This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abun...This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,respectively.As both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 h.In-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water oxidation.Additionally,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER activities.This study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.展开更多
In this work,P and Mo dual-doped CoNiS(PMo-CoNiS)nanosheet arrays were successfully constructed through a common solvothermal treatment.The precise doping of P and Mo species into the CoNiS can regulate the microstruc...In this work,P and Mo dual-doped CoNiS(PMo-CoNiS)nanosheet arrays were successfully constructed through a common solvothermal treatment.The precise doping of P and Mo species into the CoNiS can regulate the microstructures and meanwhile endow with PMo-CoNiS abundant amorphous/crystalline heterointerfaces,which can adjust the electronic structure,thus enhancing the intrinsic activity of hydro-gen evolution reaction(HER)and oxygen evolution reaction(OER).As a result,ultra-low overpotentials of merely 156 and 58 mV are required to deliver a current density of 10 mA cm^(−2) for OER and HER,respec-tively,and the electrocatalysts PMo-CoNiS also exhibit low Tafel slopes and maintain robust stability for 48 h in alkaline media at a high current density of 50 mA cm^(−2).In addition,in an assembled electrolyte cell for overall water splitting,a voltage as low as 1.48 V is sufficient to yield a current density of 10 mA cm^(−2).Density functional theory(DFT)calculations further confirmed that the enhanced OER and HER result from the optimized OH^(∗)and H^(∗)adsorption energy of PMo-CoNiS due to P,Mo dual doping and generated interfacial effect.This work may offer an avenue for designing low-cost bifunctional catalysts with superior catalytic activity and provide a new application strategy for broader applications in various electrocatalytic fields.展开更多
基金National Programs for NanoKey Project(2022YFA1504002)National Natural Science Foundation of China(22078233)。
文摘This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,respectively.As both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 h.In-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water oxidation.Additionally,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER activities.This study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.
基金financial support of the National Natural Science Foundation of China(22078233)。
文摘In this work,P and Mo dual-doped CoNiS(PMo-CoNiS)nanosheet arrays were successfully constructed through a common solvothermal treatment.The precise doping of P and Mo species into the CoNiS can regulate the microstructures and meanwhile endow with PMo-CoNiS abundant amorphous/crystalline heterointerfaces,which can adjust the electronic structure,thus enhancing the intrinsic activity of hydro-gen evolution reaction(HER)and oxygen evolution reaction(OER).As a result,ultra-low overpotentials of merely 156 and 58 mV are required to deliver a current density of 10 mA cm^(−2) for OER and HER,respec-tively,and the electrocatalysts PMo-CoNiS also exhibit low Tafel slopes and maintain robust stability for 48 h in alkaline media at a high current density of 50 mA cm^(−2).In addition,in an assembled electrolyte cell for overall water splitting,a voltage as low as 1.48 V is sufficient to yield a current density of 10 mA cm^(−2).Density functional theory(DFT)calculations further confirmed that the enhanced OER and HER result from the optimized OH^(∗)and H^(∗)adsorption energy of PMo-CoNiS due to P,Mo dual doping and generated interfacial effect.This work may offer an avenue for designing low-cost bifunctional catalysts with superior catalytic activity and provide a new application strategy for broader applications in various electrocatalytic fields.
