We previously functionally characterized a novel marine microbial GDSL lipase MT6 and identified that the stereo-selectivity of MT6 was opposite to that of other common lipases in trans-esterification reactions.Herein...We previously functionally characterized a novel marine microbial GDSL lipase MT6 and identified that the stereo-selectivity of MT6 was opposite to that of other common lipases in trans-esterification reactions.Herein,we have investigated the use of MT6 in stereo-selective biocatalysis through direct hydrolysis reactions.Notably,the stereo-selectivity of MT6 was also demonstrated to be opposite to that of other common lipases in hydrolysis reactions.Parameters,including temperature,organic co-solvents,pH,ionic strength,catalyst loading,substrate concentration,and reaction time,affecting the enzymatic resolution of racemic 1-phenylethyl acetate were further investigated,with the e.e.of the final(S)-l-Phenylethanol product and the conversion being 97%and 28.5%,respectively,after process optimization.The lengths of side chains of 1-phenylethyl esters greatly affected the stereo-selectivity and conversion during kinetic resolutions.MT6 is a novel marine microbial GDSL lipase exhibiting opposite stereo-selectivities than other common lipases in both trans-esterification reactions and hydrolysis reactions.展开更多
In this work,a novel alcohol alkali hydrolysis method was explored for the preparation of terephthalic acid(TPA)from waste polyethylene terephthalate(PET).First,a series of single factor experiments on the depolymeriz...In this work,a novel alcohol alkali hydrolysis method was explored for the preparation of terephthalic acid(TPA)from waste polyethylene terephthalate(PET).First,a series of single factor experiments on the depolymerization rate of waste PET bottles and the yield of TPA were conducted to determine the optimized experimental conditions,in terms of reaction time,reaction temperature,dosage of ethylene glycol and sodium bicarbonate,amount of distilled water and stirring rate.Then IR spectra and elemental analysis were carried out for the characterization of obtained product.Under optimal experimental conditions,over 98%PET can be depolymerized into the target product(TPA)and the purity and yield of TPA are over 97%and 94%,respectively.Both the experimental and analytical results support a feasible process for the preparation of TPA from waste PET.It is expected that this alcohol alkali hydrolysis method can promise an effective way for the sustainable recycling of waste PET.展开更多
The selective oxidation of alcohol using molecular oxygen as an oxidant and water as a green sol‐vent is of great interest in green chemistry. In this work, we present a systematic study of a Pt/ZnO catalyst for the ...The selective oxidation of alcohol using molecular oxygen as an oxidant and water as a green sol‐vent is of great interest in green chemistry. In this work, we present a systematic study of a Pt/ZnO catalyst for the selective oxidation of benzyl alcohol at room temperature under base‐free aqueous conditions. Experimental observations and density functional theory calculations suggest that ZnO as a support can facilitate the adsorption of benzyl alcohol, which subsequently reacts with the activated oxygen species on the Pt catalyst, producing benzaldehyde. The resulting solid achieves a high conversion(94.1 ± 5.1% in 10 h) of benzyl alcohol and nearly 100% selectivity to benzalde‐hyde with ambient air as the oxidant. In addition, by introducing a small amount of Bi(1.78 wt%) into Pt/ZnO, we can further enhance the activity by 350%.展开更多
In an equilibrium vessel,the solid-liquid equilibria(SLE) for three binary mixtures of phenyl salicylate with 1-butanol,2-butanol,and 2-methyl-1-propanol,respectively,have been measured from 283.15 K to the melting te...In an equilibrium vessel,the solid-liquid equilibria(SLE) for three binary mixtures of phenyl salicylate with 1-butanol,2-butanol,and 2-methyl-1-propanol,respectively,have been measured from 283.15 K to the melting temperature of the solute using a method in which an excess amount of solute was equilibrated with the alcohol solution.The liquid concentrations of the investigated phenyl salicylate in the saturated solution were analyzed by UV spectrometry.Activity coefficients for phenyl salicylate have been calculated by means of the Wilson,NRTL,and UNIQUAC equations and with them were correlated solubility data that were compared with the experimental ones.The best correlation of the solubility data has been obtained by the Wilson equation by which the average root-mean-square deviation of temperature for the three systems is 1.03 K.展开更多
