Photothermal material applied in environmental governance has attracted growing attention.By combining the Stober method and dopamine-triggered coating strategy,Co-Mn precursor was in situ incorporated into the poly d...Photothermal material applied in environmental governance has attracted growing attention.By combining the Stober method and dopamine-triggered coating strategy,Co-Mn precursor was in situ incorporated into the poly dopamine(PDA)layer over the surface of silica cores.Afterwards,a unique photothermal nanosphere with SiO_(2)core and thin carbon layer and dual Co-Mn oxides shell was allowed to form by sequential heat treatment in the inert atmosphere(SiO_(2)@CoMn/C).The bimetallic fraction of Co/Mn in the carbon layer and post-treatment calcination temperature was comprehensively tuned to optimize the peroxymonosulfate(PMS)activation performance of the catalyst.The state of bimetallic species was studied including their physical distribution,chemical valence,and interplay by various characterizations.Impressively,Co oxides appear as dominant monodispersed nanoparticles(~10 nm),while Mn with cluster-like morphology is observed to uniformly distribute over thin-layer carbon and adhered to the surface of SiO_(2)nanospheres(~250 nm).The calcined temperature could tune the oxidized state of Co species,leading to the optimization of the catalytic performance of introduced dual metal species.As a result,this obtained optimal catalyst integrated the advantages of exposed bimetallic CoMn species and N-doped thin carbon to deliver excellent catalytic PMS activation performance and photothermal synergetic catalytic mineralization ability for diversiform pollutants.Further reactions condition controls and anion interference studies were conducted to identify the adaptability of the optimal catalyst.Moreover,the application of solar-driven interfacial water evaporation using optimal SiO_(2)@Co_3Mn_1/C-600 catalyst was explored,showing a high water evaporation rate of 1.48 kg·m^(-2)·h^(-1)and an efficiency of 95.2%,further revealing a comprehensive governance functionality of obtained material in the complex pollution condition.展开更多
The development of effective and sustainable solutions for pleiotropic water purification becomes urgent and attractive.Heterogeneous Fenton-like catalysts for activation of peroxymonosulfate(PMS)to purify organic was...The development of effective and sustainable solutions for pleiotropic water purification becomes urgent and attractive.Heterogeneous Fenton-like catalysts for activation of peroxymonosulfate(PMS)to purify organic wastewater show great promise.In this work,by tuning metal loading with an in-situ polydopamine coating strategy,oxygen vacancy-enriched Co_(3)O_(4) loading on N-doped carbon nanotubes(CNTs)were constructed to enhance PMS activation efficiency for pollutants degradation.Impressively,the obtained modified CNTs afford a well-developed N-containing network structure,which is further endowed with abundant Co(Ⅱ)/Co(Ⅲ)redox cycles and significant metal-carbon interactions.In particular,the surface N doping in CNTs might induce the oriented enrichment of pollutants around the catalyst,which reduces the migration distance and correspondingly improves the utilization of reactive oxidative species.The electron transfer efficiency of the catalyst can be further improved by incorporating oxygen vacancy-enriched Co_(3)O_(4).The performance results show that the optimal NC/Co-1 could mineralize 20×10^(-6)of bisphenol A(BPA)by almost 98%in 8 min.A low reaction activation energy(26.05 kJ·mol^(-1))in BPA degradation was demonstrated by the NC/Co-1.More importantly,NC/Co-1 can inherit excellent degradation performance towards oxytetracycline,2,4-dichlorophenol,and tetracycline,showing wide practical flexibility.In addition,by virtue of the photothermal conversion property,NC/Co-1 achieves an additive function for interfacial solar water evaporation(1.84 kg·m^(-2)·h^(-1),112.51%),showing impressive potential for clean water recovery under complicated environmental pollution conditions.展开更多
基金financially supported by the China National Natural Science Foundation(No.21908085)China Postdoctoral Science Foundation(No.2022M711686)Jiangsu Provincial Founds for the Young Scholars(No.BK20190961)。
