Polymetallic layered double hydroxides are promising cost-effective catalysts for the oxygen evolution reaction(OER) due to their versatile anionic and cationic tunability. Nevertheless, several challenges persist, no...Polymetallic layered double hydroxides are promising cost-effective catalysts for the oxygen evolution reaction(OER) due to their versatile anionic and cationic tunability. Nevertheless, several challenges persist, notably, issues related to low electrical conductivity, poor catalytic activity, and stability, especially at high current density. Herein, we report the design of Ce-and Ladoped Co Ni Fe-layered double hydroxide(Ce La Co Ni Fe-LDH) nanosheets through a facile and scalable in situ self-assembly strategy that displays enhanced OER activity. Experimental and theoretical investigations provide insights into the impact of Ceand La-doping by comparing Ce Co Ni Fe-LDH, La Co Ni Fe-LDH, and pristine Co Ni Fe-LDH, all synthesized using the same methodology. These results reveal that doping Ce^(3+)and La^(3+)into Co Ni Fe-LDH substantially improves its electronic structure,resulting in enhanced conductivity, more oxygen vacancies(Vo), electron interaction, and active site formation. Consequently,significantly reduced overpotentials of 175, 314, and 424 m V at 10, 100, and 500 m A cm^(-2), respectively, and a highly stable current density of 120 h in 1 M KOH were achieved. Notably, these performance metrics surpass those of unmodified LDHs and are competitive with many lanthanide-doped transition metal-based LDH electrocatalysts, as well as noble metal catalysts like ruthenium catalysts. This work represents a pioneering effort in doping Ce^(3+)and La^(3+)ions into a functional Co Ni Fe-based electrocatalyst, offering inspiring OER performance and scalability potential.展开更多
基金supported by the National Natural Science Foundation of China (22122113)the National Key R&D Program of China (2022YFB3506200)。
文摘Polymetallic layered double hydroxides are promising cost-effective catalysts for the oxygen evolution reaction(OER) due to their versatile anionic and cationic tunability. Nevertheless, several challenges persist, notably, issues related to low electrical conductivity, poor catalytic activity, and stability, especially at high current density. Herein, we report the design of Ce-and Ladoped Co Ni Fe-layered double hydroxide(Ce La Co Ni Fe-LDH) nanosheets through a facile and scalable in situ self-assembly strategy that displays enhanced OER activity. Experimental and theoretical investigations provide insights into the impact of Ceand La-doping by comparing Ce Co Ni Fe-LDH, La Co Ni Fe-LDH, and pristine Co Ni Fe-LDH, all synthesized using the same methodology. These results reveal that doping Ce^(3+)and La^(3+)into Co Ni Fe-LDH substantially improves its electronic structure,resulting in enhanced conductivity, more oxygen vacancies(Vo), electron interaction, and active site formation. Consequently,significantly reduced overpotentials of 175, 314, and 424 m V at 10, 100, and 500 m A cm^(-2), respectively, and a highly stable current density of 120 h in 1 M KOH were achieved. Notably, these performance metrics surpass those of unmodified LDHs and are competitive with many lanthanide-doped transition metal-based LDH electrocatalysts, as well as noble metal catalysts like ruthenium catalysts. This work represents a pioneering effort in doping Ce^(3+)and La^(3+)ions into a functional Co Ni Fe-based electrocatalyst, offering inspiring OER performance and scalability potential.
