The unique adsorption performance of metal-organic frameworks(MOFs) indicates a new direction for gas separation and purification. The low-temperature distillation, as a traditional technique for hydrogen isotope sepa...The unique adsorption performance of metal-organic frameworks(MOFs) indicates a new direction for gas separation and purification. The low-temperature distillation, as a traditional technique for hydrogen isotope separation, is limited as it is a high energy-and cost-intensive process. Instead of utilizing such a conventional separation route, we use ordered microporous frameworks based on a physical adsorption mechanism to solve the challenge of hydrogen isotope separation. Herein we analyze M-MOF-74(M=Co, Ni, Mg, Zn), featuring a hexagonal channel about 11 ? and high density of open metal sites, for their ability to separate and purify deuterium from the hydrogen isotope mixture by dynamic column breakthrough experiments. Our results show that the combination of the strength of binding sites, density of coordinatively unsaturated metal sites and hydrogen isotope adsorption capacity of materials renders Co-MOF-74 as an optimal adsorbent for the capture of deuterium from hydrogen isotope mixtures in a simulated industrial process.展开更多
Hydrogen isotope separation is a challenging task due to their similar properties.Herein,based on the chemical affinity quantum sieve(CAQS)effect,the D_(2)/H_(2)separation performance of M_(2)(m-dobdc)(M=Co,Ni,Mg,Mn;m...Hydrogen isotope separation is a challenging task due to their similar properties.Herein,based on the chemical affinity quantum sieve(CAQS)effect,the D_(2)/H_(2)separation performance of M_(2)(m-dobdc)(M=Co,Ni,Mg,Mn;m-dobdc^(4-)=4,6-dioxido-1,3-benzenedicarboxylate),a series of honeycomb-shaped MOFs with high stability and abundant open metal sites,are studied by gases sorption and breakthrough experiments,in which two critical factors,gas uptake and adsorption enthalpy,are taken into consideration.Among these MOFs,Co_(2)(m-dobdc)exhibits the longest D_(2)retention time of 180 min/g(H_(2)/D_(2)/Ne:1/1/98)at 77 K because of its second-highest adsorption enthalpy(10.7 kJ/mol for H_(2)and 11.8 kJ/mol for D_(2))and the best sorption capacity(5.22 mmol/g for H_(2)and 5.49 mmol/g for D_(2))under low pressure of 1 kPa and 77 K,which make it a promising material for industrial hydrogen isotope separation.Moreover,the results indicate that H_(2)and D_(2)capacities under low pressure(about 1 kPa)dominate the final D_(2)/H_(2)separation property of MOFs.展开更多
基金supported by the National Natural Science Foundation of China (21771177)the Strategic Priority Research Program of Chinese Academy of Sciences (XDB20000000)the Key Research Program of Frontier Sciences, Chinese Academy of Sciences (QYZDB-SSW-SLH019)。
文摘The unique adsorption performance of metal-organic frameworks(MOFs) indicates a new direction for gas separation and purification. The low-temperature distillation, as a traditional technique for hydrogen isotope separation, is limited as it is a high energy-and cost-intensive process. Instead of utilizing such a conventional separation route, we use ordered microporous frameworks based on a physical adsorption mechanism to solve the challenge of hydrogen isotope separation. Herein we analyze M-MOF-74(M=Co, Ni, Mg, Zn), featuring a hexagonal channel about 11 ? and high density of open metal sites, for their ability to separate and purify deuterium from the hydrogen isotope mixture by dynamic column breakthrough experiments. Our results show that the combination of the strength of binding sites, density of coordinatively unsaturated metal sites and hydrogen isotope adsorption capacity of materials renders Co-MOF-74 as an optimal adsorbent for the capture of deuterium from hydrogen isotope mixtures in a simulated industrial process.
基金financially supported by the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB20000000)the Key Research Program of Frontier Sciences,Chinese Academy of Sciences(No.QYZDB-SSW-SLH019)the National Natural Science Foundation of China(Nos.21771177,51603206 and 21203117).
文摘Hydrogen isotope separation is a challenging task due to their similar properties.Herein,based on the chemical affinity quantum sieve(CAQS)effect,the D_(2)/H_(2)separation performance of M_(2)(m-dobdc)(M=Co,Ni,Mg,Mn;m-dobdc^(4-)=4,6-dioxido-1,3-benzenedicarboxylate),a series of honeycomb-shaped MOFs with high stability and abundant open metal sites,are studied by gases sorption and breakthrough experiments,in which two critical factors,gas uptake and adsorption enthalpy,are taken into consideration.Among these MOFs,Co_(2)(m-dobdc)exhibits the longest D_(2)retention time of 180 min/g(H_(2)/D_(2)/Ne:1/1/98)at 77 K because of its second-highest adsorption enthalpy(10.7 kJ/mol for H_(2)and 11.8 kJ/mol for D_(2))and the best sorption capacity(5.22 mmol/g for H_(2)and 5.49 mmol/g for D_(2))under low pressure of 1 kPa and 77 K,which make it a promising material for industrial hydrogen isotope separation.Moreover,the results indicate that H_(2)and D_(2)capacities under low pressure(about 1 kPa)dominate the final D_(2)/H_(2)separation property of MOFs.