Two 1,3-alternate thiacalix[4]arene derivatives bearing amide groups, 1,3-alternate p-tert-butylthiacalix[4]arene tetraamide （4）, and 1,3-alternate p-H-thiacalix[4]arene tetraamide （6） were prepared, and their cry...Two 1,3-alternate thiacalix[4]arene derivatives bearing amide groups, 1,3-alternate p-tert-butylthiacalix[4]arene tetraamide （4）, and 1,3-alternate p-H-thiacalix[4]arene tetraamide （6） were prepared, and their crystal structures were determined by single-crystal X-ray diffraction method. The steric hindrances posed by tert-butyl groups play an important part in the synthesis and the self-assembly of the two compounds. Compound 6 was synthesized from the corresponding ester, which was obtained by the reaction of acid chloride with ammonia. In the crystal structure, compound 4 presents a highly symmetric molecular structure, while for compound 6, because of absence of tert-butyl groups, it presents a more flexible molecular structure.展开更多
Mixed matrix membrane used to selective removal of CO2 was considered as an efficient solution to energy and environmental sustainability. In this study, a MMM that consists of amide functionalized porous coordination...Mixed matrix membrane used to selective removal of CO2 was considered as an efficient solution to energy and environmental sustainability. In this study, a MMM that consists of amide functionalized porous coordination polymer filler（MIL-53-NH2） was successfully prepared, which sharply promotes the CO2/N2 selectivity from 44（neat polymeric membrane） to 75. Remarkably, the positive effect of amide group and nanochannel of MIL-53-NH2 filler was illustrated by decreased selectivity of the MMM with formic acid modified MIL-53-NH2 filler（MIL-53-NHCOH）.展开更多
The safety and performance of lithium-ion batteries(LIBs)largely depend on the structural design and performance characteristics of the separator.Commercial polyolefin separators suffer from problems such as poor ther...The safety and performance of lithium-ion batteries(LIBs)largely depend on the structural design and performance characteristics of the separator.Commercial polyolefin separators suffer from problems such as poor thermal stability,insufficient porosity,and inferior electrolyte wettability,which not only easily lead to battery safety issues but also significantly affect the ionic conductivity and energy density of the batteries.Herein,we have designed a facile,efficient and controllable methodology to develop a high-porosity poly(m-phenylene isophthalamide)(PMIA)separator with both excellent wettability and superior thermal resistance by a vapor-induced phase separation technique.Specifically,the PMIA separator undergoes a thermal shrinkage of less than 1%even after being treated at 200℃ for one hour,which greatly enhances the thermal safety of the battery.In addition,a continuous and interconnected high-porosity structure(porosity of 69%)is formed by utilizing a stable and controllable solvent exchange rate,thereby constructing abundant channels for the transportation of ions within the battery.Moreover,the amide groups in the PMIA molecular structure further confer the separator with excellent wettability,enabling it to possess outstanding electrolyte absorption capacity(electrolyte absorption rate of 270%).As a result,the Li||LFP full cell with PMIA separator exhibits excellent capacity and cycling stability,maintaining a reversible specific capacity of 105.6 mAh g^(-1)after 600 cycles at 5 C.And Li||NCM811 full cell with PMIA separator show no significant degradation(168.1 mAh g^(-1)at 0.5 C)after long-cycle at high temperature.These results indicate the potential of the PMIA separator for high thermal stability and high energy battery,and the scalability of this technology also provides new ideas and directions for the preparation of separators with superior comprehensive performance.展开更多
High and cost-efficient capture of CO_(2) is a prerequisite and an inevitable path of carbon emission reduction. To address the challenges(high cost, low efficiency, less sustainability, etc.) of existing petroleum-ba...High and cost-efficient capture of CO_(2) is a prerequisite and an inevitable path of carbon emission reduction. To address the challenges(high cost, low efficiency, less sustainability, etc.) of existing petroleum-based CO_(2) absorbents, herein, a class of efficient and sustainable lignin-based absorbents were resoundingly prepared by grafting the active amine group on a lignin derived compound vanillin and alkali lignin. The results demonstrated that vanillin modified by acrylamide achieved the excellent absorption capacity among the three absorbents, whose ability was 0.114 g CO_(2) per gram of absorbent under 25 ℃ and 100 kPa. In addition, the absorbent retained stable absorbability of CO_(2) after 6 cycles.The absorbing capacity of the absorbent formed by the coupling of vanillin and acrylamide to CO_(2) was much greater than their own(i.e. 0 g CO_(2) ·g^(-1)vanillin, 0.01 g CO_(2) ·g^(-1) acrylamide, respectively).Detailed information revealed the multi-site synergistic absorption mechanism, in which CO_(2) has C and O double interactions with the amide group of the absorbent, and single interaction with the hydroxyl oxygen on the benzene ring of the absorbent. The absorption capacity of modified lignin for CO_(2) is as high as 0.12 g CO_(2) per gram of absorbent, which is comparable with that of model compound vanillin.This work not only provides a new idea for the design of bio-absorbents for CO_(2) capture, but explores the application potential of lignin-based materials.展开更多
基金Supported by the National Natural Science Foundation of China(20772092)the Hubei Province Natural Science Fund for Distinguished Young Scholars(2007ABB021)
文摘Two 1,3-alternate thiacalix[4]arene derivatives bearing amide groups, 1,3-alternate p-tert-butylthiacalix[4]arene tetraamide （4）, and 1,3-alternate p-H-thiacalix[4]arene tetraamide （6） were prepared, and their crystal structures were determined by single-crystal X-ray diffraction method. The steric hindrances posed by tert-butyl groups play an important part in the synthesis and the self-assembly of the two compounds. Compound 6 was synthesized from the corresponding ester, which was obtained by the reaction of acid chloride with ammonia. In the crystal structure, compound 4 presents a highly symmetric molecular structure, while for compound 6, because of absence of tert-butyl groups, it presents a more flexible molecular structure.
