Self-Supported Electrocatalysts for Practical Water Electrolysis

Constructing an electrocatalyst with highly durable active and cost-effective core-shell with a porous carbon nanosheet for the development of high efficiency energy conversion and storage devices. Herein, we developed core-shell nickel-iron oxide on a highly porous N-doped carbon nanosheet (CS-NFO@PNC) via a facile solvothermal calcination route. The optimized CS-NFO@PNC-700 showed remarkable electrocatalytic activity towards ORR (0.85 V vs RHE), OER ƞ10 = 217 mV, and HER ƞ10 = 200 mV with excellent durability towards the corresponding half-cell reactions. Further, we investigated the ORR, OER, and HER mechanistic pathways of the electrocatalyst using the density functional theory. Finally, we fabricated a rechargeable liquid electrolyte-based zinc–air battery with CS-NFO@PNC-700 as the cathode which displayed an improved power density of 130 mW cm−2 at 217 mA cm−2 with excellent durability of 180 h. The rechargeable flexible quasi-solid-state zinc–air battery with CS-NFO@PNC-700 air cathode, which exhibited excellent long term durability over 40 h at 5 mA cm−2.

Rational design of multifunctional electrocatalyst: An approach towards efficient overall water splitting and rechargeable flexible solid-state zinc–air battery

The development of a high-performance electrocatalyst for oxygen evolution reaction (OER) is imperative but challenging. Here, a partial sulfidation route to construct Ni2Fe-LDH/FeNi2S4 heterostructure on nickel foam (Ni2Fe-LDH/FeNi2S4/NF) by adjusting the hydrothermal duration is reported. The heterostructures afford abundant hydroxide/sulfide interfaces that offer plentiful active sites, rapid charge and mass transfer, favorable adsorption energy to oxygenated species (OH− and OOH) evidenced by the density functional theory calculations, which synergistically boost the alkaline water oxidation. In the 1.0 m KOH solution, Ni2Fe-LDH/FeNi2S4/NF exhibits an excellent OER catalytic activity with a much smaller overpotential (240 mV) to reach the current density of 100 mA cm−2 than single-phase Ni2Fe-LDH/NF (279 mV) or FeNi2S4/NF (271 mV). More impressively, 2000 cycles of cyclic voltammetry scan for water oxidation results in the formation of a sulfate layer over the catalyst. The corresponding post-catalyst demonstrates better OER activity and durability than the initial one in the alkaline simulated seawater electrolyte. The post-Ni2Fe-LDH/FeNi2S4/NF delivers smaller overpotential (250 mV) at 100 mA cm−2 and longer stability time than the original form (260 mV). The post-formed sulfate passivating layer is responsible for the outstanding corrosion resistance of the salty-water oxidation anode since it can effectively repel chloride. 

Partial Sulfidation Strategy to NiFe‐LDH@FeNi 2 S 4 Heterostructure Enable High‐Performance Water/Seawater Oxidation

Employing seawater splitting systems to generate hydrogen can be economically advantageous but still remains challenging, particularly for designing efficient and high Cl−‐corrosion resistant trifunctional catalysts toward the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Herein, single CoNC catalysts with well‐defined symmetric CoN4 sites are selected as atomic platforms for electronic structure tailoring. Density function theory reveals that P‐doping into CoNC can lead to the formation of asymmetric CoN3P1 sites with symmetry‐breaking electronic structures, enabling the affinity of strong oxygen‐containing intermediates, moderate H adsorption, and weak Cl− adsorption. Thus, ORR/OER/HER activities and stability are optimized simultaneously with high Cl−‐corrosion resistance. The asymmetric CoN3P1 structure based catalyst with boosted ORR/OER/HER performance endows seawater‐based Zn–air batteries (S‐ZABs) with superior long‐term stability over 750 h and allows seawater splitting to operate continuously for 1000 h. A self‐driven seawater splitting powered by S‐ZABs gives ultrahigh H2 production rates of 497 μmol h−1. This work is the first to advance the scientific understanding of the competitive adsorption mechanism between Cl− and reaction intermediates from the perspective of electronic structure, paving the way for synthesis of efficient trifunctional catalysts with high Cl−‐corrosion resistance.

Asymmetric CoN3P1 Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System

Recent progress in transition-metal-oxide-based electrocatalysts for the oxygen evolution reaction in natural seawater splitting: A critical review

Development of efficient non-precious catalysts for seawater electrolysis is of great significance but challenging due to the sluggish kinetics of oxygen evolution reaction (OER) and the impairment of chlorine electrochemistry at anode. Herein, we report a heterostructure of Ni3S2 nanoarray with secondary Fe-Ni(OH)2 lamellar edges that exposes abundant active sites towards seawater oxidation. The resultant Fe-Ni(OH)2/Ni3S2 nanoarray works directly as a free-standing anodic electrode in alkaline artificial seawater. It only requires an overpotential of 269 mV to afford a current density of 10 mA·cm−2 and the Tafel slope is as low as 46 mV·dec−1. The 27-hour chronopotentiometry operated at high current density of 100 mA·cm−2 shows negligible deterioration, suggesting good stability of the Fe·Ni(OH)2/Ni3S2@NF electrode. Faraday efficiency for oxygen evolution is up to ∼ 95%, revealing decent selectivity of the catalyst in saline water. Such desirable catalytic performance could be benefitted from the introduction of Fe activator and the heterostructure that offers massive active and selective sites. The density functional theory (DFT) calculations indicate that the OER has lower theoretical overpotential than Cl2 evolution reaction in Fe sites, which is contrary to that of Ni sites. The experimental and theoretical study provides a strong support for the rational design of high-performance Fe-based electrodes for industrial seawater electrolysis.

Heterogeneous lamellar-edged Fe-Ni(OH) 2 /Ni 3 S 2 nanoarray for efficient and stable seawater oxidation

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Heterogeneous lamellar-edged Fe-Ni(OH) 2 /Ni 3 S 2 nanoarray for efficient and stable seawater oxidation