Activated carbon-supported HgCl2 catalysts have seriously impeded the development of the polyvinyl chloride(PVC)industry due to the sublimation of Hg species and environmental pollution problems.Herein,the template-fr...Activated carbon-supported HgCl2 catalysts have seriously impeded the development of the polyvinyl chloride(PVC)industry due to the sublimation of Hg species and environmental pollution problems.Herein,the template-free and organic solvent-free strategy was devised to synthesize non-metallic based nitrogen-doped carbon(U-NC)sphere catalyst for acetylene hydrochlorination.This green strategy via ultrasonic chemistry initiates resin crosslinking reactions between aminophenol and formaldehyde resin by free radicals,leading to the ultra-rapid formation of U-NC with remarkably high pyrrolic N content in only 5 min.This U-NC catalyst exhibited an outstanding space-time-yield(1.6 gVCM·gcat^(−1)·h^(−1)),even comparable to the reported metallic catalyst.By combining kinetic analysis,advanced characterizations,density functional theory,it is found that the amount of pyrrolic N is in linear with C_(2)H_(2)conversion,pyrrolic N in U-NC can effectively improve acetylene hydrochlorination performance by mediating HCl adsorption.This work sheds new light on rationally constructing metal-free catalyst for acetylene hydrochlorination.展开更多
基金the National Natural Science Foundation of China(No.21978325)Innovation Research Projects(Nos.20CX06072A,20CX06095A,and 20CX06096A)+1 种基金the Natural Science Foundation of Shandong Province(Nos.ZR2020KB006 and ZR2020YQ17)the Science and Technology Project of Xinjiang Bingtuan Supported by Central Government(No.2022BC001).
文摘Activated carbon-supported HgCl2 catalysts have seriously impeded the development of the polyvinyl chloride(PVC)industry due to the sublimation of Hg species and environmental pollution problems.Herein,the template-free and organic solvent-free strategy was devised to synthesize non-metallic based nitrogen-doped carbon(U-NC)sphere catalyst for acetylene hydrochlorination.This green strategy via ultrasonic chemistry initiates resin crosslinking reactions between aminophenol and formaldehyde resin by free radicals,leading to the ultra-rapid formation of U-NC with remarkably high pyrrolic N content in only 5 min.This U-NC catalyst exhibited an outstanding space-time-yield(1.6 gVCM·gcat^(−1)·h^(−1)),even comparable to the reported metallic catalyst.By combining kinetic analysis,advanced characterizations,density functional theory,it is found that the amount of pyrrolic N is in linear with C_(2)H_(2)conversion,pyrrolic N in U-NC can effectively improve acetylene hydrochlorination performance by mediating HCl adsorption.This work sheds new light on rationally constructing metal-free catalyst for acetylene hydrochlorination.
