The quality of MAPbI3 film prepared by solvent engineering process highly depends on environment and antisolvent control.Here,we provided a simple methylamine chloride(MACl)solution treatment using a two-step process ...The quality of MAPbI3 film prepared by solvent engineering process highly depends on environment and antisolvent control.Here,we provided a simple methylamine chloride(MACl)solution treatment using a two-step process to enlarge the perovskite crystal grain sizes to more than 1 lm.Other than treatment on the film surface,the MACl solution diffuses into the MAPbI_(3) films to assist the recrystallization of small crystal at the bottom of perovskite film.The imitative contact between perovskite and substrate is formed.Meanwhile,the enlargement of grain size and ten times enhancement of crystalline reduce trap-assisted recombination of perovskite films.Thus,the significant improvement of cell efficiency of 20.89%as well as device stability is obtained with the MACl treatment.展开更多
The initial decomposition of methylamine on Mo(100) surface has been investigated by self-consistent (GGA-PW91) density functional theory combined with periodic slab model. The adsorption energies of possible spec...The initial decomposition of methylamine on Mo(100) surface has been investigated by self-consistent (GGA-PW91) density functional theory combined with periodic slab model. The adsorption energies of possible species and the activation energies for possible elementary reactions involved are obtained in the present work. Our results indicate that the barriers decreased with the order of C-NN-HC-H. In addition, metastable adsorption of the abstracted hydrogen atom on the hollow site in the final state is also considered for the N-H and C-H bond breaking. For the C-H bond cleavage, the reaction barrier that the abstracted hydrogen located on the hollow site in the final state is lower than that on the bridge site. However, for the N H bond breaking, the barriers are alike for the abstracted hydrogen on both hollow and bridge sites in the final state.展开更多
Upscaling perovskite solar cell fabrication is one of the key challenges in the pathway for commercialization.The slow evaporation of frequently used solvents(DMF or DMSO) limits the fast perovskite layer crystallizat...Upscaling perovskite solar cell fabrication is one of the key challenges in the pathway for commercialization.The slow evaporation of frequently used solvents(DMF or DMSO) limits the fast perovskite layer crystallization,hindering their implementation in large scale deposition methods.Alternatively,methylamine-based precursors have demonstrated rapid crystallization,leading to uniform and specular films.Nonetheless,their application has been limited to MAPbI3 perovskites with limited efficiency and stability.In this work,we report the requirements for stabilizing α-phase of mixed cation perovskites with high amount of formamidinium by using a methylamine-based precursor.We found that even though,there are many methods for incorporating the methylamine(MA) in precursors or films;the MA content determines stabilization of the α-phase and therefore the viscous-solution route is the only method to incorporate high amounts of MA.At low amounts of MA,perovskite tend to crystallize in 1D dimensional FA_(3)(MA)PbI5 phases due to the incomplete solvation of the PbI6-clusters.In contrast,high MA ratio induces a full solvation of the clusters,leading to a rapid crystallization and a full stabilization of the active 3D α-phase.These results open a window in the development and understanding of new precursors for the fabrication of high efficient,stable and scalable perovskite devices.展开更多
N-pivot lariat ethers with picrylamino group as a chromophore (1, 2 and 3) have been prepared by reaction of N-(4-aminoaryl)monoaza crown ethers with picryl chrolide, and the selective coloration of 1, 2 and 3 for alk...N-pivot lariat ethers with picrylamino group as a chromophore (1, 2 and 3) have been prepared by reaction of N-(4-aminoaryl)monoaza crown ethers with picryl chrolide, and the selective coloration of 1, 2 and 3 for alkali metal salts and amines has been studied by UV-Vis spectra.展开更多
Enantiomers of a-substituted-(2-pyridyl)-methylarfdnes uere separated on SC -7 gas chromatograph with a 20m×0.25mm Chirasil-Val capIlary column,Carrier gas was nitro- gen or hydrogen.The resolution factors(ri.s) ...Enantiomers of a-substituted-(2-pyridyl)-methylarfdnes uere separated on SC -7 gas chromatograph with a 20m×0.25mm Chirasil-Val capIlary column,Carrier gas was nitro- gen or hydrogen.The resolution factors(ri.s) were 1.02 to 1.06.Enantiomers of pyridyl anines were separated to and near to base line.展开更多