文摘Photothermal material applied in environmental governance has attracted growing attention.By combining the Stober method and dopamine-triggered coating strategy,Co-Mn precursor was in situ incorporated into the poly dopamine(PDA)layer over the surface of silica cores.Afterwards,a unique photothermal nanosphere with SiO_(2)core and thin carbon layer and dual Co-Mn oxides shell was allowed to form by sequential heat treatment in the inert atmosphere(SiO_(2)@CoMn/C).The bimetallic fraction of Co/Mn in the carbon layer and post-treatment calcination temperature was comprehensively tuned to optimize the peroxymonosulfate(PMS)activation performance of the catalyst.The state of bimetallic species was studied including their physical distribution,chemical valence,and interplay by various characterizations.Impressively,Co oxides appear as dominant monodispersed nanoparticles(~10 nm),while Mn with cluster-like morphology is observed to uniformly distribute over thin-layer carbon and adhered to the surface of SiO_(2)nanospheres(~250 nm).The calcined temperature could tune the oxidized state of Co species,leading to the optimization of the catalytic performance of introduced dual metal species.As a result,this obtained optimal catalyst integrated the advantages of exposed bimetallic CoMn species and N-doped thin carbon to deliver excellent catalytic PMS activation performance and photothermal synergetic catalytic mineralization ability for diversiform pollutants.Further reactions condition controls and anion interference studies were conducted to identify the adaptability of the optimal catalyst.Moreover,the application of solar-driven interfacial water evaporation using optimal SiO_(2)@Co_3Mn_1/C-600 catalyst was explored,showing a high water evaporation rate of 1.48 kg·m^(-2)·h^(-1)and an efficiency of 95.2%,further revealing a comprehensive governance functionality of obtained material in the complex pollution condition.
基金financially supported by the China National Natural Science Foundation(No.201808085)the National Key Research and Development Program of China(No.2022YFB3504100)+2 种基金Jiangsu Provincial Founds for Young Scholars(No.BK20190961)the Natural Science Foundation of Jiangsu Higher Education Institutions of China(No.22KJB610012)the International Cooperation Foundation for the Chunhui Plan Program of Ministry of Education of China(No.HZKY20220136)。
文摘The development of effective and sustainable solutions for pleiotropic water purification becomes urgent and attractive.Heterogeneous Fenton-like catalysts for activation of peroxymonosulfate(PMS)to purify organic wastewater show great promise.In this work,by tuning metal loading with an in-situ polydopamine coating strategy,oxygen vacancy-enriched Co_(3)O_(4) loading on N-doped carbon nanotubes(CNTs)were constructed to enhance PMS activation efficiency for pollutants degradation.Impressively,the obtained modified CNTs afford a well-developed N-containing network structure,which is further endowed with abundant Co(Ⅱ)/Co(Ⅲ)redox cycles and significant metal-carbon interactions.In particular,the surface N doping in CNTs might induce the oriented enrichment of pollutants around the catalyst,which reduces the migration distance and correspondingly improves the utilization of reactive oxidative species.The electron transfer efficiency of the catalyst can be further improved by incorporating oxygen vacancy-enriched Co_(3)O_(4).The performance results show that the optimal NC/Co-1 could mineralize 20×10^(-6)of bisphenol A(BPA)by almost 98%in 8 min.A low reaction activation energy(26.05 kJ·mol^(-1))in BPA degradation was demonstrated by the NC/Co-1.More importantly,NC/Co-1 can inherit excellent degradation performance towards oxytetracycline,2,4-dichlorophenol,and tetracycline,showing wide practical flexibility.In addition,by virtue of the photothermal conversion property,NC/Co-1 achieves an additive function for interfacial solar water evaporation(1.84 kg·m^(-2)·h^(-1),112.51%),showing impressive potential for clean water recovery under complicated environmental pollution conditions.