Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified ...Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),respectively.In addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air batteries.The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and HER.Density functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of reactions.These electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster reactions.This study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.展开更多
Modulating Pt surfaces through the introduction of lattice distortion emerges as immensely effective strategy that enhances the kinetics of alkaline hydrogen evolution and oxidation processes.In this study,we fabricat...Modulating Pt surfaces through the introduction of lattice distortion emerges as immensely effective strategy that enhances the kinetics of alkaline hydrogen evolution and oxidation processes.In this study,we fabricated lattice-distorted Pt wrinkled nanoparticles(LD-Pt WNPs)for efficient hydrogen electrocatalysis.The LD-Pt WNPs not only outperform the Pt/C benchmark in hydrogen oxidation reaction,achieving an excellent mass-specific current of 968.5 mA·mg_(Pt)^(-1)(9 times that of Pt/C),but also demonstrate outstanding hydrogen evolution reaction activity with a small overpotential of 58.0 mV.Comprehensive experiments and density functional theory calculations reveal that lattice defects introduce an abundance of unsaturated coordination atoms while modifying the d-band center of Pt.This dual effect optimizes the binding strength of crucial H and OH intermediates,leading to a significant reduction in the energy barrier of the reaction bottleneck,commonly known as the Volmer step.This work unveils a fresh viewpoint on projecting and developing high efficiency electrocatalysts through defect engineering.展开更多
基金supported by the National Natural Science Foundation of China(Nos.51872209,52171145,21972106,22105146)Zhejiang Province Natural Science Foundation project key project(No.LZ20B030001)Zhejiang Provincial Special Support Program for High-level Talents(No.2019R52042).
文摘Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),respectively.In addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air batteries.The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and HER.Density functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of reactions.These electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster reactions.This study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.
基金supported by the National Natural Science Foundation of China(Nos.U1909213,51872209,52171145,22105146)Zhejiang Provincial Special Support Program for High-level Talents(No.2019R52042).
文摘Modulating Pt surfaces through the introduction of lattice distortion emerges as immensely effective strategy that enhances the kinetics of alkaline hydrogen evolution and oxidation processes.In this study,we fabricated lattice-distorted Pt wrinkled nanoparticles(LD-Pt WNPs)for efficient hydrogen electrocatalysis.The LD-Pt WNPs not only outperform the Pt/C benchmark in hydrogen oxidation reaction,achieving an excellent mass-specific current of 968.5 mA·mg_(Pt)^(-1)(9 times that of Pt/C),but also demonstrate outstanding hydrogen evolution reaction activity with a small overpotential of 58.0 mV.Comprehensive experiments and density functional theory calculations reveal that lattice defects introduce an abundance of unsaturated coordination atoms while modifying the d-band center of Pt.This dual effect optimizes the binding strength of crucial H and OH intermediates,leading to a significant reduction in the energy barrier of the reaction bottleneck,commonly known as the Volmer step.This work unveils a fresh viewpoint on projecting and developing high efficiency electrocatalysts through defect engineering.