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Register a new userThe Influence of Elastic Strain on Catalytic Activity Towards the Hydrogen Evolution Reaction
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Understanding the role of elastic strain in modifying catalytic reaction rates is crucial for catalyst design, but experimentally, this effect is often coupled with a ligand effect. To isolate the strain effect, we have investigated the influence of externally applied elastic strain on the catalytic activity of metal films towards the hydrogen evolution reaction (HER). We show that elastic strain tunes the catalytic activity in a controlled and predictable way. Both theory and experiment show strain controls reactivity in a controlled manner consistent with the qualitative predictions of the HER volcano plot and the d-band theory: Ni and Pt activity were accelerated by compression, while Cu activity was accelerated by tension. By isolating the elastic strain effect from the ligand effect, this study provides a greater insight into the role of elastic strain in controlling electrocatalytic activity.
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The design of efficient electrocatalysts for electrochemical water splitting with minimal amount of precious metal is crucial to attain renewable and sustainable energy conversion. Here, we report the use of a network of CdSe branched colloidal nanocrystals, made of a CdSe core and eight CdSe pods (so-called octapods), able to host on their pods Pt particles, and thus catalyzing water splitting reactions. Thanks to the octapod shape, the resulting Pt-hosting network is mechanically trapped onto carbon nanotube buckypaper, providing mechanically flexible and binder-free electrodes. We found that such hierarchical configuration maximizes the mass activity and the utilization efficiency of Pt for the hydrogen evolution reaction (HER). At a potential of -0.15 V vs. reversible hydrogen electrode, the Pt/octapod network-based electrodes display a Pt mass activity on the HER of 166 A mg-1 and 42 A mg-1 in acidic and alkaline media, respectively. These values correspond to turnover frequencies of 168 s-1 and 42 s-1, respectively, which are in that order 14 and 21 times higher compared to commercially available Pt/C benchmarks. The strong chemical and mechanical interactions between the Pt and the octapod surface, along with pod-aided adhesion of the Pt/octapod network to the buckypaper, result in a long-term durability (>20 h) of the HER-activity in both media. These results experimentally prove that the exploitation of our network of branched nanocrystals hosting Pt particles can circumvent the durability issues of the catalysts while adopting either ultralow Pt loadings or benchmarking carbon-supported Pt nanocrystals. Our work opens up prospects for using porous networks made by branched nanocrystals as catalysts with ultralow amount of noble metals and controlled catalytic properties.
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