期刊
CHEMICAL ENGINEERING JOURNAL
卷 404, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2020.126492
关键词
Carbon monoxide (CO); Adsorption; Separation; Adsorbent; Metal-organic framework (MOF); Cu(I)
资金
- Next Generation Carbon Upcycling Project through the National Research Foundation of Korea. (NRF) - Ministry of Science and ICT, Republic of Korea [NRF-2017M1A2A2043451, 2017M1A2A2043449]
- Engineering Research Center of Excellence Program through the National Research Foundation of Korea. (NRF) - Ministry of Science and ICT, Republic of Korea [NRF-2014R1A5A1009799]
- National Research Foundation of Korea [2017M1A2A2043451, 2017M1A2A2043449] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
A novel Cu(I)-incorporated MIL-100(Fe) adsorbent for CO/CO2 separation was prepared using a host-guest redox strategy by exploiting the co-addition of Zn(II) and Cu(II). The addition of Zn(II) resulted in a higher Cu(I) yield of the adsorbent and significantly increased the CO/CO2 selectivity of the resulting Cu(I)Zn@MIL-100(Fe)-10.
The development of a CO-selective adsorbent with large CO adsorption capacity, high CO/CO2 selectivity, and good stability is an industrial challenge. In this study, a novel Cu(I)-incorporated MIL-100(Fe) adsorbent for CO/CO2 separation is prepared using a host-guest redox strategy by exploiting the co-addition of Zn(II) and Cu(II). The addition of Zn(II) resulted in a higher Cu(I) yield of the adsorbent due to the facilitated regeneration of Fe (II), which was utilized for the reduction of Cu(II). Remarkably, the CO/CO2 selectivity (104) of Cu(I)Zn@MIL-100(Fe)-10 was considerably higher than that of the benchmark Cu(I)-incorporated adsorbents. Increasing the Zn(II) concentration in Cu(I)Zn@MIL-100(Fe)-10 improved the oxygen resistance. Density functional theory calculations support our hypothesis that the above improvements are derived from stronger sigma-bonding between Cu(I) and CO and the facilitation of Fe(II) regeneration by the addition of Zn(II). This study opens a new perspective for developing efficient CO-selective pi-complexation adsorbents with high CO/CO2 selectivity and superior oxygen resistance.
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