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<p>Direct seawater electrolysis at ampere-level current densities, powered by coastal/offshore renewables, is an attractive avenue for sustainable hydrogen production but is undermined by chloride-induced anode degradation. Here we demonstrate the use of hexafluorophosphate (PF₆⁻) as an electrolyte additive to overcome this limitation, achieving prolonged operation for over 5,000 hours at 1 A cm<sup>−2</sup> and 2300 hours at 2 A cm<sup>−2</sup> using NiFe layered double hydroxide (LDH) as anode. Together with the experimental findings, PF₆⁻ can intercalate into LDH interlayers and adsorb onto the electrode surface under an applied electric field, blocking Cl⁻ and stabilizing Fe to prevent segregation. The constant-potential molecular dynamics simulations further reveal the accumulation of high surface concentrations of PF<sub>6</sub><sup>−</sup> on the electrode surface that can effectively exclude Cl<sup>−</sup>, mitigating corrosion. Our work showcases synchronous interlayer and surface engineering by single non-oxygen anion species to enable Cl<sup>−</sup> rejection and marks a crucial step forward in seawater electrolysis.</p>

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Hexafluorophosphate additive enables durable seawater oxidation at ampere-level current density

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年5月29日

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  • Xun He,
  • Yongchao Yao,
  • Limei Zhang,
  • Hefeng Wang,
  • Hong Tang,
  • Wenlong Jiang,
  • Yuchun Ren,
  • Jue Nan,
  • Yongsong Luo,
  • Tongwei Wu,
  • Fengming Luo,
  • Bo Tang,
  • Xuping Sun

摘要

Direct seawater electrolysis at ampere-level current densities, powered by coastal/offshore renewables, is an attractive avenue for sustainable hydrogen production but is undermined by chloride-induced anode degradation. Here we demonstrate the use of hexafluorophosphate (PF₆⁻) as an electrolyte additive to overcome this limitation, achieving prolonged operation for over 5,000 hours at 1 A cm−2 and 2300 hours at 2 A cm−2 using NiFe layered double hydroxide (LDH) as anode. Together with the experimental findings, PF₆⁻ can intercalate into LDH interlayers and adsorb onto the electrode surface under an applied electric field, blocking Cl⁻ and stabilizing Fe to prevent segregation. The constant-potential molecular dynamics simulations further reveal the accumulation of high surface concentrations of PF6− on the electrode surface that can effectively exclude Cl−, mitigating corrosion. Our work showcases synchronous interlayer and surface engineering by single non-oxygen anion species to enable Cl− rejection and marks a crucial step forward in seawater electrolysis.