Exploring efficient catalyst is critical for the application of persulfate-based advanced oxidation processes(AOPs)for environment remediation.Herein,perovskite CoTiO_(3)was demonstrated an efficient catalyst for pero...Exploring efficient catalyst is critical for the application of persulfate-based advanced oxidation processes(AOPs)for environment remediation.Herein,perovskite CoTiO_(3)was demonstrated an efficient catalyst for peroxymonosulfate(PMS)activation,which shows superior performance compared with single metal oxide system and homogenous systems:It removes 98.2%of hydroxychloroquine(HCQ,drugs for effective treatment of COVID-19)within 20 min at low dose of PMS(0.5 mmol/L),showing high tolerance to the environmental p H range(3.5–10.6)and significant versatility for various refractory organics.Combined with the material characterization and DFT calculations,it is found Co–O–Ti bond in CoTiO_(3)serves as an electron mediator to facilitate the rapid redox cycles of Co^(2+)/Co^(3+)during activation process,thus maintaining the high catalytic activity.Further mechanism exploration showed that fast regeneration of Co^(2+)ensures the production of high concentration of SO_(4)·-and·OH,thus securing the rapid degradation of HCQ.Moreover,a designed CoTiO_(3)-CNT-PVDF membrane reactor can effectively remove refractory pollutant via practically feasible filter-through mode,which delivers a highest removal efficiency and longest operation duration compared with previous developed membrane-based AOPs.The corresponding mechanism revealed in this work can serve as guidelines for the design of advanced heterogenous catalysts and membrane reactors for AOPs.展开更多
Photocatalytic hydrogen(H_(2))production via water splitting in the absence of sacrificial agents is a promising strategy for producing clean and sustainable hydrogen energy from solar energy.However,the realization o...Photocatalytic hydrogen(H_(2))production via water splitting in the absence of sacrificial agents is a promising strategy for producing clean and sustainable hydrogen energy from solar energy.However,the realization of a photocatalytic pure water splitting system with desirable efficiency is still a huge challenge.Herein,visible light photocatalytic H_(2) production from pure water splitting was successfully achieved using a g-C_(3)N_(4)/CoTiO_(3) S-scheme heterojunction photocatalyst in the absence of sacrificial agents.An optimum hydrogen evolution rate of 118μmol∙h^(−1)∙g^(−1) was reached with the addition of 1.5 wt%CoTiO_(3).The remarkably promoted hydrogen evolution rate was attributed to the intensified light absorption coupled with the synergistic effect of visible light responsive CoTiO_(3),the promoted efficiency in charge separation,and the reserved strong redox capacity induced by the S-scheme charge transfer mechanism.This work provides an alternative to visible light-responding oxidation photocatalysts for the construction of S-scheme heterojunctions and high-efficiency photocatalytic systems for pure water splitting.展开更多
The rapid migration and separation of photoinduced carriers is a key factor influencing photocatalytic efficiency.Constructing an S-scheme heterojunction is a strategic technique to enhance the separation of photogene...The rapid migration and separation of photoinduced carriers is a key factor influencing photocatalytic efficiency.Constructing an S-scheme heterojunction is a strategic technique to enhance the separation of photogenerated carriers and boost overall catalytic activity.Herein,a simple physical stirring technique was adopted to successfully fabricate a novel NiCo_(2)S_(4)/CoTiO_(3) S-scheme heterojunction photocatalyst.Upon exposure to light,the NiCo_(2)S_(4)/CoTiO_(3)-10 specimen demonstrated an outstanding hydrogen evolution rate of 2037.76μmol·g^(-1)·h^(-1),exceeding twice the rate observed for the pristine NiCo_(2)S_(4)(833.72μmol·g^(–1)·h^(–1)).The experimental outcomes reveal that the incorporation of CoTiO_(3) significantly enhances the charge separation and transfer within the system.Concurrently,the formation of the S-scheme mechanism facilitates the separation of carriers while maintaining high redox capabilities.This work introduces an innovative approach to forming S-scheme heterojunctions based on bimetallic sulfides,thereby offering new prospects for the efficient utilization of solar energy.展开更多
Environmental contamination by hexavalent chromium(Cr(VI))and antibiotic drug residues pose significant chal-lenges to public health and ecosystems.This study investigates the application ofCoTiO_(3)/BiVO_(4)@MIL-Fe(5...Environmental contamination by hexavalent chromium(Cr(VI))and antibiotic drug residues pose significant chal-lenges to public health and ecosystems.This study investigates the application ofCoTiO_(3)/BiVO_(4)@MIL-Fe(53)(CT/BV@Fe-MOF)for the reduction of Cr(VI)and degradation of tetracycline(TCL)under visible light.After grafting an iron-based metal–organic framework MIL-Fe(53)on a modified CoTiO_(3)/BiVO_(4)composite,the photogenerated electrons could easily be transferred from CoTiO_(3)to BiVO_(4)/Fe-MOF species via interfacial charge transfer.UV–vis diffuse reflec-tance spectroscopy showed that charge carriers were formed in response to visible light absorption.The effect of different operating parameters,including catalyst load,pH,initial Cr(VI),and TCL concentration,was systematically evaluated during the photocatalytic process.The CT/BV@Fe-MOF composite exhibited 98.7%reduction efficiency in Cr(VI)(50 ppm)and 97.5%degradation efficiency towards TCL(30 ppm)within 90 min,resulting in a greater efficiency than the pristine CoTiO_(3),BiVO_(4),and Fe-MOF materials.The CT/BV@Fe-MOF composite displayed excellent stability over six cycles,highlighting its potential for practical applications.In addition,the plausible degradation pathway of TCL was evaluated using LC-ESI/MS analysis,while the TEST program was utilized to investigate the toxicity of the products generated during the degradation process.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52100084 and 52170155)Shenzhen Natural Science Fund(the stable support plan program,No.GXWD20231129152058003)。
