96-26-4Relevant articles and documents
One-pot biotransformation of glycerol into serinol catalysed by biocatalytic composites made of whole cells and immobilised enzymes
Ripoll, Magdalena,Velasco-Lozano, Susana,Jackson, Erienne,Diamanti, Eleftheria,Betancor, Lorena,López-Gallego, Fernando
supporting information, p. 1140 - 1146 (2021/02/26)
Biocatalytic cascades afford the development of economically sustainable and green processes. Herein we examined the unprecedented coupling of co-immobilisedGluconobacter oxydansand an isolated transaminase to synthesise serinol from glycerol. Through this approach, we manufactured up to 36 mM serinol, the highest titer ever reported for a non-fermentative biosynthesis. More importantly, similar productivities are obtained starting from the industrial by-product crude glycerol, demonstrating the possibilities of this hybrid heterogenenous biocatalyst for valorising bio-based raw materials.
Assembly of platinum nanoparticles and single-atom bismuth for selective oxidation of glycerol
Huang, Ning,Jiang, Dong,Jiang, Pingping,Leng, Yan,Lu, Yubing,Tian, Jinshu,Yue, Chenguang,Zhang, Pingbo,Zhang, Zihao
supporting information, p. 25576 - 25584 (2021/12/07)
Selective oxidation of the secondary hydroxyl group of glycerol to dihydroxyacetone (DHA) is an extremely challenging yet important reaction. The main difficulty is that the three hydroxyl groups in glycerol are prone to randomly oxidize, resulting in an unsatisfactory DHA selectivity. We show here that an assembly of platinum nanoparticles (NPs, ～2 nm) and N-stabilized single-atom bismuth (Bi), namely Pt/Bi@NC, shows a record-high DHA selectivity of ～95.0% towards glycerol oxidation under optimized reaction conditions. Characterization and theoretical calculations confirm that single-atom Bi in the vicinity of Pt NPs provides a preferred site to chelate with the primary -OH of glycerol, and its secondary -OH is prone to bind to a surface Pt atom of a Pt NP with a shorter Pt-H bond length. This as-formed unique adsorption configuration of glycerol on the Pt-Bi dual site significantly facilitates the oxidation of the secondary -OH of glycerol, thus contributing to a record-high selectivity to DHA. This journal is
Enantioselective Reductive Oligomerization of Carbon Dioxide into l-Erythrulose via a Chemoenzymatic Catalysis
Bontemps, Sébastien,Clapés, Pere,Desmons, Sarah,Dumon, Claire,Fauré, Régis,Grayson-Steel, Katie,Hurtado, John,Nu?ez-Dallos, Nelson,Vendier, Laure
supporting information, p. 16274 - 16283 (2021/10/12)
A cell-free enantioselective transformation of the carbon atom of CO2has never been reported. In the urgent context of transforming CO2into products of high value, the enantiocontrolled synthesis of chiral compounds from CO2would be highly desirable. Using an original hybrid chemoenzymatic catalytic process, we report herein the reductive oligomerization of CO2into C3(dihydroxyacetone, DHA) and C4(l-erythrulose) carbohydrates, with perfect enantioselectivity of the latter chiral product. This was achieved with the key intermediacy of formaldehyde. CO2is first reduced selectively by 4e-by an iron-catalyzed hydroboration reaction, leading to the isolation and complete characterization of a new bis(boryl)acetal compound derived from dimesitylborane. In an aqueous buffer solution at 30 °C, this compound readily releases formaldehyde, which is then involved in selective enzymatic transformations, giving rise either (i) to DHA using a formolase (FLS) catalysis or (ii) to l-erythrulose with a cascade reaction combining FLS and d-fructose-6-phosphate aldolase (FSA) A129S variant. Finally, the nature of the synthesized products is noteworthy, since carbohydrates are of high interest for the chemical and pharmaceutical industries. The present results prove that the cell-freede novosynthesis of carbohydrates from CO2as a sustainable carbon source is a possible alternative pathway in addition to the intensely studied biomass extraction andde novosyntheses from fossil resources.
