With the increasing demand for synthetic rubber,the purification of 1,3-butadiene(C_(4)H_(6))is of great industrial significance.Herein,the successful removal of n-butene(n-C_(4)H_(8))and iso-butene(iso-C_(4)H_(8))fro...With the increasing demand for synthetic rubber,the purification of 1,3-butadiene(C_(4)H_(6))is of great industrial significance.Herein,the successful removal of n-butene(n-C_(4)H_(8))and iso-butene(iso-C_(4)H_(8))from 1,3-butadiene(C_(4)H_(6))was realized by synthesizing a novel TaOF_(5)^(2-) anion-pillared ultramicroporous material TaOFFIVE-3-Ni(also referred to as ZU-96,TaOFFIVE=TaOF_(5)^(2-),3=pyrazine).Single-component adsorption isotherms show that TaOFFIVE-3-Ni can achieve the exclusion of n-C_(4)H_(8) and iso-C_(4)H_(8) in the low pressure region(0–30 kPa),and uptake C_(4)H_(6) with a high capacity of 92.78 cm^(3)·cm^(-3)(298 K and 100 kPa).The uptake ratio of C_(4)H_(6)/iso-C_(4)H_(8) on TaOFFIVE-3-Ni was 20.83(298 K and 100 kPa),which was the highest among the state-of-the-art adsorbents reported so far.With the rotation of anion and pyrazine ring,the pore size changes continuously,which makes smaller-size C_(4)H_(6) enter the channel while larger-size n-C_(4)H_(8) and iso-C_(4)H_(8) are completely blocked.The excellent breakthrough performance of TaOFFIVE-3-Ni shows great potential in industrial separation of C4 olefins.The specific adsorption binding sites within ZU-96 was further revealed through the modeling calculation.展开更多
基金supported by Natural Science Foundation of Zhejiang Province(LR20B060001 and LZ18B060001)the National Natural Science Foundation of China(21725603,21938011),the Entrepreneur Team Introduction Program of Zhejiang(2019R01006)the Research Computing Center in College of Chemical and Biological Engineering at Zhejiang University.
文摘With the increasing demand for synthetic rubber,the purification of 1,3-butadiene(C_(4)H_(6))is of great industrial significance.Herein,the successful removal of n-butene(n-C_(4)H_(8))and iso-butene(iso-C_(4)H_(8))from 1,3-butadiene(C_(4)H_(6))was realized by synthesizing a novel TaOF_(5)^(2-) anion-pillared ultramicroporous material TaOFFIVE-3-Ni(also referred to as ZU-96,TaOFFIVE=TaOF_(5)^(2-),3=pyrazine).Single-component adsorption isotherms show that TaOFFIVE-3-Ni can achieve the exclusion of n-C_(4)H_(8) and iso-C_(4)H_(8) in the low pressure region(0–30 kPa),and uptake C_(4)H_(6) with a high capacity of 92.78 cm^(3)·cm^(-3)(298 K and 100 kPa).The uptake ratio of C_(4)H_(6)/iso-C_(4)H_(8) on TaOFFIVE-3-Ni was 20.83(298 K and 100 kPa),which was the highest among the state-of-the-art adsorbents reported so far.With the rotation of anion and pyrazine ring,the pore size changes continuously,which makes smaller-size C_(4)H_(6) enter the channel while larger-size n-C_(4)H_(8) and iso-C_(4)H_(8) are completely blocked.The excellent breakthrough performance of TaOFFIVE-3-Ni shows great potential in industrial separation of C4 olefins.The specific adsorption binding sites within ZU-96 was further revealed through the modeling calculation.
