Chemically modified carbonaceous materials have attained utmost attention in the fields of renewable energy storage and conversion,due to the controllable physicochemical properties,tailorable micro-/nanostructures,an...Chemically modified carbonaceous materials have attained utmost attention in the fields of renewable energy storage and conversion,due to the controllable physicochemical properties,tailorable micro-/nanostructures,and respectable stability.Herein,P-doped mesoporous carbons were synthesized by using F127 as the soft template,organophosphonic acid as the P source and phenolic resin as the carbon source.Small amounts of iron species were introduced to act as a graphitization catalyst.The synthesized carbons exhibit the well-defined wormhole-like pore structure featuring high specific surface area and homogenously doped P heteroatoms.Notably,introducing iron species during the synthesis process can optimize the textural properties and the degree of graphitization of carbon materials.The doping amount of P has an important effect on the porous structure and the defect degree,which correspondingly influence the active sites and the oxygen reduction reaction(ORR)activity.The resultant material presents superior catalytic activity for the ORR,together with remarkably enhanced durability and methanol tolerance in comparison with the commercial Platinum catalyst,demonstrating the possibility for its use in electrode materials and electronic nanodevices for metal-air batteries and fuel cells.展开更多
A convenient,expeditious,and high-efficiency protocol for the transformation of alcohols into esters using a Co-modified N-doped mesoporous carbon material(Co-N/m-C)as the catalyst is proposed.The catalyst was prepa...A convenient,expeditious,and high-efficiency protocol for the transformation of alcohols into esters using a Co-modified N-doped mesoporous carbon material(Co-N/m-C)as the catalyst is proposed.The catalyst was prepared through direct pyrolysis of a macromolecular precursor.The catalyst prepared using a pyrolysis temperature of 900°C(labeled Co-N/m-C-900) exhibited the best per-formance.The strong coordination between the ultra-dispersed cobalt species and the pyridine nitrogen as well as the large area of the mesoporous surface resulted in a high turnover frequencymethyl benzoate.This value is much higher than those of state-of-the-art transition-metal-based nanocatalysts reported in the literature.Moreover,the catalyst exhibited general applicability to various structurally diverse alcohols,including benzylic,allylic,and heterocyclic alcohols,achieving the target esters in high yields.In addition,a preliminary evaluation revealed that Co-N/m-C-900 can be used six times without significant activity loss.In general,the process was rapid,simple,and cost-effective.展开更多
基金supported by the National Natural Science Foundation of China(21421001,21573115)~~
文摘Chemically modified carbonaceous materials have attained utmost attention in the fields of renewable energy storage and conversion,due to the controllable physicochemical properties,tailorable micro-/nanostructures,and respectable stability.Herein,P-doped mesoporous carbons were synthesized by using F127 as the soft template,organophosphonic acid as the P source and phenolic resin as the carbon source.Small amounts of iron species were introduced to act as a graphitization catalyst.The synthesized carbons exhibit the well-defined wormhole-like pore structure featuring high specific surface area and homogenously doped P heteroatoms.Notably,introducing iron species during the synthesis process can optimize the textural properties and the degree of graphitization of carbon materials.The doping amount of P has an important effect on the porous structure and the defect degree,which correspondingly influence the active sites and the oxygen reduction reaction(ORR)activity.The resultant material presents superior catalytic activity for the ORR,together with remarkably enhanced durability and methanol tolerance in comparison with the commercial Platinum catalyst,demonstrating the possibility for its use in electrode materials and electronic nanodevices for metal-air batteries and fuel cells.
基金supported by the National Natural Science Foundation of China (21773232, 21403219, 21773227)~~
文摘A convenient,expeditious,and high-efficiency protocol for the transformation of alcohols into esters using a Co-modified N-doped mesoporous carbon material(Co-N/m-C)as the catalyst is proposed.The catalyst was prepared through direct pyrolysis of a macromolecular precursor.The catalyst prepared using a pyrolysis temperature of 900°C(labeled Co-N/m-C-900) exhibited the best per-formance.The strong coordination between the ultra-dispersed cobalt species and the pyridine nitrogen as well as the large area of the mesoporous surface resulted in a high turnover frequencymethyl benzoate.This value is much higher than those of state-of-the-art transition-metal-based nanocatalysts reported in the literature.Moreover,the catalyst exhibited general applicability to various structurally diverse alcohols,including benzylic,allylic,and heterocyclic alcohols,achieving the target esters in high yields.In addition,a preliminary evaluation revealed that Co-N/m-C-900 can be used six times without significant activity loss.In general,the process was rapid,simple,and cost-effective.