It has been found that microwave assisted decarboxylation of malonic acid derivatives can be achieved under solvent-free and catalyst free conditions. This new method produces the corresponding carboxylic acid in a pu...It has been found that microwave assisted decarboxylation of malonic acid derivatives can be achieved under solvent-free and catalyst free conditions. This new method produces the corresponding carboxylic acid in a pure manner and with a high yield in a very short reaction time: 3 - 10 min. In general terms, the condition under which this reaction is carried out accelerates the decarboxylation significantly of a series of disubstituted malonic acid derivatives, and makes this new process efficient, easy and environmentally friendly.展开更多
Catalytic hydrodeoxygenation(HDO)is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels,but highly challenging due to the lack of highly efficien...Catalytic hydrodeoxygenation(HDO)is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels,but highly challenging due to the lack of highly efficient nonprecious metal catalysts.Herein,we report for the first time of a facile synthetic approach to controllably fabricate well-defined Ni-Co alloy NPs confined on the tip of N-CNTs as HDO catalyst.The resultant Ni-Co alloy catalyst possesses outstanding HDO performance towards biomass-derived vanillin into 2-methoxy-4-methylphenol in water with 100%conversion efficiency and selectivity under mild reaction conditions,surpassing the reported high performance nonprecious HDO catalysts.Impressively,our experimental results also unveil that the Ni-Co alloy catalyst can be generically applied to catalyze HDO of vanillin derivatives and other aromatic aldehydes in water with 100%conversion efficiency and over 90%selectivity.Importantly,our DFT calculations and experimental results confirm that the achieved outstanding HDO catalytic performance is due to the greatly promoted selective adsorption and activation of C=O,and desorption of the activated hydrogen species by the synergism of the alloyed Ni-Co NPs.The findings of this work affords a new strategy to design and develop efficient transition metal-based catalysts for HDO reactions in water.展开更多
This paper deals with the enantioseparation of phenylsuccinic acid(H2A)enantiomers by liquid-liquid reactive extraction usingβ-CD derivatives as aqueous selectors.Cyclodextrin and its derivatives can interact with gu...This paper deals with the enantioseparation of phenylsuccinic acid(H2A)enantiomers by liquid-liquid reactive extraction usingβ-CD derivatives as aqueous selectors.Cyclodextrin and its derivatives can interact with guest molecules selectively to form complexes with different stabilities.Cyclodextrin derivatives are not soluble in organic liquids,but highly soluble in water.In this work,hydroxypropyl-β-cyclodextrin(HP-β-CD),hydroxyethyl- β-cyclodextrin(HE-β-CD)and methyl-β-cyclodextrin(Me-β-CD)were selected as chiral selectors in aqueous phase for the reactive extraction of phenylsuccinic acid enantiomers from organic phase to aqueous phase.The results show that the efficiency of the extraction depends,often strongly,on a number of process variables,including the types of organic solvents andβ-CD derivatives,the concentrations of the extractants and H2A enantiomers,pH and temperature.HP-β-CD,HE-β-CD and Me-β-CD have stronger recognition abilities for R-phenylsuccinic acid than for S-phenylsuccinic acid.Among the three kinds ofβ-CD derivatives,HP-β-CD has the strongest separation ability. Excellent enantioseparation was achieved under the optimal conditions of pH of 2.5 and temperature of 5°C with a maximum enantioselectivity(a)of 2.38.Reactive extraction of enantiomers with hydrophilicβ-CD derivatives is of strong chiral separation ability and can be hopeful for separations of various enantiomers at a large-scale.展开更多
An efficient solution-processable route employing Pb(Ac)2 as lead source and anti-solvent treatment to achieve fully covered and homogenous perovskite films is reported. The effect of different solution methods and de...An efficient solution-processable route employing Pb(Ac)2 as lead source and anti-solvent treatment to achieve fully covered and homogenous perovskite films is reported. The effect of different solution methods and device architectures on the morphologies of perovskite films were systematically investigated. Our results show that the planar perovskite layer fabricated by one-step solution method achieved fully covered and pinhole-free films. Further anti-solvent treatment using chlorobenzene (CB) promoted a perovskite film with highly smooth surfaces and enlarged grain sizes. Device fabricated from CB treated perovskite film achieved a best PCE of 15.80%, in comparison with 14.02%for the untreated device. These results evidently suggest a feasible route towards controlling the crystallization and morphology of planar heterojunction (PHJ) PSCs for improved efficiency.展开更多
文摘It has been found that microwave assisted decarboxylation of malonic acid derivatives can be achieved under solvent-free and catalyst free conditions. This new method produces the corresponding carboxylic acid in a pure manner and with a high yield in a very short reaction time: 3 - 10 min. In general terms, the condition under which this reaction is carried out accelerates the decarboxylation significantly of a series of disubstituted malonic acid derivatives, and makes this new process efficient, easy and environmentally friendly.
