Electrochemical ozone(O_(3))production(EOP)faces a critical challenge due to the competitive oxygen evolution reaction(OER),which severely limits ozone yields.Inspired by the oxygen-binding mechanism of heme,we design...Electrochemical ozone(O_(3))production(EOP)faces a critical challenge due to the competitive oxygen evolution reaction(OER),which severely limits ozone yields.Inspired by the oxygen-binding mechanism of heme,we designed a biomimetic catalyst,FePP@SnO_(2)@CA,by electrodepositing iron porphyrin(FePP)onto SnO_(2)@CA nanosheets,endowing it with an“oxygen-locking property”to suppress competing OER.This catalyst demonstrates exceptional EOP performance,achieving an ozone production rate of 8.9 mmol cm^(−2)h^(−1)and a Faraday efficiency(FE)of 20.46%±1.6%.DFT calculations confirm that Fe–O_(2)interactions stabilize O_(2)*intermediates,redirecting the reaction pathway from OER to ozone generation and reducing the O–O coupling energy barrier,thereby enabling thermodynamic selectivity control.In addition,when FePP@SnO_(2)@CA is used as a dual-functional material for sea sand desalination,the chlorine removal efficiency can reach 52.7%.This work provides a novel bioinspired strategy for EOP catalyst design and broadens the application potential of FePP@SnO_(2)@CA in sustainable technologies.展开更多
基金supported by the Natural Science Foundation of China,China(52173235)the Hainan Province Science and Technology Special Fund,China(ZDYF2024SHFZ038)+1 种基金the Venture&Innovation Support Program for Chongqing Overseas Returnees,China(CX2021018)the Innovative Research Group Project of National Natural Science Foundation of China,China(52021004)。
文摘Electrochemical ozone(O_(3))production(EOP)faces a critical challenge due to the competitive oxygen evolution reaction(OER),which severely limits ozone yields.Inspired by the oxygen-binding mechanism of heme,we designed a biomimetic catalyst,FePP@SnO_(2)@CA,by electrodepositing iron porphyrin(FePP)onto SnO_(2)@CA nanosheets,endowing it with an“oxygen-locking property”to suppress competing OER.This catalyst demonstrates exceptional EOP performance,achieving an ozone production rate of 8.9 mmol cm^(−2)h^(−1)and a Faraday efficiency(FE)of 20.46%±1.6%.DFT calculations confirm that Fe–O_(2)interactions stabilize O_(2)*intermediates,redirecting the reaction pathway from OER to ozone generation and reducing the O–O coupling energy barrier,thereby enabling thermodynamic selectivity control.In addition,when FePP@SnO_(2)@CA is used as a dual-functional material for sea sand desalination,the chlorine removal efficiency can reach 52.7%.This work provides a novel bioinspired strategy for EOP catalyst design and broadens the application potential of FePP@SnO_(2)@CA in sustainable technologies.
