Abstract

Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy, but detrimental chlorine species (i.e., chloride and hypochlorite) cause severe corrosion at the anode. Here, we report our recent finding that benzoate anions-intercalated NiFe-layered double hydroxide nanosheet on carbon cloth (BZ-NiFe-LDH/CC) behaves as a highly efficient and durable monolithic catalyst for alkaline seawater oxidation, affords enlarged interlayer spacing of LDH, inhibits chlorine (electro)chemistry, and alleviates local pH drop of the electrode. It only needs an overpotential of 320 mV to reach a current density of 500 mA·cm<sup>–2</sup> in 1 M KOH. In contrast to the fast activity decay of NiFe-LDH/CC counterpart during long-term electrolysis, BZ-NiFe-LDH/CC achieves stable 100-h electrolysis at an industrial-level current density of 500 mA·cm<sup>–2</sup> in alkaline seawater. <i>Operando</i> Raman spectroscopy studies further identify structural changes of disordered <i>δ</i> (Ni<sup>III</sup>-O) during the seawater oxidation process.

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