Real-time observation of the exchange process between H 2 O and NO in the metal–organic framework Ni-MOF-74
Molecular exchange is a common step occurring in many technological processes such as competitive adsorption, chemical separation, capture, delivery, and release. However, the underlying principle is not fully understood, especially in nanoconfined environments where the energetics and kinetics of s...
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| Published in | Journal of materials chemistry. A, Materials for energy and sustainability Vol. 12; no. 12; pp. 6880 - 6884 |
|---|---|
| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United Kingdom
Royal Society of Chemistry (RSC)
19.03.2024
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| Abstract | Molecular exchange is a common step occurring in many technological processes such as competitive adsorption, chemical separation, capture, delivery, and release. However, the underlying principle is not fully understood, especially in nanoconfined environments where the energetics and kinetics of such processes can deviate from that on flat surfaces. In this paper, we unravel the mechanism of a molecular exchange process by studying the displacement of NO by H
2
O in Ni-MOF-74 in real-time using
in situ
infrared spectroscopy combined with
ab initio
calculations. We show that weakly bound H
2
O gradually displaces strongly bound NO on the metal sites by first weakening the M–N bond through forming H-bond and then moving the NO away so that it eventually desorbs. Interestingly, we further find that additional water facilitates this exchange by significantly lowering the kinetic barrier associated with this process as well as the overall energy of the final state. Although our study focuses on Ni-MOF-74, we believe that our finding and explanation of unexpected exchange phenomena—where strongly adsorbed molecules are apparently easily displaced by much weaker bound H
2
O—is applicable to a much larger group of frameworks and will be helpful in designing and improving MOFs for real-world applications where humidity is often present. |
|---|---|
| AbstractList | Combination of
in situ
IR spectroscopy and
ab initio
calculations reveals the detailed exchange process of H
2
O and NO in Ni-MOF-74 and uncovers its unusual energetics and kinetics caused by H-bonding interaction. Molecular exchange is a common step occurring in many technological processes such as competitive adsorption, chemical separation, capture, delivery, and release. However, the underlying principle is not fully understood, especially in nanoconfined environments where the energetics and kinetics of such processes can deviate from that on flat surfaces. In this paper, we unravel the mechanism of a molecular exchange process by studying the displacement of NO by H 2 O in Ni-MOF-74 in real-time using in situ infrared spectroscopy combined with ab initio calculations. We show that weakly bound H 2 O gradually displaces strongly bound NO on the metal sites by first weakening the M–N bond through forming H-bond and then moving the NO away so that it eventually desorbs. Interestingly, we further find that additional water facilitates this exchange by significantly lowering the kinetic barrier associated with this process as well as the overall energy of the final state. Although our study focuses on Ni-MOF-74, we believe that our finding and explanation of unexpected exchange phenomena—where strongly adsorbed molecules are apparently easily displaced by much weaker bound H 2 O—is applicable to a much larger group of frameworks and will be helpful in designing and improving MOFs for real-world applications where humidity is often present. |
| Author | Li, Jing Pandey, Haardik Tan, Kui Alfaro, Monica Vasquez Thonhauser, Timo Wang, Hao |
| Author_xml | – sequence: 1 givenname: Haardik orcidid: 0000-0002-3082-7784 surname: Pandey fullname: Pandey, Haardik organization: Department of Physics and Center for Functional Materials, Wake Forest University, Winston-Salem, NC 27109, USA – sequence: 2 givenname: Hao surname: Wang fullname: Wang, Hao organization: Department of Chemistry and Chemical Biology, Rutgers University, Piscataway, NJ 08854, USA – sequence: 3 givenname: Monica Vasquez surname: Alfaro fullname: Alfaro, Monica Vasquez organization: Department of Materials Science & Engineering, University of Texas at Dallas, Richardson, Texas 75080, USA – sequence: 4 givenname: Jing orcidid: 0000-0001-7792-4322 surname: Li fullname: Li, Jing organization: Department of Chemistry and Chemical Biology, Rutgers University, Piscataway, NJ 08854, USA – sequence: 5 givenname: Timo orcidid: 0000-0003-4771-7511 surname: Thonhauser fullname: Thonhauser, Timo organization: Department of Physics and Center for Functional Materials, Wake Forest University, Winston-Salem, NC 27109, USA – sequence: 6 givenname: Kui orcidid: 0000-0002-5167-7295 surname: Tan fullname: Tan, Kui organization: Department of Chemistry, University of North Texas, Denton, TX 76203, USA |
| BackLink | https://www.osti.gov/biblio/2282206$$D View this record in Osti.gov |
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| Snippet | Molecular exchange is a common step occurring in many technological processes such as competitive adsorption, chemical separation, capture, delivery, and... Combination of in situ IR spectroscopy and ab initio calculations reveals the detailed exchange process of H 2 O and NO in Ni-MOF-74 and uncovers its unusual... |
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| Title | Real-time observation of the exchange process between H 2 O and NO in the metal–organic framework Ni-MOF-74 |
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