Highly Selective CO₂ Separation on Na-exchanged DNL-6 Synthesized by Utilization of Spent Industrial Catalyst

Abstract

Conversion of industrial solid wastes into functional materials has attracted considerable interest, as it can reduce environmental pollution and facilitate the sustainable development of relevant processes. Herein, spent methanol-to-olefins (MTO) industrial catalyst was explored for the synthesis of DNL-6 molecular sieve, a promising SAPO-type adsorbent for CO₂ capture. It was demonstrated that DNL-6 with high purity and crystallinity, and various silica contents can be readily synthesized. Na-exchanged DNL-6 was further prepared using the as-synthesized DNL-6 as the precursor, and its structure was investigated by Rietveld refinement, revealing that Na cations were mainly located in the single 8-rings (S8Rs). Na-DNL-6 with varied silica contents and Na contents were investigated for adsorption studies. Na-DNL-6 with a high Na exchange degree exhibited comparable CO₂ uptake with H-DNL-6 (298 K and 101 kPa), but superior separation selectivity for CO₂/CH₄ (as high as 1369, 50/50 kPa) and CO₂/N₂ (∞, 15/85 kPa) owing to the “trapdoor” effect associated with the Na cations sited in the S8Rs. This work provides an eco-friendly approach for the synthesis of efficient silicoaluminophosphate adsorbent for CO₂ capture.

Keywords

DNL-6 / SAPO molecular sieve / Synthesis / CO₂ separation / Spent industrial catalyst

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