Seven novel platinum (Ⅱ) complexes [ Pt(Ⅱ) (NH3) (CH3NH2)X2] (Ⅰ-Ⅶ ) ( X: CH3COO^-, CH2CICOO^- , CHCI2COO^- , C6H5-COO^- , p-CH3O--C6H4-COO^- , p-NH2-C6H4-COO^- , p-NO2--C6H4- COO^-) were prepared and ...Seven novel platinum (Ⅱ) complexes [ Pt(Ⅱ) (NH3) (CH3NH2)X2] (Ⅰ-Ⅶ ) ( X: CH3COO^-, CH2CICOO^- , CHCI2COO^- , C6H5-COO^- , p-CH3O--C6H4-COO^- , p-NH2-C6H4-COO^- , p-NO2--C6H4- COO^-) were prepared and characterized by means of elemental analysis, molar conductivity, thermal analysis, IR, UV, and ^1H NMR spectrometries. The cytotoxicity against HCT-8, BGC-823, MCF-7, EJ, and HL-60 cell lines increases in the following sequence: cisplatin 〉 Ⅳ 〉 Ⅴ 〉 Ⅵ 〉 Ⅶ 〉 Ⅰ 〉 Ⅱ 〉 Ⅲ. Moreover, the complexes ( Ⅰ --Ⅻ) display substantially greater activities agaist EJ and HL-60 cell lines than those against the cell lines from other carcinomas. They can induce a concentration-dependent accumulation of HL-60 cells in the G2/M phase of the cell cycle as cisplatin. There is no significant correlation between total DNA platination levels and cytotoxicity of the complexes.展开更多
Three polymeric adsorbents with hydrogen bonding acceptors, methylamine, N-methyl-acetamide and aminotri(hydroxymethyl)methane modified resins are synthesized from chloromethylated X-5 resin. Adsorption isotherms of p...Three polymeric adsorbents with hydrogen bonding acceptors, methylamine, N-methyl-acetamide and aminotri(hydroxymethyl)methane modified resins are synthesized from chloromethylated X-5 resin. Adsorption isotherms of phenol and theophylline onto the three modified resins and the original X-5 resin from aqueous solution are measured. The results show that adsorption of compounds with hydrogen bonding donor onto methylamine and N-methylacetamide modified resins is enhanced as compared with that onto X-5 resin, and adsorption mechanism between the adsorbents and the adsorbates is mainly based on hydrogen bonding and hydrophobic interaction. While adsorption of compounds with hydrogen bonding donor onto aminotri(hydroxymethyl)methane modified resin is lowered as compared with that onto X-5 resin, and adsorption mechanism between the adsorbent and the adsorbates is mainly based on hydrophobic interaction.展开更多
All-inorganic CsPbX3(X = I, Br) perovskites without organic component are promising for long-term stability but face main challenges of facile fabrication and phase stability. Here we discover a general organic methyl...All-inorganic CsPbX3(X = I, Br) perovskites without organic component are promising for long-term stability but face main challenges of facile fabrication and phase stability. Here we discover a general organic methylamine acetate salt mediated growth method to deposit high quality phase pure and stable CsPbX3(X = I, Br) perovskite films via a novel precursor consisting of stoichiometric cesium acetate(CsAc),methylamine halide(MAX) and lead halide(PbX2). Interestingly, these organic salts of CsAc and MAX could efficiently promote the crystallization process especially lower the crystallization temperature,but do not introduce the incorporation of organic MA cation into all-inorganic CsPbX3 perovskites.These phase pure and stable CsPbX3 perovskites with tunable band gaps can be fabricated into high efficiency photovoltaics. Our organic salt mediated growth of all-inorganic perovskite not only reveals the all-inorganic CsPbX3 perovskite’s unique crystal growth mechanism but also demonstrates their promising application for photovoltaics.展开更多
A series of 10-methyl-1,2,3,4,5,6,7,8,9,10-decahydroacridine-1,8-dione derivatives were synthesized by one-pot reaction of aldehyde, dimedone or 1,3-cyclohexanedione and methylamine in glycol or water under microwave ...A series of 10-methyl-1,2,3,4,5,6,7,8,9,10-decahydroacridine-1,8-dione derivatives were synthesized by one-pot reaction of aldehyde, dimedone or 1,3-cyclohexanedione and methylamine in glycol or water under microwave heating without catalyst. The method has the advantage of short routine and reaction time, high yields as well as friendly environment. And the reaction was not only suitable for aliphatic and aromatic monoaldehyde, but also for aromatic dialdehyde.展开更多
