The notorious growth of zinc dendrite and the water-induced corrosion of zinc metal anodes(ZMAs)restrict the practical development of aqueous zinc ion batteries(AZIBs).In this work,a zinc metallized,imide-pillared cov...The notorious growth of zinc dendrite and the water-induced corrosion of zinc metal anodes(ZMAs)restrict the practical development of aqueous zinc ion batteries(AZIBs).In this work,a zinc metallized,imide-pillared covalent organic framework(ZPC)protective film has been engineered as a stable Zn^(2+)ion-conducting interphase to modulate interfacial kinetics and suppress side reactions for ZMAs.Compared to bare Zn,ZPC@Zn exhibits a higher Zn^(2+)ionic conductivity,a larger Zn^(2+)transference number,a lower electronic conductivity,a smaller desolvation activation energy and correspondingly a significant suppression of corrosion,hydrogen evolution and Zn dendrites.Impressively,the ZPC@Zn||ZPC@Zn symmetric cell obtains a cycling lifespan over 3000 h under 5 mA cm^(-2)for 1 mA h cm^(-2).The ZPC@Zn||NH_(4)V_(4)O_(10)coin-type full battery delivers a specific capacity of 195.8 mA h g^(-1)with a retention rate of78.5%at 2 A g^(-1)after 1100 cycles,and the ZPC@Zn||NH_(4)V_(4)O_(10) pouch full cell shows a retention of70.1%in reversible capacity at 3 A g^(-1)after 1100 cycles.The present incorporation of imide-linked covalent organic frameworks in the surface modification of ZMAs will offer fresh perspectives in the search for ideal protective films for the practicality of AZIBs.展开更多
A novel poly(ether block amide)(PEBA)based solid-state polymer electrolyte(SPE)was prepared using a casting method,in which 20wt%lithium(Li)bis-(trifluoromethanesulfonyl)imide(LiTFSI)and aluminum oxide(Al_(2)O_(3))nan...A novel poly(ether block amide)(PEBA)based solid-state polymer electrolyte(SPE)was prepared using a casting method,in which 20wt%lithium(Li)bis-(trifluoromethanesulfonyl)imide(LiTFSI)and aluminum oxide(Al_(2)O_(3))nanoparticles were used as the Li salt and solid plasticizer,respectively.In the case of addition of 3wt%Al_(2)O_(3) nanoparticles,ion conductivity of the obtained PEBA 2533-20wt%LiTFSI-3wt%Al_(2)O_(3) SPE was 3.57×10^(−5) S cm^(−1) at 25°C.Furthermore,the Li symmetrical battery assembled with it showed excellent cycling stability(1000 h)at 0.1 mA cm^(−2).While,the assembled all-solid-state Li/PEBA 2533-20%LiTFSI-3wt%Al_(2)O_(3)/LiFePO 4(areal capacity:0.15 mAh cm^(−2))battery maintained 94.9%of the maximal capacity(133.9 mAh g^(−1@0.1) mA cm^(−2))at 60°C even after 650 cycles with a superior average coulombic efficiency(CE)of 99.84%.By using X-ray photoelectron spectroscope(XPS),self-aggregation layer(SAL)of polyamide 12(PA12)of PEBA 2533 was discovered,which should contribute to promoting the robustness of lithium fluoride(LiF)enriched solid-electrolyte interphase(SEI)layer.In addition,it is considered that the state of interface between SPE and cathode should be the cause of voltage polarization of the full cell.展开更多
A series of novel aromatic poly ( amide imide)s containing phthalazinone moieties were prepared from 2-(4-aminophenyl)-4-[3-methyl-4-(4-aminophenoxy)-2,3-phthalazinone-1], a novel diamine 1 with four diimide-dicarboxy...A series of novel aromatic poly ( amide imide)s containing phthalazinone moieties were prepared from 2-(4-aminophenyl)-4-[3-methyl-4-(4-aminophenoxy)-2,3-phthalazinone-1], a novel diamine 1 with four diimide-dicarboxylic acids by Yamazaki phosphorylation method with the inherent viscosity of 0.36~0.65 dL/g. These polymers had high glass transition temperatures above 300C and they lost 10% weight between 426~475C in N2. The structure of diamine 1 and the polymers was confirmed by IR, 1H NMR and MS. The obtained polymers were readily soluble in polar solvents such as NMP, m-cresol etc. and easily cast into tough, flexible films. The X-ray indicated that they are all amorphous.展开更多
