Developing high-efficient non-platinum （Pt） catalysts for oxygen reduction reaction （ORR） is the key to reduce the usage of Pt and the palladium （Pd）-based cata- lyst is a promising alternative. Here, we present...Developing high-efficient non-platinum （Pt） catalysts for oxygen reduction reaction （ORR） is the key to reduce the usage of Pt and the palladium （Pd）-based cata- lyst is a promising alternative. Here, we presented a facile approach to core/shell FePd/Pd nanoparticle （NP） catalyst with the FePd core in chemically ordered face-centered tetragonal （fct-） structure and the shell in controlled thickness from 0.32 to 0.81 nm via the thermal annealing of FePd NP followed by an electro-anodization process. With a 0.71 nm-thick Pd shell, the fct-FePd/Pd shows a robust catalytic activity and durability for ORR with the mass activities at 0.85 and 0.90 V reaching 453 and 96.7 A/mgpd, respectively, which are about 3.0 and 2.1 times higher than those of commercial Pt in alkaline media. This work presents a new class of non-Pt catalyst with superior performance to Pt for ORR catalysis, and the strategy demonstrated here can be extended to design highefficient catalysts for other chemical reactions.展开更多
Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and ...Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high efficiency.Herein,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this goal.The electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m V.Moreover,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish OER.The splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and theoretically.The selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent stability.This work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.展开更多
Reducing Pt loading, while improving electrocatalytic activity and the stability of Pt-based nanostructured materials, is currently a key challenge in green energy technology. Herein, we report the controllable synthe...Reducing Pt loading, while improving electrocatalytic activity and the stability of Pt-based nanostructured materials, is currently a key challenge in green energy technology. Herein, we report the controllable synthesis of tri-metallic （Au@Ag@Pt） and bimetallic （Ag@Pt） particles consisting of a controllable thin Pt shell, via interface-mediated galvanic displacement. Through oil-ethanol-H2O interface mediation, the controllable ＂out to in＂ displacement of Ag atoms to Pt enables the formation of a thin Pt shell on monodisperse sub-ten-nanometer Au@Ag and Ag nanocrystals. The synthesized nanoparticles with a thin Pt shell exhibited potential catalytic activity towards the oxygen reduction reaction （ORR） due to the high exposure of Pt atoms.展开更多
基金Acknowledgments This work was supported by the Key Projects of Applied Technology Development in Chongqing （cstc2014yykfB900027, the Science and Technology Project of Chongqing Municipal Education Commission （KJI500601） and the Natural Science Foundation of Chongqing Science and Technology Commission （cstc2015jcyjA20007）.
文摘Developing high-efficient non-platinum （Pt） catalysts for oxygen reduction reaction （ORR） is the key to reduce the usage of Pt and the palladium （Pd）-based cata- lyst is a promising alternative. Here, we presented a facile approach to core/shell FePd/Pd nanoparticle （NP） catalyst with the FePd core in chemically ordered face-centered tetragonal （fct-） structure and the shell in controlled thickness from 0.32 to 0.81 nm via the thermal annealing of FePd NP followed by an electro-anodization process. With a 0.71 nm-thick Pd shell, the fct-FePd/Pd shows a robust catalytic activity and durability for ORR with the mass activities at 0.85 and 0.90 V reaching 453 and 96.7 A/mgpd, respectively, which are about 3.0 and 2.1 times higher than those of commercial Pt in alkaline media. This work presents a new class of non-Pt catalyst with superior performance to Pt for ORR catalysis, and the strategy demonstrated here can be extended to design highefficient catalysts for other chemical reactions.
基金finically supported by the National Key R&D Program of China(2017YFE0120500)the National Natural Science Foundation of China(51972129,51702150,and 21725102)+2 种基金the Key Research and Development Program of Hubei(2020BAB079)Bintuan Science and Technology Program(2020DB002,and 2022DB009)the Science and Technology Innovation Committee Foundation of Shenzhen(JCYJ20210324141613032 and JCYJ20190809142019365)。
文摘Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high efficiency.Herein,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this goal.The electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m V.Moreover,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish OER.The splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and theoretically.The selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent stability.This work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.
文摘Reducing Pt loading, while improving electrocatalytic activity and the stability of Pt-based nanostructured materials, is currently a key challenge in green energy technology. Herein, we report the controllable synthesis of tri-metallic （Au@Ag@Pt） and bimetallic （Ag@Pt） particles consisting of a controllable thin Pt shell, via interface-mediated galvanic displacement. Through oil-ethanol-H2O interface mediation, the controllable ＂out to in＂ displacement of Ag atoms to Pt enables the formation of a thin Pt shell on monodisperse sub-ten-nanometer Au@Ag and Ag nanocrystals. The synthesized nanoparticles with a thin Pt shell exhibited potential catalytic activity towards the oxygen reduction reaction （ORR） due to the high exposure of Pt atoms.
