Spin regulation of active sites is sparking much interest in boosting oxygen electrocatalytic performance.However,in amorphous electrocatalysts,the design principle of spin regulation to promote catalytic activity rem...Spin regulation of active sites is sparking much interest in boosting oxygen electrocatalytic performance.However,in amorphous electrocatalysts,the design principle of spin regulation to promote catalytic activity remains unclear.Herein,we synthesized a series of heteroatom-doped amorphous transition metal sulfides with regulated spin states using a one-step hydrothermal process.Especially in Modoped CoS,the spin state of Co^(2+)was successfully modulated to the low-spin state,which could optimize the adsorption free energy of various intermediates,improving the oxygen reduction reaction kinetics.The fabricated Zn-air batteries(ZABs)delivered good cycle stability(over 100 h).The large ZAB(100 cm^(2))exhibited a high discharge voltage(1.25 V under 0.5 A)and a superior overall mass-energy density(93 W h kg^(−1)),which illuminated a 2.5-m light-emitting-diode ribbon for over seven days.This work provides new insight into the mechanism of engineering spin states in amorphous materials for oxygen electrocatalysis.展开更多
基金the National Natural Science Foundation of China(52122107 and 972224)the Postdoctoral International Exchange Program(YJ20200139).
文摘Spin regulation of active sites is sparking much interest in boosting oxygen electrocatalytic performance.However,in amorphous electrocatalysts,the design principle of spin regulation to promote catalytic activity remains unclear.Herein,we synthesized a series of heteroatom-doped amorphous transition metal sulfides with regulated spin states using a one-step hydrothermal process.Especially in Modoped CoS,the spin state of Co^(2+)was successfully modulated to the low-spin state,which could optimize the adsorption free energy of various intermediates,improving the oxygen reduction reaction kinetics.The fabricated Zn-air batteries(ZABs)delivered good cycle stability(over 100 h).The large ZAB(100 cm^(2))exhibited a high discharge voltage(1.25 V under 0.5 A)and a superior overall mass-energy density(93 W h kg^(−1)),which illuminated a 2.5-m light-emitting-diode ribbon for over seven days.This work provides new insight into the mechanism of engineering spin states in amorphous materials for oxygen electrocatalysis.
