Chemical Research in Chinese Universities ›› 2024, Vol. 40 ›› Issue (6): 1171-1178.doi: 10.1007/s40242-024-4056-y

• Articles • Previous Articles     Next Articles

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

TANG Yanling1,2, WANG Quanyi2, YAN NaNa2, ZHANG Xiaosi2,3, YANG Miao2, TIAN Peng2, LIU Zhongmin2   

  1. 1. School of Chemistry, Dalian University of Technology, Dalian 116024, P. R. China;
    2. National Engineering Research Center of Lower-Carbon Catalysis Technology, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, P. R. China;
    3. University of Chinese Academy of Sciences, Beijing 100049, P. R. China
  • Received:2024-03-04 Online:2024-12-01 Published:2024-10-26
  • Contact: TIAN Peng,tianpeng@dicp.ac.cn;LIU Zhongmin,liuzm@dicp.ac.cn E-mail:tianpeng@dicp.ac.cn;liuzm@dicp.ac.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (Nos. 21991090, 21991091, 22171259, 22272173) and the AI S&T Program of Yulin Branch, Dalian National Laboratory for Clean Energy, CAS (No. DNL-YL A202206). The authors thank to the funding from the Sino-French IRN (International Research Network).

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.

Key words: DNL-6, SAPO molecular sieve, Synthesis, CO2 separation, Spent industrial catalyst