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作 者:Diyi Fang Chuanlei Liu Yu Chen Qilong Peng Kongguo Wu Yuxiang Chen Hao Jiang Yuan Wu Benxian Shen Qiumin Wu Di Wu Hui Sun
机构地区:[1]International Joint Research Center of Green Energy Chemical Engineering,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China [2]Alexandra Navrotsky Institute for Experimental Thermodynamics,The Gene and Linda Voiland School of Chemical Engineering and Bioengineering,Materials Science and Engineering,and Department of Chemistry,Washington State University,Washington 99163,USA
出 处:《Nano Research》2024年第1期344-353,共10页纳米研究(英文版)
基 金:supported by the National Natural Science Foundation of China(Nos.22178109 and 21878097);the Natural Science Foundation of Shanghai(No.21ZR1417700)。
摘 要:Porous heterogeneous lyophobic systems(HLSs)find potential applications in energy restoring,dissipating,and absorbing.However,the development of controllable HLSs still lacks rational structure design of nanoporous materials matching the molecular sizes of adopted liquids.Besides that,thoroughly understanding the underlying transportation mechanism in the confined nano channels is greatly challenging.In this work,a series of Co/Zn bimetallic zeolitic imidazolate frameworks(ZIFs)with tunable structures were synthesized via regulating the Co to Zn ratios and employed to investigate the intrusion–extrusion of liquid water in confined nanopores.Structural characterizations confirm the heterometallic coordination in the Co/Zn-doped frameworks.Water intrusion–extrusion experiments unlock the relationship between the intrusion pressure and the nanopore size and realize the evolution of the HLSs between molecular spring and shock-absorber.In addition,cycling tests indicate the reversible structure change of Co/Zn ZIFs encountering pressure-induced water intrusion.In combination with molecular dynamics simulations,we present that the water multimers intrude into nanopores of ZIFs in chain-like forms along with dissociation of hydrogen bonds(HBs).Water molecules in the pre-intrusion state exhibit reduced HBs in response to the increase of pressure and linear structure with 1.6–3.0 HBs on average.After transition to the post-intrusion situation,the associative configuration of water tends to exhibit the tetrahedral structure.Herein,we highlight the roles of pore size and HB in synergically dominating the pressure-induced intrusion–extrusion of liquid water in hydrophobic nanopores.Furthermore,the present work can also guide the development of functional guest–host systems based on porous architectures.
关 键 词:HETEROMETALLIC zeolitic imidazolate frameworks NANOPORE intrusion hydrogen bonds
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