文摘Exploring efficient catalyst is critical for the application of persulfate-based advanced oxidation processes(AOPs)for environment remediation.Herein,perovskite CoTiO_(3)was demonstrated an efficient catalyst for peroxymonosulfate(PMS)activation,which shows superior performance compared with single metal oxide system and homogenous systems:It removes 98.2%of hydroxychloroquine(HCQ,drugs for effective treatment of COVID-19)within 20 min at low dose of PMS(0.5 mmol/L),showing high tolerance to the environmental p H range(3.5–10.6)and significant versatility for various refractory organics.Combined with the material characterization and DFT calculations,it is found Co–O–Ti bond in CoTiO_(3)serves as an electron mediator to facilitate the rapid redox cycles of Co^(2+)/Co^(3+)during activation process,thus maintaining the high catalytic activity.Further mechanism exploration showed that fast regeneration of Co^(2+)ensures the production of high concentration of SO_(4)·-and·OH,thus securing the rapid degradation of HCQ.Moreover,a designed CoTiO_(3)-CNT-PVDF membrane reactor can effectively remove refractory pollutant via practically feasible filter-through mode,which delivers a highest removal efficiency and longest operation duration compared with previous developed membrane-based AOPs.The corresponding mechanism revealed in this work can serve as guidelines for the design of advanced heterogenous catalysts and membrane reactors for AOPs.
文摘Photocatalytic hydrogen(H_(2))production via water splitting in the absence of sacrificial agents is a promising strategy for producing clean and sustainable hydrogen energy from solar energy.However,the realization of a photocatalytic pure water splitting system with desirable efficiency is still a huge challenge.Herein,visible light photocatalytic H_(2) production from pure water splitting was successfully achieved using a g-C_(3)N_(4)/CoTiO_(3) S-scheme heterojunction photocatalyst in the absence of sacrificial agents.An optimum hydrogen evolution rate of 118μmol∙h^(−1)∙g^(−1) was reached with the addition of 1.5 wt%CoTiO_(3).The remarkably promoted hydrogen evolution rate was attributed to the intensified light absorption coupled with the synergistic effect of visible light responsive CoTiO_(3),the promoted efficiency in charge separation,and the reserved strong redox capacity induced by the S-scheme charge transfer mechanism.This work provides an alternative to visible light-responding oxidation photocatalysts for the construction of S-scheme heterojunctions and high-efficiency photocatalytic systems for pure water splitting.
基金supported by the Fundamental Research Funds for the Central Universities of the North Minzu University(Grant No.2023ZRLG20)。
文摘The rapid migration and separation of photoinduced carriers is a key factor influencing photocatalytic efficiency.Constructing an S-scheme heterojunction is a strategic technique to enhance the separation of photogenerated carriers and boost overall catalytic activity.Herein,a simple physical stirring technique was adopted to successfully fabricate a novel NiCo_(2)S_(4)/CoTiO_(3) S-scheme heterojunction photocatalyst.Upon exposure to light,the NiCo_(2)S_(4)/CoTiO_(3)-10 specimen demonstrated an outstanding hydrogen evolution rate of 2037.76μmol·g^(-1)·h^(-1),exceeding twice the rate observed for the pristine NiCo_(2)S_(4)(833.72μmol·g^(–1)·h^(–1)).The experimental outcomes reveal that the incorporation of CoTiO_(3) significantly enhances the charge separation and transfer within the system.Concurrently,the formation of the S-scheme mechanism facilitates the separation of carriers while maintaining high redox capabilities.This work introduces an innovative approach to forming S-scheme heterojunctions based on bimetallic sulfides,thereby offering new prospects for the efficient utilization of solar energy.
基金supported by the National Science Foundation of China(No.22175059 and 62264015).
文摘Environmental contamination by hexavalent chromium(Cr(VI))and antibiotic drug residues pose significant chal-lenges to public health and ecosystems.This study investigates the application ofCoTiO_(3)/BiVO_(4)@MIL-Fe(53)(CT/BV@Fe-MOF)for the reduction of Cr(VI)and degradation of tetracycline(TCL)under visible light.After grafting an iron-based metal–organic framework MIL-Fe(53)on a modified CoTiO_(3)/BiVO_(4)composite,the photogenerated electrons could easily be transferred from CoTiO_(3)to BiVO_(4)/Fe-MOF species via interfacial charge transfer.UV–vis diffuse reflec-tance spectroscopy showed that charge carriers were formed in response to visible light absorption.The effect of different operating parameters,including catalyst load,pH,initial Cr(VI),and TCL concentration,was systematically evaluated during the photocatalytic process.The CT/BV@Fe-MOF composite exhibited 98.7%reduction efficiency in Cr(VI)(50 ppm)and 97.5%degradation efficiency towards TCL(30 ppm)within 90 min,resulting in a greater efficiency than the pristine CoTiO_(3),BiVO_(4),and Fe-MOF materials.The CT/BV@Fe-MOF composite displayed excellent stability over six cycles,highlighting its potential for practical applications.In addition,the plausible degradation pathway of TCL was evaluated using LC-ESI/MS analysis,while the TEST program was utilized to investigate the toxicity of the products generated during the degradation process.
