Microporous heteropolyoxometalates Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\}/SiO\-2 were synthesized by a sol\|gel technique and characterized by IR, UV\|Vis, BET adsorption/desorption isotherm. The structural fr...Microporous heteropolyoxometalates Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\}/SiO\-2 were synthesized by a sol\|gel technique and characterized by IR, UV\|Vis, BET adsorption/desorption isotherm. The structural frameworks of Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\} are preserved within the silica networks. Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\}/SiO\-2 are a kind of polyoxometalate\|silica gel hybrids with uniform micropores of ca. 0.65 nm. They show a high catalytic activity for oxidation reaction of benzyl alcohol by H\-2O\-2(30%) in liquid\|solid systems and product selectivity for benzaldehyde(>96%). The highest activity is observed at \%x\%=2.5 in Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\}/SiO\-2 and little formation of benzoic acid and a more deeply oxidized product is observed.展开更多
Benzyl and phenylpropanoid acids are widely used in organic synthesis of fine chemicals,such as pharmaceuticals and condiments.However,biocatalysis of these acids has received less attention than chemical synthesis.On...Benzyl and phenylpropanoid acids are widely used in organic synthesis of fine chemicals,such as pharmaceuticals and condiments.However,biocatalysis of these acids has received less attention than chemical synthesis.One of the main challenges for biological production is the limited availability of alcohol dehydrogenases and aldehyde dehydrogenases.Environmental microorganisms are potential sources of these enzymes.In this study,129 alcohol dehydrogenases and 42 aldehyde dehydrogenases from Corynebacterium glutamicum,Pseudomonas aeruginosa,and Bacillus subtilis were identified and explored with various benzyl and phenylpropanoid alcohol and aldehyde substrates,among which four alcohol dehydrogenases and four aldehyde dehydrogenases with broad substrate specificity and high catalytic activity were obtained.Moreover,a cascade whole-cell catalytic system including ADH-90,ALDH-40,and the NAD(P)H oxidase LreNox was established,which showed high efficiency in converting cinnamyl alcohol and p-methylbenzyl alcohol into the respective carboxylic acids.Remarkably,this biocatalytic system can be easily scaled up to gram-level production,facilitating preparation purposes.展开更多
文摘Microporous heteropolyoxometalates Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\}/SiO\-2 were synthesized by a sol\|gel technique and characterized by IR, UV\|Vis, BET adsorption/desorption isotherm. The structural frameworks of Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\} are preserved within the silica networks. Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\}/SiO\-2 are a kind of polyoxometalate\|silica gel hybrids with uniform micropores of ca. 0.65 nm. They show a high catalytic activity for oxidation reaction of benzyl alcohol by H\-2O\-2(30%) in liquid\|solid systems and product selectivity for benzaldehyde(>96%). The highest activity is observed at \%x\%=2.5 in Cs\-\%x\%H\-\{5-\%x\%\}PW\-\{10\}V\-2O\-\{40\}/SiO\-2 and little formation of benzoic acid and a more deeply oxidized product is observed.
基金This work was supported by the National Key Research and Development Program of China(2021YFA0911500)the National Natural Science Foundation of China(32071266,32170088,and 32370032)+1 种基金the Shandong Provincial Natural Science Foundation(ZR2020ZD23)the State Key Laboratory of Microbial Technology Open Projects Fund(M2022-01).
文摘Benzyl and phenylpropanoid acids are widely used in organic synthesis of fine chemicals,such as pharmaceuticals and condiments.However,biocatalysis of these acids has received less attention than chemical synthesis.One of the main challenges for biological production is the limited availability of alcohol dehydrogenases and aldehyde dehydrogenases.Environmental microorganisms are potential sources of these enzymes.In this study,129 alcohol dehydrogenases and 42 aldehyde dehydrogenases from Corynebacterium glutamicum,Pseudomonas aeruginosa,and Bacillus subtilis were identified and explored with various benzyl and phenylpropanoid alcohol and aldehyde substrates,among which four alcohol dehydrogenases and four aldehyde dehydrogenases with broad substrate specificity and high catalytic activity were obtained.Moreover,a cascade whole-cell catalytic system including ADH-90,ALDH-40,and the NAD(P)H oxidase LreNox was established,which showed high efficiency in converting cinnamyl alcohol and p-methylbenzyl alcohol into the respective carboxylic acids.Remarkably,this biocatalytic system can be easily scaled up to gram-level production,facilitating preparation purposes.
基金Project supported by the Sichuan Youth Science&Technology Foundation(No.2017JQ0010)the National High Technology Research&Development Program(No.2016ZX05053)+1 种基金the Key Fund Project of Educational Commission of Sichuan Province(No.16CZ0008)the Explorative Project Fund of the State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation(Southwest Petroleum University)(No.G201601)~~