基金financial support of the National Natural Science Foundation of China (No. 21671102)Natural Science Foundation of Jiangsu Province (No. BK20161538)+2 种基金Innovative Research Team Program by the Ministry of Education of China (No. IRT17R54)Six Talent Peaks Project in Jiangsu Province (No. JY-030)State Key Laboratory of Materials-Oriented Chemical Engineering (No. ZK201406)
文摘Mixed matrix membrane used to selective removal of CO2 was considered as an efficient solution to energy and environmental sustainability. In this study, a MMM that consists of amide functionalized porous coordination polymer filler（MIL-53-NH2） was successfully prepared, which sharply promotes the CO2/N2 selectivity from 44（neat polymeric membrane） to 75. Remarkably, the positive effect of amide group and nanochannel of MIL-53-NH2 filler was illustrated by decreased selectivity of the MMM with formic acid modified MIL-53-NH2 filler（MIL-53-NHCOH）.
基金supported by the National Natural Science Foundation of China(52273059,52403046)the Science and Technology Plans of Tianjin(22JCYBJC01030)+1 种基金the Tianjin Research Innovation Project for Postgraduate Students(2022BKY145)partially supported by financial contributions from Yantai Tayho Advanced Materials Co.,Ltd。
文摘The safety and performance of lithium-ion batteries(LIBs)largely depend on the structural design and performance characteristics of the separator.Commercial polyolefin separators suffer from problems such as poor thermal stability,insufficient porosity,and inferior electrolyte wettability,which not only easily lead to battery safety issues but also significantly affect the ionic conductivity and energy density of the batteries.Herein,we have designed a facile,efficient and controllable methodology to develop a high-porosity poly(m-phenylene isophthalamide)(PMIA)separator with both excellent wettability and superior thermal resistance by a vapor-induced phase separation technique.Specifically,the PMIA separator undergoes a thermal shrinkage of less than 1%even after being treated at 200℃ for one hour,which greatly enhances the thermal safety of the battery.In addition,a continuous and interconnected high-porosity structure(porosity of 69%)is formed by utilizing a stable and controllable solvent exchange rate,thereby constructing abundant channels for the transportation of ions within the battery.Moreover,the amide groups in the PMIA molecular structure further confer the separator with excellent wettability,enabling it to possess outstanding electrolyte absorption capacity(electrolyte absorption rate of 270%).As a result,the Li||LFP full cell with PMIA separator exhibits excellent capacity and cycling stability,maintaining a reversible specific capacity of 105.6 mAh g^(-1)after 600 cycles at 5 C.And Li||NCM811 full cell with PMIA separator show no significant degradation(168.1 mAh g^(-1)at 0.5 C)after long-cycle at high temperature.These results indicate the potential of the PMIA separator for high thermal stability and high energy battery,and the scalability of this technology also provides new ideas and directions for the preparation of separators with superior comprehensive performance.
基金supported by National Natural Science Foundation of China (22078023, 22178187)Natural Science Foundation of Shandong Province (ZR202102180830)+1 种基金Taishan Scholars Program of Shandong Province (tsqn201909091)the Startup Foundation of China (3160011181808)。
文摘High and cost-efficient capture of CO_(2) is a prerequisite and an inevitable path of carbon emission reduction. To address the challenges(high cost, low efficiency, less sustainability, etc.) of existing petroleum-based CO_(2) absorbents, herein, a class of efficient and sustainable lignin-based absorbents were resoundingly prepared by grafting the active amine group on a lignin derived compound vanillin and alkali lignin. The results demonstrated that vanillin modified by acrylamide achieved the excellent absorption capacity among the three absorbents, whose ability was 0.114 g CO_(2) per gram of absorbent under 25 ℃ and 100 kPa. In addition, the absorbent retained stable absorbability of CO_(2) after 6 cycles.The absorbing capacity of the absorbent formed by the coupling of vanillin and acrylamide to CO_(2) was much greater than their own(i.e. 0 g CO_(2) ·g^(-1)vanillin, 0.01 g CO_(2) ·g^(-1) acrylamide, respectively).Detailed information revealed the multi-site synergistic absorption mechanism, in which CO_(2) has C and O double interactions with the amide group of the absorbent, and single interaction with the hydroxyl oxygen on the benzene ring of the absorbent. The absorption capacity of modified lignin for CO_(2) is as high as 0.12 g CO_(2) per gram of absorbent, which is comparable with that of model compound vanillin.This work not only provides a new idea for the design of bio-absorbents for CO_(2) capture, but explores the application potential of lignin-based materials.
