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Direct Seawater Hydrogen Evolution via Atomically Precise Regulation of Interfacial pH and Ion-Water Interactions
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DOI：10.1002/anie.7140350.png)
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Abstract
En 中文
Direct seawater electrolysis offers a sustainable route to green hydrogen production from abundant saline water resources, yet industrial applications are limited by sluggish kinetics and catalyst deactivation caused by Mg(OH)2/Ca(OH)2 precipitation or Cl− corrosion. Here, we report a pH-gradient-mediated interfacial engineering strategy that simultaneously enhances activity and stability of metal nanocatalysts for the hydrogen evolution reaction (HER) in natural seawater. By using atomically precise Pt6(TPP)4Cl5 nanoclusters (NCs) (Pt6-TPP, TPP = triphenylphosphine) as paradigm catalysts, we demonstrate self-organized TPP ligands on cluster surface tether Na+/K+ via cation–π interactions. The locally concentrated Na+/K+ cations disrupt the hydrogen-bond network of water molecules for accelerating HER kinetics, and electrostatically attract OH− to establish an alkaline interfacial pH, which can propagate into a diffuse pH gradient toward the bulk of the solution. This pH gradient drives Mg2+/Ca2+ precipitation away from the catalytic surface, preventing site blockage. The enriched OH− can also resist Cl− corrosion of Pt6-TPP NCs. Consequently, Pt6-TPP achieves 10 mA cm−2 at an overpotential of 292 mV and retains exceptional stability (> 500 h) under intermittent renewable-energy operation, with one-tenth the Pt loading of commercial Pt/C. This work establishes a pH gradient-mediated interfacial chemistry framework enabled by atomically precise engineering, providing guidance for sustainable and efficient direct seawater hydrogen evolution.
Keywords:
atomically precise
direct seawater electrolysis
interfacial engineering
nanoclusters
pH-gradient
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