<p>Triggering the adsorbate evolution and lattice oxygen mechanisms coupled path holds promise for overcoming the activity-stability trade-off of oxygen evolution reaction (OER). However, achieving precise regulation and activation of multiple OER pathways via 3d-metal modification strategy remains challenging due to the external effects of crystal fields and coordination environments. Herein, we propose an atomic-dispersed rare earth substitution strategy to construct a spatially partitioned reaction mechanism, and achieve dual activation between adsorbate evolution and lattice oxygen mechanisms. The strong shielding effect of 5 <i>s</i>/5<i>p</i> electrons in RE significantly reduces the influence of the external environment on the 4 <i>f</i> orbitals, thereby enhancing the controllability of the reaction pathway. The optimized Sm-NiMoO<sub>4</sub> exhibits favorable OER performance. At an industrial temperature of 70 °C, the OER in simulated seawater exhibits an overpotential of only 214 mV at 0.5 A cm<sup>−2</sup>, while maintaining stability for 1500 h. Preliminary techno-economic analysis reveals that the cost of hydrogen produced from the Sm-NiMoO<sub>4</sub> is US$2.56 kg<sup>−1</sup>. This synthetic strategy and mechanism analysis represent a valuable contribution towards achieving industrial-scale seawater hydrogen production.</p>

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Breaking the activity-stability trade-off via dual-mechanism induced by rare earths for lasting seawater electrolysis

  • Le-le Ma,
  • Huihui Cao,
  • Zhen Yan,
  • Yi-ru Hao,
  • Jiawen Sun,
  • Yaqin Chen,
  • Chunhao Li,
  • Jia Liu,
  • Hui Xue,
  • Jing Sun,
  • Yali Zhang,
  • Yaowen Li,
  • Limin Wu,
  • Qin Wang

摘要

Triggering the adsorbate evolution and lattice oxygen mechanisms coupled path holds promise for overcoming the activity-stability trade-off of oxygen evolution reaction (OER). However, achieving precise regulation and activation of multiple OER pathways via 3d-metal modification strategy remains challenging due to the external effects of crystal fields and coordination environments. Herein, we propose an atomic-dispersed rare earth substitution strategy to construct a spatially partitioned reaction mechanism, and achieve dual activation between adsorbate evolution and lattice oxygen mechanisms. The strong shielding effect of 5 s/5p electrons in RE significantly reduces the influence of the external environment on the 4 f orbitals, thereby enhancing the controllability of the reaction pathway. The optimized Sm-NiMoO4 exhibits favorable OER performance. At an industrial temperature of 70 °C, the OER in simulated seawater exhibits an overpotential of only 214 mV at 0.5 A cm−2, while maintaining stability for 1500 h. Preliminary techno-economic analysis reveals that the cost of hydrogen produced from the Sm-NiMoO4 is US$2.56 kg−1. This synthetic strategy and mechanism analysis represent a valuable contribution towards achieving industrial-scale seawater hydrogen production.