The direct polymerization of an unsymmetrical kink non-coplanar heterocyclic diamine (1) with various aromatic bis(trimellitimide)s (2a-e) using triphenyl phosphite and pyridine as condensing agents could generate a s...The direct polymerization of an unsymmetrical kink non-coplanar heterocyclic diamine (1) with various aromatic bis(trimellitimide)s (2a-e) using triphenyl phosphite and pyridine as condensing agents could generate a series of new aromatic poly(amide imide)s (3a-e) containing the kink non-coplanar phthalazinone heterocyclic units in the polymer main chains with inherent viscosities of 0.58-0.66 dL/g. The polymers are readily soluble in a variety of solvents such as N,N- dimethylformamide, N,N-dimethylacetamide, dimethyl sulfoxide, N-methyl-2-pyrrolidinone, pyridine and m-cresol and can be cast to form flexible and tough films. The glass transition temperatures of polymers (Tg) are in the range of 301-327°C, and the temperatures for 5% weight loss in nitrogen are in the range of 498-521 'C.展开更多
A novel poly (amide-imide) was prepared from a novel monomer: 5,6-diphenyl-chloroformyl-3,4-benzenedicarboxylic anhydride and bis (4-aminophenyl) ether. The polymer was characterized by FTIR. (HNMR)-H-1. DSC and TGA.
The synthesis and characterization of a series of novel poly(aryl amide imide)s based on o diphenyltrimellitic anhydride are described.The poly(aryl amide imide)s having inherent viscosities of 0.39-1.43dL/g in N m...The synthesis and characterization of a series of novel poly(aryl amide imide)s based on o diphenyltrimellitic anhydride are described.The poly(aryl amide imide)s having inherent viscosities of 0.39-1.43dL/g in N methyl 2 pyrrolidinone at 30℃,were prepared by polymerization with aromatic diamines in N,N-dimethylacetamide and subsequent chemical imidization.All the polymers were amorphous,readily soluble in aprotic polar solvents such as DMAC,NMP,DMF,DMSO,and m cresol,and could be cast to form flexible and tough films.The glass trsanition temperatures were in the range of 284-336℃,and the temperatures for 5% weight loss in nitrogen were above 468℃.展开更多
In this article,six new optically active copoly(amide-imide)s(10a-f) were synthesized through the direct polycondensation reaction of N-phthalimido-L-aspartic acid(4) with 1,5-diamino naphthalene(8),3,4-diamino benzop...In this article,six new optically active copoly(amide-imide)s(10a-f) were synthesized through the direct polycondensation reaction of N-phthalimido-L-aspartic acid(4) with 1,5-diamino naphthalene(8),3,4-diamino benzophenone(9) in the presence of therphthahc acid(7),fumaric acid(6) and adipic acid(5) as a second diacid in a medium consisting of N-methyl-2-pyrrolidone,triphenyl phosphite, calcium chloride and pyridine.The resulting copolymers were fully characterized by means of FT-IR spectroscopy,elemental a...展开更多
Six new optically active poly（amide-imide）s （5a-f） were synthesized through the direct polycondensation reaction of N,N′-（4,4′- diphthaloyl）-bis-L-leucine （3） with six hydantoin derivatives （4a-f）. Tripben...Six new optically active poly（amide-imide）s （5a-f） were synthesized through the direct polycondensation reaction of N,N′-（4,4′- diphthaloyl）-bis-L-leucine （3） with six hydantoin derivatives （4a-f）. Tripbenyl phosphite （TPP）/pyridine in the presence of calcium chloride （CaCl2） and N-methyl-2-pyrrolidone （NMP） were successfully applied for direct polycondensation. The polycondensation reactions produce a series of new poly（amide-imide）s （5a-f） in high yields, and inherent viscosity between 0.42 and 0,55 dL/g. The resulting poly（amide-imide）s （5a-f） were characterized by elemental analysis, viscosity measurements, thermal gravimetric analysis （TGA and DTG）, solubility test and FT-IR spectroscopy.展开更多
