The improvement of catalysts’stability under harsh reaction conditions is vital for their practical applica-bility.Herein,iron carbide(Fe_(3)C)nanoparticles were encapsulated in graphitic carbon in situ and a carbon ...The improvement of catalysts’stability under harsh reaction conditions is vital for their practical applica-bility.Herein,iron carbide(Fe_(3)C)nanoparticles were encapsulated in graphitic carbon in situ and a carbon ball served as the carrier.The synthesized Fe_(3)C@C/C was first utilized to treat an m-cresol wastewater containing Si via catalytic ozonation.Compared with the commercial Fe/Al_(2)O_(3)catalyst,the resistance to Si of the Fe_(3)C@C/C was improved 22.68 times,while the TOC removal rate increased by a factor of 2.9,and it remained stable during 10 cycles and 12000 min of continuous reaction,which further demon-strated its potential for diverse applications.The catalyst exhibits improved resistance to Si because of the dual protection from the carbon-encapsulated structure and carbon carrier.Density functional theory calculations show that the encapsulation of Fe_(3)C using carbon significantly increases the resistance to adsorption of Si on its active sites.In addition,the activation of O_(3)is unimpeded on the Fe_(3)C adsorption sites by the protection from C,thus the generation of reactive oxygen species(ROS)by ozone is largely promoted.The mechanism associated with the resistance of the Fe_(3)C@C/C catalyst to Si and its elevated activity are also elucidated.展开更多
基金This work was financially supported by the Youth Innovation Promotion Association CAS(No.2020190)the National Natural Science Foundation of China(No.52100072)+1 种基金the Scientific Research Common Program of Beijing Municipal,Commission of Education(No.KM202010017006)the Beijing Natural Science Foundation(No.8214056).
文摘The improvement of catalysts’stability under harsh reaction conditions is vital for their practical applica-bility.Herein,iron carbide(Fe_(3)C)nanoparticles were encapsulated in graphitic carbon in situ and a carbon ball served as the carrier.The synthesized Fe_(3)C@C/C was first utilized to treat an m-cresol wastewater containing Si via catalytic ozonation.Compared with the commercial Fe/Al_(2)O_(3)catalyst,the resistance to Si of the Fe_(3)C@C/C was improved 22.68 times,while the TOC removal rate increased by a factor of 2.9,and it remained stable during 10 cycles and 12000 min of continuous reaction,which further demon-strated its potential for diverse applications.The catalyst exhibits improved resistance to Si because of the dual protection from the carbon-encapsulated structure and carbon carrier.Density functional theory calculations show that the encapsulation of Fe_(3)C using carbon significantly increases the resistance to adsorption of Si on its active sites.In addition,the activation of O_(3)is unimpeded on the Fe_(3)C adsorption sites by the protection from C,thus the generation of reactive oxygen species(ROS)by ozone is largely promoted.The mechanism associated with the resistance of the Fe_(3)C@C/C catalyst to Si and its elevated activity are also elucidated.