The UV/Clprocess is commonly used to achieve a multiple-barrier disinfection and maintain residuals. The study chose methylamine as a precursor to study the formation of hightoxic halonitromethanes(HNMs) in the presen...The UV/Clprocess is commonly used to achieve a multiple-barrier disinfection and maintain residuals. The study chose methylamine as a precursor to study the formation of hightoxic halonitromethanes(HNMs) in the presence of bromide ions(Br-) during UV/Cldisinfection. The maximum yield of HNMs increased first and then decreased with increasing concentration of Br-. An excessively high concentration of Br-induced the maximum yield of HNMs in advance. The maximum bromine incorporation factor(BIF) increased, while the maximum bromine utilization factor(BUF) decreased with the increase of Br-concentration. The maximum yield of HNMs decreased as p H value increased from 6.0 to 8.0 due to the deprotonation process. The BUF value remained relatively higher under an acidic condition, while p H value had no evident influence on the BIF value. The maximum yield of HNMs and value of BUF maximized at a Cl:Br-ratio of 12.5, whereas the BIF value remained relatively higher at low Cl:Br-ratios(2.5 and 5). The amino group in methylamine was first halogenated, and then released into solution as inorganic nitrogen by the rupture of C-N bond or transformed to nitro group by oxidation and elimination pathways. The maximum yield of HNMs in real waters was higher than that in pure water due to the high content of dissolved organic carbon. Two real waters were sampled to verify the law of HNMs formation. This study helps to understand the HNMs formation(especially brominated species) when the UV/Clprocess is adopted as a disinfection technique.展开更多
The adsorption and decomposition mechanisms of methylamine catalyzed by Pt4 cluster supported on ruffle(110) titania[namely, Pt4/TiO2-R(110)] were investigated via density functional theory slab calculations with ...The adsorption and decomposition mechanisms of methylamine catalyzed by Pt4 cluster supported on ruffle(110) titania[namely, Pt4/TiO2-R(110)] were investigated via density functional theory slab calculations with Hubbard corrections(DFT+U). The adsorption energies under the most stable configuration of the possible species and the energy barriers of the possible elementary reactions involved in methylamine decomposition were obtained. Through systematic calculations for the reaction mechanism of methylamine decomposition on the PtVTiO2-R(110), the most possible decomposition path is CHaNH2→CH2NH2+H→CH2NH+2H→CHNH+3H→HCN+4H→CN+5H, which is similar to that of methylamine dissociation catalyzed by Pt(100) surface.展开更多
基金financially supported by the National Key R&D Program of China (Grant No. 2020YFB1506404)the 111 Project (Grant No. B16016)+1 种基金the National Natural Science Foundation of China (Grant Nos. 51961165106, 51572080 and 61904053)the Fundamental Research Funds for the Central Universities (Grant Nos. 2019MS026, 2019MS027 and 2020MS080)。
文摘The quality of MAPbI3 film prepared by solvent engineering process highly depends on environment and antisolvent control.Here,we provided a simple methylamine chloride(MACl)solution treatment using a two-step process to enlarge the perovskite crystal grain sizes to more than 1 lm.Other than treatment on the film surface,the MACl solution diffuses into the MAPbI_(3) films to assist the recrystallization of small crystal at the bottom of perovskite film.The imitative contact between perovskite and substrate is formed.Meanwhile,the enlargement of grain size and ten times enhancement of crystalline reduce trap-assisted recombination of perovskite films.Thus,the significant improvement of cell efficiency of 20.89%as well as device stability is obtained with the MACl treatment.
基金supported by the National Natural Science Foundation of China (Grants No. 21073113)the Intramural Foundation of Shanxi Datong University
文摘The initial decomposition of methylamine on Mo(100) surface has been investigated by self-consistent (GGA-PW91) density functional theory combined with periodic slab model. The adsorption energies of possible species and the activation energies for possible elementary reactions involved are obtained in the present work. Our results indicate that the barriers decreased with the order of C-NN-HC-H. In addition, metastable adsorption of the abstracted hydrogen atom on the hollow site in the final state is also considered for the N-H and C-H bond breaking. For the C-H bond cleavage, the reaction barrier that the abstracted hydrogen located on the hollow site in the final state is lower than that on the bridge site. However, for the N H bond breaking, the barriers are alike for the abstracted hydrogen on both hollow and bridge sites in the final state.
