Nano structure including pore structure and amine assembly is critical for improving sorption and desorption kinetics for adsorptive CO_(2) separation.The present work delineates(1)the influence of the nano-scale pore...Nano structure including pore structure and amine assembly is critical for improving sorption and desorption kinetics for adsorptive CO_(2) separation.The present work delineates(1)the influence of the nano-scale pore structure of amine-functionalized solid sorbents,and(2)effect of changing the assembly of amine molecules on surface of nano-porous SiO_(2) on the rates of adsorption and desorption of CO_(2).50PEI-MSN sorbent with inverted cone-shaped pores was prepared by using mesoporous silica nanospheres(MSN)with inverted cone-shaped pores for the loading of polyethyleneimine(PEI).Co-structure-directing(CSD)method was used to synthesize the sorbent with arranged amine assembly at nano-scale(2N-CSD).By comparison with 50PE卜SBA15 as a benchmark sorbent,both sorbents have improved sorption and desorption kinetics.There are significant effects of nano pore structure and amine assembly on the sorption and desorption kinetics.The inverted cone-shaped pores in MSN allow loading polymeric amines in their narrower ends and leaving larger pore mouths open for the transport of CO_(2);50PEI-MSN shows a maximum sorption rate of 81.4 mg·g^(-1)·min^(-1) with average sorption rate of 25.4mg·g^(-1)·min^(-1) at 80℃ which are 34%and 59%higher than the corresponding values for 50PEI-SBA15;a maximum desorption rate of 38.4mg·g^(-1)·min^(-1) with average desorption rate of 11.8 mg·g^(-1)·min^(-1) ramping from 30 to 95℃ which are 37%and 156%higher than the corresponding values for 50PEI-SBA15.The arranged monolayer-like amine assembly on surface of nanoporous SiO_(2) likely provides high amine sorption sites through improved accessibility of amine,and 2N-CSD shows a maximum sorption rate of 60.5 mg·g^(-1)·min^(-1),with average sorption rate of 12.8mg·g^(-1)·min^(-1) at 300C which are 108%and 205%higher than the corresponding values for 50PEI-SBA15;a lower maximum desorption rate of 9.7 mg g'1min"1 and average desorption rate of 9.8mg·g^(-1)·min^(-1) ramping from 30 to 95℃ which is 250%higher than the correspondi展开更多
3-Aminopropyltriethoxysilane functionalized worm-like mesoporous silica monolithic（WMSM-NH2） was prepared and used as a new regenerable adsorbent for the removal of Cu2＋ ions. The analysis results show that the WMS...3-Aminopropyltriethoxysilane functionalized worm-like mesoporous silica monolithic（WMSM-NH2） was prepared and used as a new regenerable adsorbent for the removal of Cu2＋ ions. The analysis results show that the WMSM-NH2 monolithic had a high efficiency value of 99.3% for Cu2＋ remediation when the Cu2＋ solution was at an initial concentration of 10.32 mg/L. The regeneration study of the WMSM-NH2 monolithic presented that the adsorp- tion efficiency of 89.0% was remained and a mass of 92.0% was left after seven adsorption-desorption cycles were executed. The monolithic material with high resistance to the acid and good mechanical stability can facilitate the operations of adsorption and regeneration of the adsorbent.展开更多
Palladium nanoparticles were deposited on the amine-grafted glass fiber mat （GFM-NH2） catalyst support by a conventional impregnation process followed by the borohydride reduction in aqueous solution at room tempera...Palladium nanoparticles were deposited on the amine-grafted glass fiber mat （GFM-NH2） catalyst support by a conventional impregnation process followed by the borohydride reduction in aqueous solution at room temperature to create the designed Pd/GFM-NH2 catalyst. By the use of large size glass fiber mat without nano/mesopores as the catalyst support, the internal mass transfer limitations due to the existence of nano/mesopores on the catalyst support were eliminated and the Pd/GFM-NH2 catalyst could be easily separated from treated water due to the large size of the catalyst support. Batch experiments demonstrate its good catalytic reduction performance of Cr（VI） with formic acid as the reducing agent. It also demonstrated an efficient Cr（VI） removal and stability in a lab-prepared, packed fixed-bed tube reactor for the continuous treatment of Cr（VI）-containing water. Thus, it has a good potential for the catalytic reduction of Cr（VI） in the water treatment practice.展开更多
以二乙烯三胺基丙基三甲氧基硅烷为偶联剂,采用后期修饰方法,制备出氨基修饰SBA-15(SBA代表University of California,Santa Barbara,USA)。利用扫描电镜、傅立叶红外光谱仪、N2吸附-脱附对其结构进行表征。以修饰后的SBA-15为吸附剂,...以二乙烯三胺基丙基三甲氧基硅烷为偶联剂,采用后期修饰方法,制备出氨基修饰SBA-15(SBA代表University of California,Santa Barbara,USA)。利用扫描电镜、傅立叶红外光谱仪、N2吸附-脱附对其结构进行表征。以修饰后的SBA-15为吸附剂,对水中Cu2+的吸附过程进行了动力学与热力学探讨。结果表明:修饰后的SBA-15是一种理想的铜吸附剂,pH值适应范围较宽(3~6),吸附平衡时间较短(120 min),最大吸附量可达37.94 mg/g。修饰后SBA-15对Cu2+吸附动力学符合拟二阶动力学方程,吸附过程可分为三个阶段且不只受内扩散控制。Langmuir吸附模型和Dubinin-Radushkevich(D-R)吸附模型能更好地描述了Cu2+在修饰后SBA-15上的吸附行为,其吸附平均活化能E值分别为-16.44,-17.05,-17.20 kJ/mol,表明该吸附过程为表面络合。热力学参数表明吸附过程是自发、吸热、混乱度增加的过程,升温有利于吸附。展开更多
基金financially supported by the National Key Research and Development Program of China(No.2016YFB0600902-4)the Fundamental Research Funds for the Central Universities(No.DUT20RC(5)002)the CUHK Research Startup Fund(No.#4930981).
