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Clean Elastic strain to control the electrocatalytic hydrogen generation from water splitting

严凯  刘雨倩  张曼  Ashan Ejaz  叶晨璐  胡康  仇荣亮  
【摘要】:We present a study on the effect of externally applied elastic strain on the catalytic activity of metal films in the context of a model reaction-the hydrogen evolution reaction(HER).Thin metal films supported on elastic substrates are uniaxially strained in situ in compression and tension while they participate in the HER and their catalytic activity is measured through shifts in the cyclic voltammograms.We show that elastic strain tunes the catalytic activity in a controlled and predictable way;for each metal considered here,compressive and tensile strains have the opposite effect on the catalytic activity;also,the changes in the catalytic activity scale with the strain magnitude within the range of strain values accessed in our experiments.The HER activity is often described in terms of a volcano plot(a plot of the catalytic activity vs.a descriptor parameter that controls the activity),which suggests that optimum HER catalysts will have the free energy change of hydrogen bonding △G =0.In this work,we consider metal thin-film catalysts from three regions of the volcano plot-Ni(△G0),Pt(△G~0)and Cu(△G0)-and subject them to compressive and tensile strain.1 The experimental results show that Pt and Ni films show increased HER activity under compressive strain;while Cu's HER activity is retarded by compressive strain.The opposite was observed under tensile strain.The experimental observations are understood by considering the influence of elastic strain on hydrogen binding energy,which has been calculated through density functional theory(DFT).Compressive strain increases the hydrogen binding on Ni,shifting it towards the volcano peak,while tensile strain has the opposite effect.However,the same strains have the opposite effect on Cu since it is located on the other side of the volcano peak.By isolating elastic strain from the electronic structure effects(the so called-ligand effect),this study provides a better understanding of the processes that control electrocatalytic activity towards HER and can guide design of strained core-shell nano-particle catalysts.

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