To enhance the separation selectivity of Mg-MOF-74 towards CO_(2) in a CO_(2)/N_(2) mixture,a series of Mg-MOF-74 and Ni_(x)/Mg_(1-x)-MOF-74 adsorbents were prepared by solvothermal synthesis in this paper.It was foun...To enhance the separation selectivity of Mg-MOF-74 towards CO_(2) in a CO_(2)/N_(2) mixture,a series of Mg-MOF-74 and Ni_(x)/Mg_(1-x)-MOF-74 adsorbents were prepared by solvothermal synthesis in this paper.It was found that the adsorption capacity of Mg-MOF-74 for CO_(2) could be effectively increased by optimizing the amount of acetic acid.On this basis,the bimetal MOF-74 adsorbent was prepared by metal modification.The multi-component dynamic adsorption penetration analysis was utilized to examine the CO_(2) adsorption capacity and CO_(2)/N_(2) selectivity of the diverse adsorbent materials.The results showed that Ni0.11/Mg0.89-MOF-74 showed a CO_(2) adsorption capacity of 7.02 mmol/g under pure CO_(2) atmosphere and had a selectivity of 20.50 for CO_(2)/N_(2) under 15% CO_(2)/85%N_(2) conditions,which was 10.2% and 18.02% higher than that of Mg-MOF-74 respectively.Combining XPS,SEM and N_(2) adsorption-desorption characterization analysis,it was attributed to the effect of the more stable unsaturated metal sites Ni into the Mg-MOF-74 on the pore structure and the synergistic interaction between the two metals.Density Functional Theory(DFT)simulations revealed that the synergistic interaction between modulated the electrostatic potential strength and gradient of the material,which was more favorable for the adsorption of CO_(2) molecules with small diameters and large quadrupole moment.In addition,the Ni0.11/Mg0.89-MOF-74 showed commendable cyclic stability,underscoring its promising potential for practical applications.展开更多
Ammonia is one of the most important chemical raw materials in both manufacture and life of human.Traditionally Haber-Bosch method for ammonia synthesis involves high temperature and high pressure conditions,leading t...Ammonia is one of the most important chemical raw materials in both manufacture and life of human.Traditionally Haber-Bosch method for ammonia synthesis involves high temperature and high pressure conditions,leading to significant energy consumption and environmental pollution.Non-thermal plasma(NTP) is a promising alternative approach to ammonia synthesis at low temperature and atmospheric pressure.In this study,the synergistic effect of nanosecond pulsed dielectric barrier discharge(np-DBD) and Ni-MOF-74 catalyst was investigated in ammonia synthesis by utilizing nitrogen and hydrogen as feedstock.The results demonstrated that the plasma catalytic-synthesis process parameters play a crucial role in the synthesis process of ammonia.The highest ammonia synthesis rate of 5145.16 μmol·g^(-1)·h^(-1)with an energy efficiency of 1.27 g·kWh^(-1)was observed in the presence of the Ni-MOF-74 catalyst,which was3.7 times higher than that without Ni-MOF-74 catalyst.The synergistic effect of Ni-MOF-74catalyst and nanosecond pulsed plasma was explored by in-situ plasma discharge diagnostics.展开更多
基金supported by National Natural Science Foundation of China(U23A20100)the Strategic Priority Research Program(A)of the Chinese Academy of Sciences(XDA0390404)+5 种基金ICC CAS SCJC-DT-2023-03,the Foundation of State Key Laboratory of Coal Conversion(J24-25-619)Youth Innovation Promotion Association CAS(2018209,2020179)Key R&D Program of Shanxi Province(202102090301008,202202090301013)the special fund for S&T Innovation Team of Shanxi Province(202204051001012)Project of International Cooperation and Exchange NSFC-RFBR(22011530069)Tianjin Science and Technology Plan Project(22YFYSHZ00290)。
文摘To enhance the separation selectivity of Mg-MOF-74 towards CO_(2) in a CO_(2)/N_(2) mixture,a series of Mg-MOF-74 and Ni_(x)/Mg_(1-x)-MOF-74 adsorbents were prepared by solvothermal synthesis in this paper.It was found that the adsorption capacity of Mg-MOF-74 for CO_(2) could be effectively increased by optimizing the amount of acetic acid.On this basis,the bimetal MOF-74 adsorbent was prepared by metal modification.The multi-component dynamic adsorption penetration analysis was utilized to examine the CO_(2) adsorption capacity and CO_(2)/N_(2) selectivity of the diverse adsorbent materials.The results showed that Ni0.11/Mg0.89-MOF-74 showed a CO_(2) adsorption capacity of 7.02 mmol/g under pure CO_(2) atmosphere and had a selectivity of 20.50 for CO_(2)/N_(2) under 15% CO_(2)/85%N_(2) conditions,which was 10.2% and 18.02% higher than that of Mg-MOF-74 respectively.Combining XPS,SEM and N_(2) adsorption-desorption characterization analysis,it was attributed to the effect of the more stable unsaturated metal sites Ni into the Mg-MOF-74 on the pore structure and the synergistic interaction between the two metals.Density Functional Theory(DFT)simulations revealed that the synergistic interaction between modulated the electrostatic potential strength and gradient of the material,which was more favorable for the adsorption of CO_(2) molecules with small diameters and large quadrupole moment.In addition,the Ni0.11/Mg0.89-MOF-74 showed commendable cyclic stability,underscoring its promising potential for practical applications.
基金the financial support from the Beijing Municipal Natural Science Foundation (No. 1242015)National Undergraduate Innovation and Entrepreneurship Training Program of China (No. 202310015019)Discipline Construction of Material Science and Engineering(Nos. 21090122014 and 21090123007)。
文摘Ammonia is one of the most important chemical raw materials in both manufacture and life of human.Traditionally Haber-Bosch method for ammonia synthesis involves high temperature and high pressure conditions,leading to significant energy consumption and environmental pollution.Non-thermal plasma(NTP) is a promising alternative approach to ammonia synthesis at low temperature and atmospheric pressure.In this study,the synergistic effect of nanosecond pulsed dielectric barrier discharge(np-DBD) and Ni-MOF-74 catalyst was investigated in ammonia synthesis by utilizing nitrogen and hydrogen as feedstock.The results demonstrated that the plasma catalytic-synthesis process parameters play a crucial role in the synthesis process of ammonia.The highest ammonia synthesis rate of 5145.16 μmol·g^(-1)·h^(-1)with an energy efficiency of 1.27 g·kWh^(-1)was observed in the presence of the Ni-MOF-74 catalyst,which was3.7 times higher than that without Ni-MOF-74 catalyst.The synergistic effect of Ni-MOF-74catalyst and nanosecond pulsed plasma was explored by in-situ plasma discharge diagnostics.
