首页|Valence electronic engineering of superhydrophilic Dy-evoked Ni-MOF outperforming RuO2 for highly efficient electrocatalytic oxygen evolution
Valence electronic engineering of superhydrophilic Dy-evoked Ni-MOF outperforming RuO2 for highly efficient electrocatalytic oxygen evolution
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Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs)is crucial to improve their oxygen evolution reaction(OER)performance.Herein,we introduce a novel strategy of dysprosium(Dy)doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF)nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT)calculations reveal that Dy doping can effectively mod-ify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band cen-ter to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorp-tion of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics.Ex-situ and in-situ analysis results manifest Dy2O3/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@Ni-MOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm-2 and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
Zhiyang Huang、Miao Liao、Shifan Zhang、Lixia Wang、Mingcheng Gao、Zuyang Luo、Tayirjan Taylor Isimjan、Bao Wang、Xiulin Yang
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Guangxi Key Laboratory of Low Carbon Energy Materials,School of Chemistry and Pharmaceutical Sciences,Guangxi Normal University,Guilin 541004,Guangxi,China
Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST),Thuwal 23955-6900,Saudi Arabia
State Key Laboratory of Biochemical Engineering,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China
国家自然科学基金国家自然科学基金广西自然科学基金Guangxi Technology Base and Talent SubjectGuangxi Technology Base and Talent Subject
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