biostudies-literatureDu PNational Natural Science Foundation of China (National Science Foundation of China)1427https://www.ebi.ac.uk/biostudies/studies/S-EPMC8930971biostudies-literatureUnknown13(1)Molecular sieving membranes with uniform pore size are highly desired for carbon dioxide separation. All-silica zeolite membranes feature well-defined micropores, but the size-exclusion effect is significantly compromised by the non-selective macro-pores generated during detemplation. Here we propose a template modulated crystal transition (TMCT) approach to tune the flexibility of Decadodecasil 3 R (DD3R) zeolite to prepare ultra-selective membranes for CO₂/CH₄ separation. An instantaneous overheating is applied to synchronize the template decomposition with the structure relaxation. The organic template molecules are transitionally converted to tight carbon species by the one-minute overheating at 700 °C, which are facilely burnt out by a following moderate thermal treatment. The resulting membranes exhibit CO₂/CH₄ selectivity of 157~1,172 and CO₂ permeance of (890~1,540) × 10^-10mol m^-2 s^-1 Pa^-1. The CO₂ flux and CO₂/CH₄ mixture selectivity reach 3.6 Nm³ m^-2 h^-1 and 43 even at feed pressure up to 31 bar. Such strategy could pave the way of all-silica zeolite membranes to practical applications.Nature communicationsControl of zeolite framework flexibility for ultra-selective carbon dioxide separation.PMC8930971220081112203500221908097Du PJin WGu XZhang YHong ZCanossa SWang XNenert GfalseControl of zeolite framework flexibility for ultra-selective carbon dioxide separation.Molecular sieving membranes with uniform pore size are highly desired for carbon dioxide separation. All-silica zeolite membranes feature well-defined micropores, but the size-exclusion effect is significantly compromised by the non-selective macro-pores generated during detemplation. Here we propose a template modulated crystal transition (TMCT) approach to tune the flexibility of Decadodecasil 3 R (DD3R) zeolite to prepare ultra-selective membranes for CO₂/CH₄ separation. An instantaneous overheating is applied to synchronize the template decomposition with the structure relaxation. The organic template molecules are transitionally converted to tight carbon species by the one-minute overheating at 700 °C, which are facilely burnt out by a following moderate thermal treatment. The resulting membranes exhibit CO₂/CH₄ selectivity of 157~1,172 and CO₂ permeance of (890~1,540) × 10^-10mol m^-2 s^-1 Pa^-1. The CO₂ flux and CO₂/CH₄ mixture selectivity reach 3.6 Nm³ m^-2 h^-1 and 43 even at feed pressure up to 31 bar. Such strategy could pave the way of all-silica zeolite membranes to practical applications.2022-01-01T00:00:00Z2022 Mar2025-04-19T16:19:58.534Z2025-04-19T16:19:58.534ZS-EPMC89309713530132510.1038/s41467-022-29126-6