RESUMEN
The development of catalysts for an economical and efficient oxygen evolution reaction (OER) is critical for clean and sustainable energy storage and conversion. Nickel-iron-based (NiFe) nanostructures are widely investigated as active OER catalysts and especially shape-controlled nanocrystals exhibit optimized surface structure and electronic properties. However, the structural control from amorphous to well-defined crystals is usually time-consuming and requires multiple stages. Here, a universal two-step precipitation-hydrothermal approach is reported to prepare a series of NiFe-based nanocrystals (e.g., hydroxides, sulfides, and molybdates) from amorphous precipitates. Their morphology and evolution of atomic and electronic structure during this process are studied using conclusive microscopy and spectroscopy techniques. The short-term, additive-free, and low-cost method allows for the control of the crystallinity of the materials and facilitates the generation of nanosheets, nanorods, or nano-octahedra with excellent water oxidation activity. The NiFe-based crystalline catalysts exhibit slightly compromised initial activity but more robust long-term stability than their amorphous counterparts during electrochemical operation. This facile, reliable, and universal synthesis method is promising in strategies for fabricating NiFe-based nanostructures as efficient and economically valuable OER electrocatalysts.
RESUMEN
Anion exchange membrane water electrolysis (AEMWE) is an attractive method for green hydrogen production. It allows the use of non-platinum group metal catalysts and can achieve performance comparable to proton exchange membrane water electrolyzers due to recent technological advances. While current systems already show high performances with available materials, research gaps remain in understanding electrode durability and degradation behavior. In this study, the performance and degradation tracking of a Ni3Fe-LDH-based single-cell is implemented and investigated through the correlation of electrochemical data using chemical and physical characterization methods. A performance stability of 1000 h, with a degradation rate of 84 µV h-1 at 1 A cm-2 is achieved, presenting the Ni3Fe-LDH-based cell as a stable and cost-attractive AEMWE system. The results show that the conductivity of the formed Ni-Fe-phase is one key to obtaining high electrolyzer performance and that, despite Fe leaching, change in anion-conducting binder compound, and morphological changes inside the catalyst bulk, the Ni3Fe-LDH-based single-cells demonstrate high performance and durability. The work reveals the importance of longer stability tests and presents a holistic approach of electrochemical tracking and post-mortem analysis that offers a guideline for investigating electrode degradation behavior over extended measurement periods.
RESUMEN
Nickel (poly)sulfides have been widely studied as anodic catalysts for alkaline water electrolysis owing to their diverse morphologies, high catalytic activities in the oxygen evolution reaction (OER), and low cost. To utilize low-cost and high-efficiency polysulfides with industry-relevant cycling stability, we develop a Ni-rich NiSx/Ni(OH)2/NiOOH catalyst derived from NiS2/Ni3S4 nanocubes. Ni-rich NiSx/Ni(OH)2/NiOOH shows improved OER catalytic activity (η = 374 mV@50 mA cm-2) and stability (0.1% voltage increase) after 65 h of a galvanostatic test at 10 mA cm-2 compared with commercial Ni/NiO and hydrothermally synthesized Ni(OH)2 (both show η > 460 mV@50 mA cm-2 along with 4.40 and 1.92% voltage increase, respectively). A water-splitting electrolyzer based on Pt/C||AF1-HNN8-50||NiSx/Ni(OH)2/NiOOH exhibits a current density of 1800 mA cm-2 at 2.0 V and 500 h high-rate stability at 1000 mA cm-2 with negligible attenuation of only 0.12 mV h-1. This work provides an understanding of truly stable species, intrinsic active phases of Ni polysulfides, their high-rate stability in a real cell, and sheds light on the development of stable chalcogenide-based anodic electrocatalysts for anion exchange membrane water electrolysis (AEMWE).