基金financial support provided by the committee for the development of research(CODI) of the Universidad de Antioquia,in the framework of the project 2017-16000the financial support of the Colombia Scientific Program within the framework of the call Ecosistema Cientifíco(Contract FP44842-218-2018)。
文摘Upscaling perovskite solar cell fabrication is one of the key challenges in the pathway for commercialization.The slow evaporation of frequently used solvents(DMF or DMSO) limits the fast perovskite layer crystallization,hindering their implementation in large scale deposition methods.Alternatively,methylamine-based precursors have demonstrated rapid crystallization,leading to uniform and specular films.Nonetheless,their application has been limited to MAPbI3 perovskites with limited efficiency and stability.In this work,we report the requirements for stabilizing α-phase of mixed cation perovskites with high amount of formamidinium by using a methylamine-based precursor.We found that even though,there are many methods for incorporating the methylamine(MA) in precursors or films;the MA content determines stabilization of the α-phase and therefore the viscous-solution route is the only method to incorporate high amounts of MA.At low amounts of MA,perovskite tend to crystallize in 1D dimensional FA_(3)(MA)PbI5 phases due to the incomplete solvation of the PbI6-clusters.In contrast,high MA ratio induces a full solvation of the clusters,leading to a rapid crystallization and a full stabilization of the active 3D α-phase.These results open a window in the development and understanding of new precursors for the fabrication of high efficient,stable and scalable perovskite devices.
文摘N-pivot lariat ethers with picrylamino group as a chromophore (1, 2 and 3) have been prepared by reaction of N-(4-aminoaryl)monoaza crown ethers with picryl chrolide, and the selective coloration of 1, 2 and 3 for alkali metal salts and amines has been studied by UV-Vis spectra.
基金The project is supported by National Nature science Foundation of China.
文摘Enantiomers of a-substituted-(2-pyridyl)-methylarfdnes uere separated on SC -7 gas chromatograph with a 20m×0.25mm Chirasil-Val capIlary column,Carrier gas was nitro- gen or hydrogen.The resolution factors(ri.s) were 1.02 to 1.06.Enantiomers of pyridyl anines were separated to and near to base line.
文摘Seven novel platinum (Ⅱ) complexes [ Pt(Ⅱ) (NH3) (CH3NH2)X2] (Ⅰ-Ⅶ ) ( X: CH3COO^-, CH2CICOO^- , CHCI2COO^- , C6H5-COO^- , p-CH3O--C6H4-COO^- , p-NH2-C6H4-COO^- , p-NO2--C6H4- COO^-) were prepared and characterized by means of elemental analysis, molar conductivity, thermal analysis, IR, UV, and ^1H NMR spectrometries. The cytotoxicity against HCT-8, BGC-823, MCF-7, EJ, and HL-60 cell lines increases in the following sequence: cisplatin 〉 Ⅳ 〉 Ⅴ 〉 Ⅵ 〉 Ⅶ 〉 Ⅰ 〉 Ⅱ 〉 Ⅲ. Moreover, the complexes ( Ⅰ --Ⅻ) display substantially greater activities agaist EJ and HL-60 cell lines than those against the cell lines from other carcinomas. They can induce a concentration-dependent accumulation of HL-60 cells in the G2/M phase of the cell cycle as cisplatin. There is no significant correlation between total DNA platination levels and cytotoxicity of the complexes.
基金The National Natural Science Foundation of China (No.: 29974015 and 20174017)
文摘Three polymeric adsorbents with hydrogen bonding acceptors, methylamine, N-methyl-acetamide and aminotri(hydroxymethyl)methane modified resins are synthesized from chloromethylated X-5 resin. Adsorption isotherms of phenol and theophylline onto the three modified resins and the original X-5 resin from aqueous solution are measured. The results show that adsorption of compounds with hydrogen bonding donor onto methylamine and N-methylacetamide modified resins is enhanced as compared with that onto X-5 resin, and adsorption mechanism between the adsorbents and the adsorbates is mainly based on hydrogen bonding and hydrophobic interaction. While adsorption of compounds with hydrogen bonding donor onto aminotri(hydroxymethyl)methane modified resin is lowered as compared with that onto X-5 resin, and adsorption mechanism between the adsorbent and the adsorbates is mainly based on hydrophobic interaction.