Herein,we report a condition-controlled divergent synthesis of spiro indene-2,1'-isoindolinones and spiro isochroman-3,1'-isoindolinones through cobalt-catalyzed formal[4+1]and[4+1+1]spirocyclization of aromat...Herein,we report a condition-controlled divergent synthesis of spiro indene-2,1'-isoindolinones and spiro isochroman-3,1'-isoindolinones through cobalt-catalyzed formal[4+1]and[4+1+1]spirocyclization of aromatic amides with 2-diazo-1H-indene-1,3(2H)-dione.When the reaction is carried out under air in ethyl acetate,spiro indene-2,1'-isoindolinones are formed through Co(II)-catalyzed C—H/N—H[4+1]spirocyclization.When the reaction is run under O2 in CH3CN,on the other hand,spiro isochroman-3,1'-isoindolinones are generated through Baeyer-Villiger oxidation of the in situ formed spiro indene-2,1'-isoindolinones with O2 as a cheaper and environmental-friendly oxygen source.In general,these protocols have advantages such as using non-precious and earth-abundant metal catalyst,no extra additive,high efficiency and regioselectivity.A gram-scale synthesis and the removal of the directing group further highlight its utility.展开更多
The reactions of imidates including cyclic imidates, oxazolines and dihydrooxazine with phenoxyacetyl chloride, were investigated. The results indicate that diacylamide or acylamide was generated from N-phenoxyacetyl...The reactions of imidates including cyclic imidates, oxazolines and dihydrooxazine with phenoxyacetyl chloride, were investigated. The results indicate that diacylamide or acylamide was generated from N-phenoxyacetylated imidates, while cyclic imidate oxazolines underwent a ring-opening reaction to yield different amides depending on the reaction conditions. Even under non-nucleophilic conditions, no β-lactam-fused oxazoline derivative was obtained.展开更多
The mass transfer of thiophene through pervaporation（PV） membranes could be facilitated by certain transitional metal ions like Ag+, Mn2+, and Cr3+ thanks to their p complexation with thiophene. In this study, Ag+, ...The mass transfer of thiophene through pervaporation（PV） membranes could be facilitated by certain transitional metal ions like Ag+, Mn2+, and Cr3+ thanks to their p complexation with thiophene. In this study, Ag+, Mn2+, and Cr3+ ions were loaded onto the polyether block amide（PEBAX）/PAN composite membranes and were tested on the performance for separation of thiophene/n-heptane mixture. Pervaporation test results showed that the pervaporative separation index increased significantly to 73.1%, 75.5%, and 97.2% at 30 oC for the Ag+-, Mn2+-, Cr3+-loaded PEBAX membranes, respectively,as compared to the pristine PEBAX/PAN composite membrane.展开更多
基金supported by the National Natural Science Foundation of China (52373065)the Joint Fund of Ministry of Education for Equipment Pre-research (8091B032206)+1 种基金the Guang Dong Basic and Applied Basic Research Foundation (2021A1515111067,2023A1515010735)the start-up funding of“Hundred Talent Program”from Sun Yat-sen University。
文摘The notorious growth of zinc dendrite and the water-induced corrosion of zinc metal anodes(ZMAs)restrict the practical development of aqueous zinc ion batteries(AZIBs).In this work,a zinc metallized,imide-pillared covalent organic framework(ZPC)protective film has been engineered as a stable Zn^(2+)ion-conducting interphase to modulate interfacial kinetics and suppress side reactions for ZMAs.Compared to bare Zn,ZPC@Zn exhibits a higher Zn^(2+)ionic conductivity,a larger Zn^(2+)transference number,a lower electronic conductivity,a smaller desolvation activation energy and correspondingly a significant suppression of corrosion,hydrogen evolution and Zn dendrites.Impressively,the ZPC@Zn||ZPC@Zn symmetric cell obtains a cycling lifespan over 3000 h under 5 mA cm^(-2)for 1 mA h cm^(-2).The ZPC@Zn||NH_(4)V_(4)O_(10)coin-type full battery delivers a specific capacity of 195.8 mA h g^(-1)with a retention rate of78.5%at 2 A g^(-1)after 1100 cycles,and the ZPC@Zn||NH_(4)V_(4)O_(10) pouch full cell shows a retention of70.1%in reversible capacity at 3 A g^(-1)after 1100 cycles.The present incorporation of imide-linked covalent organic frameworks in the surface modification of ZMAs will offer fresh perspectives in the search for ideal protective films for the practicality of AZIBs.
