Dynamic Spacer Installation of Multifunctionalities into Metal-Organic Frameworks for Spontaneous One-Step Ethylene Purification from a Ternary C_(2)-Hydrocarbons Mixture  

作　　者：Yang-Yang Xiong Cheng-Xia Chen Tony Pham Zhang-Wen Wei Katherine A.Forrest Mei Pan Cheng-Yong Su 

机构地区：[1]MOE Laboratory of Bioinorganic and Synthetic Chemistry,Lehn Institute of Functional Materials,School of Chemistry,Sun Yat-sen University,Guangzhou 510275 [2]Department of Chemistry,University of South Florida,Tampa,Florida 33620

出　　处：《CCS Chemistry》2024年第1期241-254,共14页中国化学会会刊（英文）

基　　金：supported by the NKRD Program of China(grant no.2021YFA1500401);NSFC Projects(grant nos.21890380,21821003,22001271,22090061,and 21801252);the LIRT Project of Guangdong PRTP(grant no.2017BT01C161);FRF for the Central Universities(grant no.20lgpy79).

摘　　要：Simultaneous ethane and acetylene removal from a C_(2)-gases mixture(C_(2)H_(6),C_(2)H_(4),and C_(2)H_(2))through a one-step separation process for ethylene purification is of great importance yet challenging in petrochemical industry,owing to their similar molecule sizes and physical properties.Herein,a series of multifunctionalized metal–organic frameworks(MOFs),LIFM-XYY-1∼8(LIFM stands for Lehn Institute of Functional Materials,and XYY are the initials of the first author),are constructed via a dynamic spacer installation(DSI)approach to optimize the pore-nanospaces for efficient C_(2)H_(4) isolation from the ternary C_(2)-gases mixture.Installation of variable organic-spacers into the prototypical MOFs,LIFM-28 or PCN-700,results in dramatically improved pore volume/surface area,contracted pore size,and functionalized pore surface,which in turn bring out high C_(2)-gases uptake capacities,enhanced C_(2)H_(6) and C_(2)H_(2) adsorption selectivities over C_(2)H_(4),and fast adsorption kinetics,providing an effective strategy to achieve delicate trade-off among these indexes for adequate separation performance.Specifically,optimized LIFM-XYY-7 presents four-times C_(2)H_(6) and C_(2)H_(2) adsorption capacities than proto-PCN-700.Dynamic breakthrough experiments reveal that poly-grade C_(2)H_(4)(>99.9%)can be obtained from binary or ternary C_(2)-hydrocarbon mixtures through a single separation process.Combined with themolecular simulations,this work demonstrates a promising protocol of porenanospace engineering via multi-functional optimization by the DSI approach to screen out MOFs for a formidable task.

关 键 词：metal-organic frameworks dynamic spacer installation C_(2)H_(6)/C_(2)H_(2)/C_(2)H_(4)gases separation pore nanospace engineering multi-functional optimization 

分 类 号：O64[理学—物理化学]