Controlled Construction of Cu(I) Sites within Confined Spaces via Host-Guest Redox: Highly Efficient Adsorbents for Selective CO Adsorption.

Autor: Li YX; State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering , Nanjing Tech University , Nanjing 210009 , China., Ji YN; State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering , Nanjing Tech University , Nanjing 210009 , China., Jin MM; State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering , Nanjing Tech University , Nanjing 210009 , China., Qi SC; State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering , Nanjing Tech University , Nanjing 210009 , China., Li SS; State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering , Nanjing Tech University , Nanjing 210009 , China., Xue DM; State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering , Nanjing Tech University , Nanjing 210009 , China., Yue MB; School of Chemistry and Chemical Engineering , Qufu Normal University , Shandong 273165 , China., Liu XQ; State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering , Nanjing Tech University , Nanjing 210009 , China., Sun LB; State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering , Nanjing Tech University , Nanjing 210009 , China.
Jazyk: angličtina
Zdroj: ACS applied materials & interfaces [ACS Appl Mater Interfaces] 2018 Nov 21; Vol. 10 (46), pp. 40044-40053. Date of Electronic Publication: 2018 Nov 12.
DOI: 10.1021/acsami.8b15913
Abstrakt: Here, we designed a double-solvent/host-guest redox combined strategy to construct Cu + sites in metal-organic frameworks (MOFs) for the first time. As a proof of concept, a representative MOF MIL-100(Fe) with tunable valence states of cations was employed as the host. The combined strategy realizes selective introduction of Cu 2+ precursors to the interior pores of MIL-100(Fe), remarkably minimizing the aggregation of Cu 2+ and subsequently formed Cu + species. Owing to the proper reducibility of in situ formed Fe 2+ in the frameworks, controlled conversation of Cu 2+ to Cu + with ∼100% yield is achieved in the absence of any additional reducing agents. These characteristics make the obtained materials Cu + -modified MIL-100(Fe) highly active in selective CO adsorption. The CO adsorption capacity is up to 3.75 mmol·g -1 at 298 K and 1 bar, which is superior to all other Cu + -containing adsorbents reported so far such as CuCl/activated carbon (2.5 mmol·g -1 ), CuCl/γ-Al 2 O 3 (1.0 mmol·g -1 ), and CuCl/SBA-15 (0.50 mmol·g -1 ). The same adsorbent also exhibits quite high selectivity of CO over N 2 , and the ideal adsorption solution theory selectivity reaches 424. The outstanding CO adsorption performance make the present adsorbents great potential in separation of CO from various mixtures.
Databáze: MEDLINE