文摘A novel poly(ether block amide)(PEBA)based solid-state polymer electrolyte(SPE)was prepared using a casting method,in which 20wt%lithium(Li)bis-(trifluoromethanesulfonyl)imide(LiTFSI)and aluminum oxide(Al_(2)O_(3))nanoparticles were used as the Li salt and solid plasticizer,respectively.In the case of addition of 3wt%Al_(2)O_(3) nanoparticles,ion conductivity of the obtained PEBA 2533-20wt%LiTFSI-3wt%Al_(2)O_(3) SPE was 3.57×10^(−5) S cm^(−1) at 25°C.Furthermore,the Li symmetrical battery assembled with it showed excellent cycling stability(1000 h)at 0.1 mA cm^(−2).While,the assembled all-solid-state Li/PEBA 2533-20%LiTFSI-3wt%Al_(2)O_(3)/LiFePO 4(areal capacity:0.15 mAh cm^(−2))battery maintained 94.9%of the maximal capacity(133.9 mAh g^(−1@0.1) mA cm^(−2))at 60°C even after 650 cycles with a superior average coulombic efficiency(CE)of 99.84%.By using X-ray photoelectron spectroscope(XPS),self-aggregation layer(SAL)of polyamide 12(PA12)of PEBA 2533 was discovered,which should contribute to promoting the robustness of lithium fluoride(LiF)enriched solid-electrolyte interphase(SEI)layer.In addition,it is considered that the state of interface between SPE and cathode should be the cause of voltage polarization of the full cell.
文摘A series of novel aromatic poly ( amide imide)s containing phthalazinone moieties were prepared from 2-(4-aminophenyl)-4-[3-methyl-4-(4-aminophenoxy)-2,3-phthalazinone-1], a novel diamine 1 with four diimide-dicarboxylic acids by Yamazaki phosphorylation method with the inherent viscosity of 0.36~0.65 dL/g. These polymers had high glass transition temperatures above 300C and they lost 10% weight between 426~475C in N2. The structure of diamine 1 and the polymers was confirmed by IR, 1H NMR and MS. The obtained polymers were readily soluble in polar solvents such as NMP, m-cresol etc. and easily cast into tough, flexible films. The X-ray indicated that they are all amorphous.
基金This work was supported by the Key Natural Science Foundation of Fujian Province (E0320003).
文摘The direct polymerization of an unsymmetrical kink non-coplanar heterocyclic diamine (1) with various aromatic bis(trimellitimide)s (2a-e) using triphenyl phosphite and pyridine as condensing agents could generate a series of new aromatic poly(amide imide)s (3a-e) containing the kink non-coplanar phthalazinone heterocyclic units in the polymer main chains with inherent viscosities of 0.58-0.66 dL/g. The polymers are readily soluble in a variety of solvents such as N,N- dimethylformamide, N,N-dimethylacetamide, dimethyl sulfoxide, N-methyl-2-pyrrolidinone, pyridine and m-cresol and can be cast to form flexible and tough films. The glass transition temperatures of polymers (Tg) are in the range of 301-327°C, and the temperatures for 5% weight loss in nitrogen are in the range of 498-521 'C.
文摘A novel poly (amide-imide) was prepared from a novel monomer: 5,6-diphenyl-chloroformyl-3,4-benzenedicarboxylic anhydride and bis (4-aminophenyl) ether. The polymer was characterized by FTIR. (HNMR)-H-1. DSC and TGA.
文摘The synthesis and characterization of a series of novel poly(aryl amide imide)s based on o diphenyltrimellitic anhydride are described.The poly(aryl amide imide)s having inherent viscosities of 0.39-1.43dL/g in N methyl 2 pyrrolidinone at 30℃,were prepared by polymerization with aromatic diamines in N,N-dimethylacetamide and subsequent chemical imidization.All the polymers were amorphous,readily soluble in aprotic polar solvents such as DMAC,NMP,DMF,DMSO,and m cresol,and could be cast to form flexible and tough films.The glass trsanition temperatures were in the range of 284-336℃,and the temperatures for 5% weight loss in nitrogen were above 468℃.
