RESUMEN
Low-energy consumption seawater electrolysis at high current density is an effective way for hydrogen production, however the continuous feeding of seawater may result in the accumulation of Cl-, leading to severe anode poisoning and corrosion, thereby compromising the activity and stability. Herein, CoFeAl layered double hydroxide anodes with excellent oxygen evolution reaction activity are synthesized and delivered stable catalytic performance for 350 hours at 2 A cm-2 in the presence of 6-fold concentrated seawater. Comprehensive analysis reveals that the Al3+ ions in electrode are etched off by OH- during oxygen evolution reaction process, resulting in M3+ vacancies that boost oxygen evolution reaction activity. Additionally, the self-originated Al(OH)n- is found to adsorb on the anode surface to improve stability. An electrode assembly based on a micropore membrane and CoFeAl layered double hydroxide electrodes operates continuously for 500 hours at 1 A cm-2, demonstrating their feasibility in brine electrolysis.
RESUMEN
Commercial alkaline water electrolysers typically operate at 80 °C to minimize energy consumption. However, NiFe-based catalysts, considered as one of the most promising candidates for anode, encounter the bottleneck of high solubility at such temperatures. Herein, we discover that the dissolution of NiFe layered double hydroxides (NiFe-LDH) during operation not only leads to degradation of anode itself, but also deactivates cathode for water splitting, resulting in decay of overall electrocatalytic performance. Aiming to suppress the dissolution, we employed oxyanions as inhibitors in electrolyte. The added phosphates to the electrolyte inhibit the loss of NiFe-LDH active sites at 400â mA cm-2 to 1/3 of the original amount, thus reducing the rate of performance decay by 25-fold. Furthermore, the usage of borates, sulfates, and carbonates yields similar results, demonstrating the reliability and universality of the active site dissolution inhibitor, and its role in elevated water electrolysis.
RESUMEN
Seawater electrolysis offers a renewable, scalable, and economic means for green hydrogen production. However, anode corrosion by Cl- pose great challenges for its commercialization. Herein, different from conventional catalysts designed to repel Cl- adsorption, we develop an atomic Ir catalyst on cobalt iron layered double hydroxide (Ir/CoFe-LDH) to tailor Cl- adsorption and modulate the electronic structure of the Ir active center, thereby establishing a unique Ir-OH/Cl coordination for alkaline seawater electrolysis. Operando characterizations and theoretical calculations unveil the pivotal role of this coordination state to lower OER activation energy by a factor of 1.93. The Ir/CoFe-LDH exhibits a remarkable oxygen evolution reaction activity (202 mV overpotential and TOF = 7.46 O2 s-1) in 6 M NaOH+2.8 M NaCl, superior over Cl--free 6 M NaOH electrolyte (236 mV overpotential and TOF = 1.05 O2 s-1), with 100% catalytic selectivity and stability at high current densities (400-800 mA cm-2) for more than 1,000 h.