Cu,N codoped carbon nanosheets encapsulating ultrasmall Cu nanoparticles for enhancing selective 1,2-propanediol oxidation  

作　　者：Yonghai Feng Min Yu Minjia Meng Lei Liu Dewei Rao 

机构地区：[1]Institute for Advanced Materials,School of Materials Science and Engineering,Jiangsu University,Zhenjiang 212013,Jiangsu,China [2]School of Chemistry and Chemical Engineering,Jiangsu University,Zhenjiang 212013,Jiangsu,China

出　　处：《Journal of Energy Chemistry》2024年第4期27-35,共9页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(32371407,82160421);the Natural Science Foundation of Jiangsu Province(BK20211322)。

摘　　要：In the selective oxidation of biomass-based 1,2-propanediol(PDO)with oxygen as the terminal oxidant,it is challenging to improve the lactic acid(LA)selectivity for nonnoble metal nanoparticles(NPs)due to their limited oxygen reduction rate and easy C-C cleavage.Given the high economic feasibility of nonnoble metals,i.e.,Cu,in this work,copper and nitrogen codoped porous carbon nanosheets encapsulating ultrafine Cu nanoparticles(Cu@Cu-N-C)were developed to realize highly selective of PDO oxidation to LA.The carbon-encapsulated ultrasmall Cu^(0)NPs in Cu@Cu-N-C have high PDO dehydrogenation activity while N-coordinated Cu(Cu-N)sites are responsible for the high oxygen reduction efficacy.Therefore,the performance of catalytic PDO conversion to LA is optimized by a proposed pathway of PDO→hydroxylacetone→lactaldehyde→LA.Specifically,the enhanced LA selectivity is 88.5%,and the PDO conversion is up to 75.1%in an O_(2)-pressurized reaction system(1.0 MPa O_(2)),superior to other Cu-based catalysts,while in a milder nonpressurized system(O_(2)flow rate of 100 mL min-1),a remarkable LA selectivity(94.2%)is obtained with 39.8%PDO conversion,2.2 times higher than that of supported Au nanoparticles(1%Au/C).Moreover,carbon encapsulation offers Cu@Cu-N-C with strong leaching resistance for better recycling.

关 键 词：Selective oxidation Copper and nitrogen doped carbon 1 2-PROPANEDIOL Ultrasmall Cu nanoparticles Lactic acid 

分 类 号：TQ225.4[化学工程—有机化工] O643.36[理学—物理化学] TB383.1[理学—化学]