A novel approach to prepare Cu(I)Zn@MIL-100(Fe) adsorbent with high CO adsorption capacity, CO/CO2 selectivity and stability via controlled host–guest redox reaction

Van Nhieu Le; The Ky Vo; Jeong Hyeon Lee; Jin Chul Kim; Tea Hoon Kim; Kwang Hyun Oh; Youn Sang Bae; Sang Kyu Kwak; Jinsoo Kim

doi:10.1016/j.cej.2020.126492

A novel approach to prepare Cu(I)Zn@MIL-100(Fe) adsorbent with high CO adsorption capacity, CO/CO₂ selectivity and stability via controlled host–guest redox reaction

Van Nhieu Le, The Ky Vo, Jeong Hyeon Lee, Jin Chul Kim, Tea Hoon Kim, Kwang Hyun Oh, Youn Sang Bae, Sang Kyu Kwak, Jinsoo Kim

Department of Chemical and Biomolecular Engineering

Research output: Contribution to journal › Article › peer-review

30 Citations (Scopus)

Abstract

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 (1 0 4) 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 σ-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 π-complexation adsorbents with high CO/CO₂ selectivity and superior oxygen resistance.

Original language	English
Article number	126492
Journal	Chemical Engineering Journal
Volume	404
DOIs	https://doi.org/10.1016/j.cej.2020.126492
Publication status	Published - 2021 Jan 15

Bibliographical note

Funding Information:
This work was supported by “Next Generation Carbon Upcycling Project” (NRF-2017M1A2A2043451 and 2017M1A2A2043449) and the Engineering Research Center of Excellence Program (NRF-2014R1A5A1009799) through the National Research Foundation of Korea. (NRF) funded by the Ministry of Science and ICT, Republic of Korea.

Funding Information:
This work was supported by “Next Generation Carbon Upcycling Project” (NRF-2017M1A2A2043451 and 2017M1A2A2043449) and the Engineering Research Center of Excellence Program (NRF-2014R1A5A1009799) through the National Research Foundation of Korea. (NRF) funded by the Ministry of Science and ICT , Republic of Korea.

Publisher Copyright:
© 2020 Elsevier B.V.

All Science Journal Classification (ASJC) codes

Chemistry(all)
Environmental Chemistry
Chemical Engineering(all)
Industrial and Manufacturing Engineering

Access to Document

10.1016/j.cej.2020.126492

Cite this

@article{7f89fcf7264f4040805b37485074ab90,

title = "A novel approach to prepare Cu(I)Zn@MIL-100(Fe) adsorbent with high CO adsorption capacity, CO/CO2 selectivity and stability via controlled host–guest redox reaction",

abstract = "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 (1 0 4) 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 σ-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 π-complexation adsorbents with high CO/CO2 selectivity and superior oxygen resistance.",

author = "Le, {Van Nhieu} and Vo, {The Ky} and Lee, {Jeong Hyeon} and Kim, {Jin Chul} and Kim, {Tea Hoon} and Oh, {Kwang Hyun} and Bae, {Youn Sang} and Kwak, {Sang Kyu} and Jinsoo Kim",

note = "Funding Information: This work was supported by “Next Generation Carbon Upcycling Project” (NRF-2017M1A2A2043451 and 2017M1A2A2043449) and the Engineering Research Center of Excellence Program (NRF-2014R1A5A1009799) through the National Research Foundation of Korea. (NRF) funded by the Ministry of Science and ICT, Republic of Korea. Funding Information: This work was supported by “Next Generation Carbon Upcycling Project” (NRF-2017M1A2A2043451 and 2017M1A2A2043449) and the Engineering Research Center of Excellence Program (NRF-2014R1A5A1009799) through the National Research Foundation of Korea. (NRF) funded by the Ministry of Science and ICT , Republic of Korea. Publisher Copyright: {\textcopyright} 2020 Elsevier B.V.",

year = "2021",

month = jan,

day = "15",

doi = "10.1016/j.cej.2020.126492",

language = "English",

volume = "404",

journal = "Chemical Engineering Journal",

issn = "1385-8947",

publisher = "Elsevier",

}

TY - JOUR

T1 - A novel approach to prepare Cu(I)Zn@MIL-100(Fe) adsorbent with high CO adsorption capacity, CO/CO2 selectivity and stability via controlled host–guest redox reaction

AU - Le, Van Nhieu

AU - Vo, The Ky

AU - Lee, Jeong Hyeon

AU - Kim, Jin Chul

AU - Kim, Tea Hoon

AU - Oh, Kwang Hyun

AU - Bae, Youn Sang

AU - Kwak, Sang Kyu

AU - Kim, Jinsoo

N1 - Funding Information: This work was supported by “Next Generation Carbon Upcycling Project” (NRF-2017M1A2A2043451 and 2017M1A2A2043449) and the Engineering Research Center of Excellence Program (NRF-2014R1A5A1009799) through the National Research Foundation of Korea. (NRF) funded by the Ministry of Science and ICT, Republic of Korea. Funding Information: This work was supported by “Next Generation Carbon Upcycling Project” (NRF-2017M1A2A2043451 and 2017M1A2A2043449) and the Engineering Research Center of Excellence Program (NRF-2014R1A5A1009799) through the National Research Foundation of Korea. (NRF) funded by the Ministry of Science and ICT , Republic of Korea. Publisher Copyright: © 2020 Elsevier B.V.

PY - 2021/1/15

Y1 - 2021/1/15

N2 - 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 (1 0 4) 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 σ-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 π-complexation adsorbents with high CO/CO2 selectivity and superior oxygen resistance.

AB - 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 (1 0 4) 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 σ-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 π-complexation adsorbents with high CO/CO2 selectivity and superior oxygen resistance.

UR - http://www.scopus.com/inward/record.url?scp=85089069332&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85089069332&partnerID=8YFLogxK

U2 - 10.1016/j.cej.2020.126492

DO - 10.1016/j.cej.2020.126492

M3 - Article

AN - SCOPUS:85089069332

SN - 1385-8947

VL - 404

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

M1 - 126492

ER -