文摘Catalytic hydrodeoxygenation(HDO)is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels,but highly challenging due to the lack of highly efficient nonprecious metal catalysts.Herein,we report for the first time of a facile synthetic approach to controllably fabricate well-defined Ni-Co alloy NPs confined on the tip of N-CNTs as HDO catalyst.The resultant Ni-Co alloy catalyst possesses outstanding HDO performance towards biomass-derived vanillin into 2-methoxy-4-methylphenol in water with 100%conversion efficiency and selectivity under mild reaction conditions,surpassing the reported high performance nonprecious HDO catalysts.Impressively,our experimental results also unveil that the Ni-Co alloy catalyst can be generically applied to catalyze HDO of vanillin derivatives and other aromatic aldehydes in water with 100%conversion efficiency and over 90%selectivity.Importantly,our DFT calculations and experimental results confirm that the achieved outstanding HDO catalytic performance is due to the greatly promoted selective adsorption and activation of C=O,and desorption of the activated hydrogen species by the synergism of the alloyed Ni-Co NPs.The findings of this work affords a new strategy to design and develop efficient transition metal-based catalysts for HDO reactions in water.
基金Supported by the National Natural Science Foundation of China(20976041)the Program for New Century Excellent Talents in University,the Natural Science Foundation of Hunan Province(10JJ1004)the Open Fund Project of Key Laboratory in Hunan University(09K095)
文摘This paper deals with the enantioseparation of phenylsuccinic acid(H2A)enantiomers by liquid-liquid reactive extraction usingβ-CD derivatives as aqueous selectors.Cyclodextrin and its derivatives can interact with guest molecules selectively to form complexes with different stabilities.Cyclodextrin derivatives are not soluble in organic liquids,but highly soluble in water.In this work,hydroxypropyl-β-cyclodextrin(HP-β-CD),hydroxyethyl- β-cyclodextrin(HE-β-CD)and methyl-β-cyclodextrin(Me-β-CD)were selected as chiral selectors in aqueous phase for the reactive extraction of phenylsuccinic acid enantiomers from organic phase to aqueous phase.The results show that the efficiency of the extraction depends,often strongly,on a number of process variables,including the types of organic solvents andβ-CD derivatives,the concentrations of the extractants and H2A enantiomers,pH and temperature.HP-β-CD,HE-β-CD and Me-β-CD have stronger recognition abilities for R-phenylsuccinic acid than for S-phenylsuccinic acid.Among the three kinds ofβ-CD derivatives,HP-β-CD has the strongest separation ability. Excellent enantioseparation was achieved under the optimal conditions of pH of 2.5 and temperature of 5°C with a maximum enantioselectivity(a)of 2.38.Reactive extraction of enantiomers with hydrophilicβ-CD derivatives is of strong chiral separation ability and can be hopeful for separations of various enantiomers at a large-scale.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.51572072 and 21402045)Wuhan Science and Technology Bureau of Hubei Province of China (No. 2013010602010209)+1 种基金Educational Commission of Hubei Province of China(No. D20141006)Department of Science & Technology of Hubei Province of China(No. 2015CFA118)
文摘An efficient solution-processable route employing Pb(Ac)2 as lead source and anti-solvent treatment to achieve fully covered and homogenous perovskite films is reported. The effect of different solution methods and device architectures on the morphologies of perovskite films were systematically investigated. Our results show that the planar perovskite layer fabricated by one-step solution method achieved fully covered and pinhole-free films. Further anti-solvent treatment using chlorobenzene (CB) promoted a perovskite film with highly smooth surfaces and enlarged grain sizes. Device fabricated from CB treated perovskite film achieved a best PCE of 15.80%, in comparison with 14.02%for the untreated device. These results evidently suggest a feasible route towards controlling the crystallization and morphology of planar heterojunction (PHJ) PSCs for improved efficiency.
