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
Current bio-ethanol production entails the enzymatic depolymerization of cellulose,but this process shows low efficiency and poor economy.In this work,we developed a consecutive aqueous hydrogenolysis process for the ...Current bio-ethanol production entails the enzymatic depolymerization of cellulose,but this process shows low efficiency and poor economy.In this work,we developed a consecutive aqueous hydrogenolysis process for the conversion of corn-stalk cellulose to produce a relatively high concentration of bio-ethanol(6.1 wt%)without humin formation.A high yield of cellulose(ca.50 wt%)is extracted from corn stalk using a green solvent(80 wt%1,4-butanediol)without destroying the structure of the lignin.The first hydrothermal hydrogenolysis step uses a Ni–WO_(x)/SiO_(2)catalyst to convert the high cumulative concentration of cellulose(30 wt%)into a polyol mixture with a 56.5 C%yield of ethylene glycol(EG).The original polyol mixture is then subjected to subsequent selective aqueous-phase hydrogenolysis of the C–O bond to produce bioethanol(75%conversion,84 C%selectivity)over the modified hydrothermally stable Cu catalysts.The added Ni component favors the good dispersion of Cu nanoparticles,and the incorporated Au3+helps to stabilize the active Cu^(0)-Cu^(+)species.This multi-functional catalytic process provides an economically competitive route for the production of cellulosic ethanol from raw lignocellulose.展开更多
The reactor unit for one-stage technology for production of concentrated ethylene glycol-water solutions is described.Such solutions could be useful for production of automotive antifreezes. The technology is based on...The reactor unit for one-stage technology for production of concentrated ethylene glycol-water solutions is described.Such solutions could be useful for production of automotive antifreezes. The technology is based on the highly selective hydration ofethylene oxide in the presence of heterogeneous catalyst-anion-exchange resin in HCO3-/CO/3/2-_form. The mathematical model of reactor allowed evaluating of economical benefit in comparison with conventional method.展开更多
Ethanol-water near-azeotropic mixture dehydration was investigated by formulated compound starchbased adsorbent(CSA), which consists of corn, sweet potato and foaming agent. The net retention time and separation facto...Ethanol-water near-azeotropic mixture dehydration was investigated by formulated compound starchbased adsorbent(CSA), which consists of corn, sweet potato and foaming agent. The net retention time and separation factor of water over ethanol were measured by inverse gas chromatography(IGC). Results indicated that water has a longer net retention time than ethanol and that low temperature is beneficial to this dehydration process. Orthogonal test was conducted under different vapor feed flow rates, bed temperatures and bed heights, to obtain optimal fixed-bed dehydration condition. Dynamic saturated adsorbance was also studied. It was found that CSA has the same water adsorption capacity(0.15 g/g)as some commercial molecular sieves. Besides, this biosorptive dehydration process was found to be the most energy-efficient compared with other ethanol purification processes.展开更多
Phase separation behavior of cocamidopropyl betaine/water/polyethylene glycol （PEG） system was studied. The effects of concentration and molecular weight of PEG on the phase separation behavior were investigated. Cl...Phase separation behavior of cocamidopropyl betaine/water/polyethylene glycol （PEG） system was studied. The effects of concentration and molecular weight of PEG on the phase separation behavior were investigated. Clouding occurred when the concentration of PEG was large enough in the betaine aqueous solution, and the concentration of PEG at cloud point decreased with the increase of PEG molecular weight for a constant betaine concentration. The bottom phase was the PEG-rich phase, and the upper phase was the betaine-rich phase. The volumetric ratio of PEG-rich phase to betaine-rich phase, at the same difference between the PEG concentration and the one at the cloud poim, △Ccp （0.1 g.ml^-1）, decreased as the PEG molecular weight increased and approached 1 for higher PEG molecular Weiglai （about 20000）, which was similar to the typicai-aqueous two-phase system. This volumetric ratio depended on the initial PEG concentration, but independent of PEG molecular weight. The concentration ratio of betaine to PEG in both phases depended on the △Ccp independent of PEG molecular weight.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.
文摘Current bio-ethanol production entails the enzymatic depolymerization of cellulose,but this process shows low efficiency and poor economy.In this work,we developed a consecutive aqueous hydrogenolysis process for the conversion of corn-stalk cellulose to produce a relatively high concentration of bio-ethanol(6.1 wt%)without humin formation.A high yield of cellulose(ca.50 wt%)is extracted from corn stalk using a green solvent(80 wt%1,4-butanediol)without destroying the structure of the lignin.The first hydrothermal hydrogenolysis step uses a Ni–WO_(x)/SiO_(2)catalyst to convert the high cumulative concentration of cellulose(30 wt%)into a polyol mixture with a 56.5 C%yield of ethylene glycol(EG).The original polyol mixture is then subjected to subsequent selective aqueous-phase hydrogenolysis of the C–O bond to produce bioethanol(75%conversion,84 C%selectivity)over the modified hydrothermally stable Cu catalysts.The added Ni component favors the good dispersion of Cu nanoparticles,and the incorporated Au3+helps to stabilize the active Cu^(0)-Cu^(+)species.This multi-functional catalytic process provides an economically competitive route for the production of cellulosic ethanol from raw lignocellulose.
文摘The reactor unit for one-stage technology for production of concentrated ethylene glycol-water solutions is described.Such solutions could be useful for production of automotive antifreezes. The technology is based on the highly selective hydration ofethylene oxide in the presence of heterogeneous catalyst-anion-exchange resin in HCO3-/CO/3/2-_form. The mathematical model of reactor allowed evaluating of economical benefit in comparison with conventional method.
基金Supported by the Independent Innovation Foundation of Tianjin University(No.2010XY-0013)
文摘Ethanol-water near-azeotropic mixture dehydration was investigated by formulated compound starchbased adsorbent(CSA), which consists of corn, sweet potato and foaming agent. The net retention time and separation factor of water over ethanol were measured by inverse gas chromatography(IGC). Results indicated that water has a longer net retention time than ethanol and that low temperature is beneficial to this dehydration process. Orthogonal test was conducted under different vapor feed flow rates, bed temperatures and bed heights, to obtain optimal fixed-bed dehydration condition. Dynamic saturated adsorbance was also studied. It was found that CSA has the same water adsorption capacity(0.15 g/g)as some commercial molecular sieves. Besides, this biosorptive dehydration process was found to be the most energy-efficient compared with other ethanol purification processes.
基金Supported by the National Natural Science Foundation of China （20676069）.
文摘Phase separation behavior of cocamidopropyl betaine/water/polyethylene glycol （PEG） system was studied. The effects of concentration and molecular weight of PEG on the phase separation behavior were investigated. Clouding occurred when the concentration of PEG was large enough in the betaine aqueous solution, and the concentration of PEG at cloud point decreased with the increase of PEG molecular weight for a constant betaine concentration. The bottom phase was the PEG-rich phase, and the upper phase was the betaine-rich phase. The volumetric ratio of PEG-rich phase to betaine-rich phase, at the same difference between the PEG concentration and the one at the cloud poim, △Ccp （0.1 g.ml^-1）, decreased as the PEG molecular weight increased and approached 1 for higher PEG molecular Weiglai （about 20000）, which was similar to the typicai-aqueous two-phase system. This volumetric ratio depended on the initial PEG concentration, but independent of PEG molecular weight. The concentration ratio of betaine to PEG in both phases depended on the △Ccp independent of PEG molecular weight.
