Carbon Oxyanion Self‐Transformation on NiFe Oxalates Enables Long‐Term Ampere‐Level Current Density Seawater Oxidation

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Abstract
Seawater electrolysis is an attractive way of making H2 in coastal areas, and NiFe‐based materials are among the top options for alkaline seawater oxidation (ASO). However, ample Cl− in seawater can severely corrode catalytic sites and lead to limited lifespans. Herein, we report that in situ carbon oxyanion self‐transformation (COST) from oxalate to carbonate on a monolithic NiFe oxalate micropillar electrode allows safeguard of high‐valence metal reaction sites in ASO. In situ/ex situ studies show that spontaneous, timely, and appropriate COST safeguards active sites against Cl− attack during ASO even at an ampere‐level current density (j). Our NiFe catalyst shows efficient and stable ASO performance, which requires an overpotential as low as 349 mV to attain a j of 1 A cm−2. Moreover, the NiFe catalyst with protective surface CO32− exhibits a slight activity degradation after 600 h of electrolysis under 1 A cm−2 in alkaline seawater. This work reports effective catalyst surface design concepts at the level of oxyanion self‐transformation, acting as a momentous step toward defending active sites in seawater‐to‐H2 conversion systems.

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