Affinity membranes are fabricated for boric acid removal by the surface functionalization of microporous polypropylene membrane(MPPM)with lactose-based polyols.The affinity is based on specific complexation between bo...Affinity membranes are fabricated for boric acid removal by the surface functionalization of microporous polypropylene membrane(MPPM)with lactose-based polyols.The affinity is based on specific complexation between boric acid and saccharide polyols.A photoinduced grafting-chemical reaction sequence was used to prepare these affinity membranes.Poly(2-aminoethyl methacrylate hydrochloride)[poly(AEMA)]was grafted on the surfaces of MPPM by UV-induced graft polymerization.Grafting in the membrane pores was visualized by dying the cross-section of poly(AEMA)-grafted MPPM with fluorescein disodium and imaging with confocal laser scanning microscopy.It is concluded that lactose ligands can be covalently immobilized on the external surface and in the pores by the subsequent coupling of poly(AEMA)with lactobionic acid(LA).Physical and chemical properties of the affinity membranes were characterized by field emission scanning electron microscopy and Fourier Transform Infrared/Attenuated Total Refraction spectroscopy(FT-IR/ATR).3-Aminophenyl boric acid(3-APBA)was removed from aqueous solution by a single piece of lactose-functionalized MPPM in a dynamic filtration system.The results show that the 3-APBA removal reaches an optimal efficiency(39.5%)under the alkaline condition(pH9.1),which can be improved by increasing the immobilization density of LA.Regeneration of these affinity membranes can be easily realized through acid-base washing because the complexation of boric acid and saccharide polyol is reversible.展开更多
In this paper, the analysis of the environmental impacts of a biopolymer based on starch is presented. These impacts were calculated from a cradle to gate LCA (Life Cycle Assessment), based on UNEEN ISO 14040:2006 ...In this paper, the analysis of the environmental impacts of a biopolymer based on starch is presented. These impacts were calculated from a cradle to gate LCA (Life Cycle Assessment), based on UNEEN ISO 14040:2006 and UNEEN ISO 14044, using as functional unit 1 kg of produced biomaterial. The impact categories analyzed were global wanning, ozone depletion, acidification and eutrophication. The results indicate that the electricity causes the highest impacts in the global warming and ozone depletion categories, but compared to synthetic polymers, the emissions are low. Finally, in the case of eutrophication, the impacts are similar to other biopolymers but higher in comparison with petroleum-based polymers like HDPE (High Density Polyethylene), LDPE (Low Density Polyethylene), PP (Polypropylene), PS (Polystyrene) and PET (Polyethylene Terephthalate).展开更多
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(XDA11030404),the Key Project from Chinese Academy of Sciences(KGZD-EW-606)the National Natural Science Foundation of China(21302199)Guangzhou Science and Technology Plan Projects(201510010012)
文摘We previously functionally characterized a novel marine microbial GDSL lipase MT6 and identified that the stereo-selectivity of MT6 was opposite to that of other common lipases in trans-esterification reactions.Herein,we have investigated the use of MT6 in stereo-selective biocatalysis through direct hydrolysis reactions.Notably,the stereo-selectivity of MT6 was also demonstrated to be opposite to that of other common lipases in hydrolysis reactions.Parameters,including temperature,organic co-solvents,pH,ionic strength,catalyst loading,substrate concentration,and reaction time,affecting the enzymatic resolution of racemic 1-phenylethyl acetate were further investigated,with the e.e.of the final(S)-l-Phenylethanol product and the conversion being 97%and 28.5%,respectively,after process optimization.The lengths of side chains of 1-phenylethyl esters greatly affected the stereo-selectivity and conversion during kinetic resolutions.MT6 is a novel marine microbial GDSL lipase exhibiting opposite stereo-selectivities than other common lipases in both trans-esterification reactions and hydrolysis reactions.
基金Project(2016TP1007)supported by the Hunan Provincial Science and Technology Plan,China
文摘In this work,a novel alcohol alkali hydrolysis method was explored for the preparation of terephthalic acid(TPA)from waste polyethylene terephthalate(PET).First,a series of single factor experiments on the depolymerization rate of waste PET bottles and the yield of TPA were conducted to determine the optimized experimental conditions,in terms of reaction time,reaction temperature,dosage of ethylene glycol and sodium bicarbonate,amount of distilled water and stirring rate.Then IR spectra and elemental analysis were carried out for the characterization of obtained product.Under optimal experimental conditions,over 98%PET can be depolymerized into the target product(TPA)and the purity and yield of TPA are over 97%and 94%,respectively.Both the experimental and analytical results support a feasible process for the preparation of TPA from waste PET.It is expected that this alcohol alkali hydrolysis method can promise an effective way for the sustainable recycling of waste PET.