文摘In this article,six new optically active copoly(amide-imide)s(10a-f) were synthesized through the direct polycondensation reaction of N-phthalimido-L-aspartic acid(4) with 1,5-diamino naphthalene(8),3,4-diamino benzophenone(9) in the presence of therphthahc acid(7),fumaric acid(6) and adipic acid(5) as a second diacid in a medium consisting of N-methyl-2-pyrrolidone,triphenyl phosphite, calcium chloride and pyridine.The resulting copolymers were fully characterized by means of FT-IR spectroscopy,elemental a...
文摘Six new optically active poly（amide-imide）s （5a-f） were synthesized through the direct polycondensation reaction of N,N′-（4,4′- diphthaloyl）-bis-L-leucine （3） with six hydantoin derivatives （4a-f）. Tripbenyl phosphite （TPP）/pyridine in the presence of calcium chloride （CaCl2） and N-methyl-2-pyrrolidone （NMP） were successfully applied for direct polycondensation. The polycondensation reactions produce a series of new poly（amide-imide）s （5a-f） in high yields, and inherent viscosity between 0.42 and 0,55 dL/g. The resulting poly（amide-imide）s （5a-f） were characterized by elemental analysis, viscosity measurements, thermal gravimetric analysis （TGA and DTG）, solubility test and FT-IR spectroscopy.
基金the National Natural Science Foundation of China(22101075,U2004189)Central Plains Science and Technology Innovation Leader Project(224200510009)+1 种基金Postdoctoral Research Grant in Henan Province(202103085)Henan Key Laboratory of Organic Functional Molecules and Drug Innovation,and 111 Project(D17007)for financial support.
文摘Herein,we report a condition-controlled divergent synthesis of spiro indene-2,1'-isoindolinones and spiro isochroman-3,1'-isoindolinones through cobalt-catalyzed formal[4+1]and[4+1+1]spirocyclization of aromatic amides with 2-diazo-1H-indene-1,3(2H)-dione.When the reaction is carried out under air in ethyl acetate,spiro indene-2,1'-isoindolinones are formed through Co(II)-catalyzed C—H/N—H[4+1]spirocyclization.When the reaction is run under O2 in CH3CN,on the other hand,spiro isochroman-3,1'-isoindolinones are generated through Baeyer-Villiger oxidation of the in situ formed spiro indene-2,1'-isoindolinones with O2 as a cheaper and environmental-friendly oxygen source.In general,these protocols have advantages such as using non-precious and earth-abundant metal catalyst,no extra additive,high efficiency and regioselectivity.A gram-scale synthesis and the removal of the directing group further highlight its utility.
文摘The reactions of imidates including cyclic imidates, oxazolines and dihydrooxazine with phenoxyacetyl chloride, were investigated. The results indicate that diacylamide or acylamide was generated from N-phenoxyacetylated imidates, while cyclic imidate oxazolines underwent a ring-opening reaction to yield different amides depending on the reaction conditions. Even under non-nucleophilic conditions, no β-lactam-fused oxazoline derivative was obtained.
基金The financial support from the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology (2013Z009)the Guangxi Natural Science Fund (2014jjAA20079)the Guangdong Province of Quality and Technical Supervision Bureau (2018ZZ01) is greatly appreciated
文摘The mass transfer of thiophene through pervaporation（PV） membranes could be facilitated by certain transitional metal ions like Ag+, Mn2+, and Cr3+ thanks to their p complexation with thiophene. In this study, Ag+, Mn2+, and Cr3+ ions were loaded onto the polyether block amide（PEBAX）/PAN composite membranes and were tested on the performance for separation of thiophene/n-heptane mixture. Pervaporation test results showed that the pervaporative separation index increased significantly to 73.1%, 75.5%, and 97.2% at 30 oC for the Ag+-, Mn2+-, Cr3+-loaded PEBAX membranes, respectively,as compared to the pristine PEBAX/PAN composite membrane.
