgs/gadsorbents, which was more than double of the best DMDS sulfur adsorption capacity from MTBE (37.07 mgs/gadsorbents) reported previously. The adsorption kinetic and isotherm analysis indicated that the adsorption of DMDS on Y zeolites was monolayer-chemisorption process, and the corresponding theoretical saturated adsorption capacity could reach up to 84.6 mgs/gadsorbents. The regeneration capability can be effectively improved by ethanol extraction before calcination, retaining a high desulfurization rate level at more than 92% even after 6 cycles.