A square lattice topology coordination network that exhibits highly selective C2H2/CO2 separation performance

C2H2/CO2 separation is an industrially important process that remains challenging because of the similar physicochemical properties of C2H2 and CO2. We herein report that the new square lattice (sql) coordination network [Cu(bipy‐xylene)2(NO3)2]n, sql‐16‐Cu‐NO3, 16 = bipy‐xylene = 4,4′‐(2,5‐dimethyl...

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Vydáno v:SmartMat (Beijing, China) Ročník 1; číslo 1
Hlavní autoři: Kumar, Naveen, Mukherjee, Soumya, Bezrukov, Andrey A., Vandichel, Matthias, Shivanna, Mohana, Sensharma, Debobroto, Bajpai, Alankriti, Gascón, Victoria, Otake, Ken‐ichi, Kitagawa, Susumu, Zaworotko, Michael J.
Médium: Journal Article
Jazyk:angličtina
Vydáno: Hoboken John Wiley & Sons, Inc 01.12.2020
Wiley
Témata:
acetylene
Adsorption
Binding sites
Carbon dioxide
Coordination
coordination networks
crystal engineering
Ligands
Network topologies
Pore size
Query languages
Selectivity
Separation
Single crystals
Sorbents
Topology
ultramicroporosity
Xylene
ISSN:2688-819X, 2688-819X
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Shrnutí:C2H2/CO2 separation is an industrially important process that remains challenging because of the similar physicochemical properties of C2H2 and CO2. We herein report that the new square lattice (sql) coordination network [Cu(bipy‐xylene)2(NO3)2]n, sql‐16‐Cu‐NO3, 16 = bipy‐xylene = 4,4′‐(2,5‐dimethyl‐1,4‐phenylene)dipyridine, exists in at least three forms, as‐synthesised (α), activated (α′) and hydrated (β). The activated phase, sql‐16‐Cu‐NO3‐α′, is an ultramicroporous material that exhibits high selectivity towards C2H2 over CO2 as revealed by dynamic gas breakthrough experiments (1:1, C2H2/CO2) that afforded 99.87% pure CO2 in the effluent stream. The separation selectivity at 298 K and 1 bar, 78, is the third best value yet reported for C2H2 selective physisorbents whereas the mid‐loading performance sets a new benchmark. The performance of sql‐16‐Cu‐NO3‐α′ is attributed to a new type of C2H2 binding site in which CH···ONO2 interactions enable moderately strong sorbent‐sorbate binding (Qst (C2H2) = 38.6 kJ/mol) at low loading. Conversely, weak CO2 binding (Qst (CO2) = 25.6 kJ/mol) at low loading means that (ΔQst)AC [Qst (C2H2)–Qst (CO2)] is 13 kJ/mol at low coverage and 11.4 kJ/mol at mid‐loading. Analysis of in situ powder X‐ray diffraction and modelling experiments provide insight into the sorption properties and high C2H2/CO2 separation performance of sql‐16‐Cu‐NO3‐α′. Crystal engineering of square lattice (sql) coordination networks has resulted in a new layered ultramicroporous adsorbent, sql‐16‐Cu‐NO3‐α′. Thanks to its poor affinity to CO2 and optimal C2H2 binding, sql‐16‐Cu‐NO3‐α′ exhibits the rare combination of (a) high C2H2versus CO2 separation selectivity and (b) a new benchmark difference between the C2H2 and CO2 adsorption enthalpies.
Bibliografie:Naveen Kumar and Soumya Mukherjee contributed equally to this study.
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ISSN:2688-819X
2688-819X
DOI:10.1002/smm2.1008