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
Ba\-\{0.5\}Sr\-\{0.5\}Co\-\{0.8\}Fe\-\{0.2\}O\-\{3-\%δ\%\} and Ba\-\{0.5\}Sr\-\{0.5\}Co\-\{0.8\}Ti\-\{0.2\}O\-\{3-\%δ\%\} oxides were synthesized by a combined EDTA\|citrate complexing method. The catalytic behavior...Ba\-\{0.5\}Sr\-\{0.5\}Co\-\{0.8\}Fe\-\{0.2\}O\-\{3-\%δ\%\} and Ba\-\{0.5\}Sr\-\{0.5\}Co\-\{0.8\}Ti\-\{0.2\}O\-\{3-\%δ\%\} oxides were synthesized by a combined EDTA\|citrate complexing method. The catalytic behavior of these two oxides with the perovskite structure was studied during the reaction of methane oxidation. The pre\|treatment with methane has different effect on the catalytic activities of both the oxides. The methane pre\|treatment has not resulted in the change of the catalytic activity of BSCFO owing to its excellent reversibility of the perovskite structure resulting from the excellent synergistic interaction between Co and Fe in the oxide. However, the substitution with Ti on Fe\|site in the lattice makes the methane pre\|treatment have an obvious influence on the activity of the formed BSCTO oxide.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Ba\-\{0.5\}Sr\-\{0.5\}Co\-\{0.8\}Fe\-\{0.2\}O\-\{3-\%δ\%\} and Ba\-\{0.5\}Sr\-\{0.5\}Co\-\{0.8\}Ti\-\{0.2\}O\-\{3-\%δ\%\} oxides were synthesized by a combined EDTA\|citrate complexing method. The catalytic behavior of these two oxides with the perovskite structure was studied during the reaction of methane oxidation. The pre\|treatment with methane has different effect on the catalytic activities of both the oxides. The methane pre\|treatment has not resulted in the change of the catalytic activity of BSCFO owing to its excellent reversibility of the perovskite structure resulting from the excellent synergistic interaction between Co and Fe in the oxide. However, the substitution with Ti on Fe\|site in the lattice makes the methane pre\|treatment have an obvious influence on the activity of the formed BSCTO oxide.