基金supported by the National Natural Science Foundation of China (21703050, 21271153, 21373181)China Postdoctoral Science Foun‐dation (512200‐X91701)Special Research Foundation of Young Teachers in Hangzhou Dianzi University (ZX150204307002/032)~~
文摘The selective oxidation of alcohol using molecular oxygen as an oxidant and water as a green sol‐vent is of great interest in green chemistry. In this work, we present a systematic study of a Pt/ZnO catalyst for the selective oxidation of benzyl alcohol at room temperature under base‐free aqueous conditions. Experimental observations and density functional theory calculations suggest that ZnO as a support can facilitate the adsorption of benzyl alcohol, which subsequently reacts with the activated oxygen species on the Pt catalyst, producing benzaldehyde. The resulting solid achieves a high conversion(94.1 ± 5.1% in 10 h) of benzyl alcohol and nearly 100% selectivity to benzalde‐hyde with ambient air as the oxidant. In addition, by introducing a small amount of Bi(1.78 wt%) into Pt/ZnO, we can further enhance the activity by 350%.
文摘In an equilibrium vessel,the solid-liquid equilibria(SLE) for three binary mixtures of phenyl salicylate with 1-butanol,2-butanol,and 2-methyl-1-propanol,respectively,have been measured from 283.15 K to the melting temperature of the solute using a method in which an excess amount of solute was equilibrated with the alcohol solution.The liquid concentrations of the investigated phenyl salicylate in the saturated solution were analyzed by UV spectrometry.Activity coefficients for phenyl salicylate have been calculated by means of the Wilson,NRTL,and UNIQUAC equations and with them were correlated solubility data that were compared with the experimental ones.The best correlation of the solubility data has been obtained by the Wilson equation by which the average root-mean-square deviation of temperature for the three systems is 1.03 K.
基金Supported by the National Natural Science Foundation of China(50933006)the National Basic Research Program of China(2009CB623401)
文摘Affinity membranes are fabricated for boric acid removal by the surface functionalization of microporous polypropylene membrane(MPPM)with lactose-based polyols.The affinity is based on specific complexation between boric acid and saccharide polyols.A photoinduced grafting-chemical reaction sequence was used to prepare these affinity membranes.Poly(2-aminoethyl methacrylate hydrochloride)[poly(AEMA)]was grafted on the surfaces of MPPM by UV-induced graft polymerization.Grafting in the membrane pores was visualized by dying the cross-section of poly(AEMA)-grafted MPPM with fluorescein disodium and imaging with confocal laser scanning microscopy.It is concluded that lactose ligands can be covalently immobilized on the external surface and in the pores by the subsequent coupling of poly(AEMA)with lactobionic acid(LA).Physical and chemical properties of the affinity membranes were characterized by field emission scanning electron microscopy and Fourier Transform Infrared/Attenuated Total Refraction spectroscopy(FT-IR/ATR).3-Aminophenyl boric acid(3-APBA)was removed from aqueous solution by a single piece of lactose-functionalized MPPM in a dynamic filtration system.The results show that the 3-APBA removal reaches an optimal efficiency(39.5%)under the alkaline condition(pH9.1),which can be improved by increasing the immobilization density of LA.Regeneration of these affinity membranes can be easily realized through acid-base washing because the complexation of boric acid and saccharide polyol is reversible.
文摘In this paper, the analysis of the environmental impacts of a biopolymer based on starch is presented. These impacts were calculated from a cradle to gate LCA (Life Cycle Assessment), based on UNEEN ISO 14040:2006 and UNEEN ISO 14044, using as functional unit 1 kg of produced biomaterial. The impact categories analyzed were global wanning, ozone depletion, acidification and eutrophication. The results indicate that the electricity causes the highest impacts in the global warming and ozone depletion categories, but compared to synthetic polymers, the emissions are low. Finally, in the case of eutrophication, the impacts are similar to other biopolymers but higher in comparison with petroleum-based polymers like HDPE (High Density Polyethylene), LDPE (Low Density Polyethylene), PP (Polypropylene), PS (Polystyrene) and PET (Polyethylene Terephthalate).