Safely and highly selective acetylene(C_(2)H_(2))capture is a great challenge,because of its highly explosive nature,as well as its nearly similar molecule size and boiling point toward the main impurity of carbon dio...Safely and highly selective acetylene(C_(2)H_(2))capture is a great challenge,because of its highly explosive nature,as well as its nearly similar molecule size and boiling point toward the main impurity of carbon dioxide(CO_(2)).Adsorption separation has shown a promising future.Herein,a new nanoporous coordination polymer(PCP)adsorbent with fixed and free Cu ions(termed NTU-66-Cu)was prepared through post-synthetic approach via cation exchanging from the pristine NTU-66,an anionic framework with new 3,4,6-c topology and two kinds of cages.The NTU-66-Cu shows significantly improved C_(2)H_(2)/CO_(2)selectivity from 6 to 32(v/v:1/1)or 4 to 4_(2)(v/v:1/4)at low pressure under 298 K,along with enhanced C_(2)H_(2)capacity(from 89.22to 111.53 cm^(3)·g^(-1)).More importantly,this observation was further validated by density functional theory(DFT)calculations and breakthrough experiments under continuous and dynamic conditions.Further,the excellent chemical stability enables this adsorbent to achieve recycle C_(2)H_(2)/CO_(2)separation without loss of C_(2)H_(2)capacity.展开更多
基金the National Natural Science Foundation of China(No.21671102,21973029)the Innovative Research Team Program by the Ministry of Education of China(No.IRT-17R54)+2 种基金the Hunan Provincial Natural Science Foundation of China(No.2020JJ4290)the Young and Middle-aged Academic Leader of Jiangsu Provincial Blue Project,the Six Talent Peaks Project in Jiangsu Province(No.JY-030)the State Key Laboratory of Materials-Oriented Chemical Engineering(No.ZK201803).We also thank Prof.M.O’Keeffe and Prof.M.Li for valuable suggestion on topology analysis.
文摘Safely and highly selective acetylene(C_(2)H_(2))capture is a great challenge,because of its highly explosive nature,as well as its nearly similar molecule size and boiling point toward the main impurity of carbon dioxide(CO_(2)).Adsorption separation has shown a promising future.Herein,a new nanoporous coordination polymer(PCP)adsorbent with fixed and free Cu ions(termed NTU-66-Cu)was prepared through post-synthetic approach via cation exchanging from the pristine NTU-66,an anionic framework with new 3,4,6-c topology and two kinds of cages.The NTU-66-Cu shows significantly improved C_(2)H_(2)/CO_(2)selectivity from 6 to 32(v/v:1/1)or 4 to 4_(2)(v/v:1/4)at low pressure under 298 K,along with enhanced C_(2)H_(2)capacity(from 89.22to 111.53 cm^(3)·g^(-1)).More importantly,this observation was further validated by density functional theory(DFT)calculations and breakthrough experiments under continuous and dynamic conditions.Further,the excellent chemical stability enables this adsorbent to achieve recycle C_(2)H_(2)/CO_(2)separation without loss of C_(2)H_(2)capacity.