基金support of the National Natural Science Foundation of China (21777096, 51861145101)Huoyingdong Grant (151046)+1 种基金the support of the Initiative Postdocs Supporting Program (BX20180185)China Postdoctoral Science Foundation (2018M640387)
文摘All-inorganic CsPbX3(X = I, Br) perovskites without organic component are promising for long-term stability but face main challenges of facile fabrication and phase stability. Here we discover a general organic methylamine acetate salt mediated growth method to deposit high quality phase pure and stable CsPbX3(X = I, Br) perovskite films via a novel precursor consisting of stoichiometric cesium acetate(CsAc),methylamine halide(MAX) and lead halide(PbX2). Interestingly, these organic salts of CsAc and MAX could efficiently promote the crystallization process especially lower the crystallization temperature,but do not introduce the incorporation of organic MA cation into all-inorganic CsPbX3 perovskites.These phase pure and stable CsPbX3 perovskites with tunable band gaps can be fabricated into high efficiency photovoltaics. Our organic salt mediated growth of all-inorganic perovskite not only reveals the all-inorganic CsPbX3 perovskite’s unique crystal growth mechanism but also demonstrates their promising application for photovoltaics.
基金Project supported by the National Natural Science Foundation of China (No. 20372057) and the Natural Science Foundation of Jiangsu Province (No. BK2001142).
文摘A series of 10-methyl-1,2,3,4,5,6,7,8,9,10-decahydroacridine-1,8-dione derivatives were synthesized by one-pot reaction of aldehyde, dimedone or 1,3-cyclohexanedione and methylamine in glycol or water under microwave heating without catalyst. The method has the advantage of short routine and reaction time, high yields as well as friendly environment. And the reaction was not only suitable for aliphatic and aromatic monoaldehyde, but also for aromatic dialdehyde.
基金financially supported by the National Natural Science Foundation of China (Nos. 22076023 , 21677032 and 51808496)。
文摘The UV/Clprocess is commonly used to achieve a multiple-barrier disinfection and maintain residuals. The study chose methylamine as a precursor to study the formation of hightoxic halonitromethanes(HNMs) in the presence of bromide ions(Br-) during UV/Cldisinfection. The maximum yield of HNMs increased first and then decreased with increasing concentration of Br-. An excessively high concentration of Br-induced the maximum yield of HNMs in advance. The maximum bromine incorporation factor(BIF) increased, while the maximum bromine utilization factor(BUF) decreased with the increase of Br-concentration. The maximum yield of HNMs decreased as p H value increased from 6.0 to 8.0 due to the deprotonation process. The BUF value remained relatively higher under an acidic condition, while p H value had no evident influence on the BIF value. The maximum yield of HNMs and value of BUF maximized at a Cl:Br-ratio of 12.5, whereas the BIF value remained relatively higher at low Cl:Br-ratios(2.5 and 5). The amino group in methylamine was first halogenated, and then released into solution as inorganic nitrogen by the rupture of C-N bond or transformed to nitro group by oxidation and elimination pathways. The maximum yield of HNMs in real waters was higher than that in pure water due to the high content of dissolved organic carbon. Two real waters were sampled to verify the law of HNMs formation. This study helps to understand the HNMs formation(especially brominated species) when the UV/Clprocess is adopted as a disinfection technique.
基金Supported by the National Natural Science Foundation of China(Nos.21503122, 21346002), the Shanxi Province Science Foundation for Youths, China(No.2014021016-2), the Scientific and Technological Programs in Shanxi Province, China(No. 2015031017), the Industrial and Technological Programs in Datong City, China(No.2015022) and the Foundation of Key Laboratory of Advanced Energy Materials Chemistry of the Ministry of Education of China.
文摘The adsorption and decomposition mechanisms of methylamine catalyzed by Pt4 cluster supported on ruffle(110) titania[namely, Pt4/TiO2-R(110)] were investigated via density functional theory slab calculations with Hubbard corrections(DFT+U). The adsorption energies under the most stable configuration of the possible species and the energy barriers of the possible elementary reactions involved in methylamine decomposition were obtained. Through systematic calculations for the reaction mechanism of methylamine decomposition on the PtVTiO2-R(110), the most possible decomposition path is CHaNH2→CH2NH2+H→CH2NH+2H→CHNH+3H→HCN+4H→CN+5H, which is similar to that of methylamine dissociation catalyzed by Pt(100) surface.