文摘Nano structure including pore structure and amine assembly is critical for improving sorption and desorption kinetics for adsorptive CO_(2) separation.The present work delineates(1)the influence of the nano-scale pore structure of amine-functionalized solid sorbents,and(2)effect of changing the assembly of amine molecules on surface of nano-porous SiO_(2) on the rates of adsorption and desorption of CO_(2).50PEI-MSN sorbent with inverted cone-shaped pores was prepared by using mesoporous silica nanospheres(MSN)with inverted cone-shaped pores for the loading of polyethyleneimine(PEI).Co-structure-directing(CSD)method was used to synthesize the sorbent with arranged amine assembly at nano-scale(2N-CSD).By comparison with 50PE卜SBA15 as a benchmark sorbent,both sorbents have improved sorption and desorption kinetics.There are significant effects of nano pore structure and amine assembly on the sorption and desorption kinetics.The inverted cone-shaped pores in MSN allow loading polymeric amines in their narrower ends and leaving larger pore mouths open for the transport of CO_(2);50PEI-MSN shows a maximum sorption rate of 81.4 mg·g^(-1)·min^(-1) with average sorption rate of 25.4mg·g^(-1)·min^(-1) at 80℃ which are 34%and 59%higher than the corresponding values for 50PEI-SBA15;a maximum desorption rate of 38.4mg·g^(-1)·min^(-1) with average desorption rate of 11.8 mg·g^(-1)·min^(-1) ramping from 30 to 95℃ which are 37%and 156%higher than the corresponding values for 50PEI-SBA15.The arranged monolayer-like amine assembly on surface of nanoporous SiO_(2) likely provides high amine sorption sites through improved accessibility of amine,and 2N-CSD shows a maximum sorption rate of 60.5 mg·g^(-1)·min^(-1),with average sorption rate of 12.8mg·g^(-1)·min^(-1) at 300C which are 108%and 205%higher than the corresponding values for 50PEI-SBA15;a lower maximum desorption rate of 9.7 mg g'1min"1 and average desorption rate of 9.8mg·g^(-1)·min^(-1) ramping from 30 to 95℃ which is 250%higher than the correspondi
基金Supported by the National Natural Science Foundation of China（Nos. 50573030 and 21171065）.
文摘3-Aminopropyltriethoxysilane functionalized worm-like mesoporous silica monolithic（WMSM-NH2） was prepared and used as a new regenerable adsorbent for the removal of Cu2＋ ions. The analysis results show that the WMSM-NH2 monolithic had a high efficiency value of 99.3% for Cu2＋ remediation when the Cu2＋ solution was at an initial concentration of 10.32 mg/L. The regeneration study of the WMSM-NH2 monolithic presented that the adsorp- tion efficiency of 89.0% was remained and a mass of 92.0% was left after seven adsorption-desorption cycles were executed. The monolithic material with high resistance to the acid and good mechanical stability can facilitate the operations of adsorption and regeneration of the adsorbent.
基金supported by the Basic Science Innovation Program of Shenyang National Laboratory for Materials Science(Grant Nos.Y4N56R1161 and Y4N56F2161)the National Natural Science Foundation of China(Grant No.51502305)
文摘Palladium nanoparticles were deposited on the amine-grafted glass fiber mat （GFM-NH2） catalyst support by a conventional impregnation process followed by the borohydride reduction in aqueous solution at room temperature to create the designed Pd/GFM-NH2 catalyst. By the use of large size glass fiber mat without nano/mesopores as the catalyst support, the internal mass transfer limitations due to the existence of nano/mesopores on the catalyst support were eliminated and the Pd/GFM-NH2 catalyst could be easily separated from treated water due to the large size of the catalyst support. Batch experiments demonstrate its good catalytic reduction performance of Cr（VI） with formic acid as the reducing agent. It also demonstrated an efficient Cr（VI） removal and stability in a lab-prepared, packed fixed-bed tube reactor for the continuous treatment of Cr（VI）-containing water. Thus, it has a good potential for the catalytic reduction of Cr（VI） in the water treatment practice.
