Recently,Zhang Tao,an academician of the CAS Member and a researcher of the Dalian Institute of Chemical Physics of the Chinese Academy of Sciences,and Wang Aiqin,a researcher,have made progress in the research of monoatomic catalytic ethylene carboxymethyl esterification.
The ethylene carboxymethyl esterification reaction(the reaction of ethylene,CO,and methanol to produce methyl propionate)is an important pathway for the industrial preparation of methyl methacrylate.Compared with traditional methods such as acetone cyanide and isobutene oxidation,this method has the advantages of wide raw material sources,high atomic economy,and high selectivity.At present,palladium phosphine complexes are still widely used as catalysts in this reaction,and strong acids such as sulfuric acid and methanesulfonic acid are used as adjuvants,resulting in difficulties in catalyst separation and equipment corrosion.
Single atom catalysts,as a special type of single core multiphase catalysts without organic ligands,are expected to bring new opportunities for traditional homogeneous catalytic carbonylation reactions.In this work,the research team developed a Pt1/MoS2 single atom catalyst supported on MoS2 nanosheets,in which Pt single atoms and neighboring coordination unsaturated Mo atoms form the Mo-S-Pt-S-Mo structure.Thanks to the synergistic effect of Pt single atom and carrier,Pt1/MoS2 can catalyze ethylene carboxylation without the addition of acid additives,with a TOF value of 320h-1,comparable to homogeneous catalysts.Moreover,it has excellent selectivity and recycling performance,with a selectivity of 91%under reaction conditions with a TOF value of 150h-1.After 4 cycles of use,the TOF value remains at 90h-1,without metal loss.This work provides new ideas for promoting the multiphase reaction of olefin carboxylation.
Since the concept of"single atom catalysis"was first proposed in 2011,the team has been committed to research related to single atom catalysis,and has made a series of progress in coordination environment regulation,single atom catalytic specific reactions,and dynamic evolution of active sites.
The relevant research results were published in the Journal of the American Chemical Society,titled Ethylene Methodology over Heterogeneous Pt1/MoS2 Single Atom Catalyst:Metal Support Certified Catalyst.The research work was supported by the National Key Research and Development Program,the National Natural Science Foundation of China,and the Chinese Academy of Sciences Youth Team Program for Stable Support in Basic Research.
Paper link
Dalian Chemical Institute utilizes a single atom catalyst and carrier synergistic mechanism to achieve ethylene carboxymethyl esterification
