采用L-精氨酸对传统均苯三甲酸(BTC)溶剂热法合成的Cu基金属有机骨架化合物(Cu-BTC)进行改性,得到新型化合物(Cu-BTC-Arg),并通过固定床动态吸附实验考察了Cu-BTC-Arg和Cu-BTC吸附CO_2的性能。表征结果显示:L-精氨酸只是辅助化溶剂,并...采用L-精氨酸对传统均苯三甲酸(BTC)溶剂热法合成的Cu基金属有机骨架化合物(Cu-BTC)进行改性,得到新型化合物(Cu-BTC-Arg),并通过固定床动态吸附实验考察了Cu-BTC-Arg和Cu-BTC吸附CO_2的性能。表征结果显示:L-精氨酸只是辅助化溶剂,并未配位至Cu^(2+)上;Cu-BTC-Arg比Cu-BTC具有更小的晶粒尺寸、更大的比表面积和微孔体积。实验结果表明,两种不同L-精氨酸加入量合成的Cu-BTC-Arg均在室温、烟气中无水蒸气、烟气流量80 m L/min的条件下CO_2吸附量最大,吸附接近饱和时的CO_2吸附量均为4.9 mmol/g,远高于Cu-BTC的CO_2吸附量。Cu-BTC-Arg对CO_2的吸附以物理吸附为主。展开更多
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
文摘采用L-精氨酸对传统均苯三甲酸(BTC)溶剂热法合成的Cu基金属有机骨架化合物(Cu-BTC)进行改性,得到新型化合物(Cu-BTC-Arg),并通过固定床动态吸附实验考察了Cu-BTC-Arg和Cu-BTC吸附CO_2的性能。表征结果显示:L-精氨酸只是辅助化溶剂,并未配位至Cu^(2+)上;Cu-BTC-Arg比Cu-BTC具有更小的晶粒尺寸、更大的比表面积和微孔体积。实验结果表明,两种不同L-精氨酸加入量合成的Cu-BTC-Arg均在室温、烟气中无水蒸气、烟气流量80 m L/min的条件下CO_2吸附量最大,吸附接近饱和时的CO_2吸附量均为4.9 mmol/g,远高于Cu-BTC的CO_2吸附量。Cu-BTC-Arg对CO_2的吸附以物理吸附为主。
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.
