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The proton exchange membrane water electrolyzer (PEMWE) is one of the most promising electrochemical energy conversion devices for hydrogen production, while still limited by performance bottlenecks at high current densities, due to the lack of mass transfer insights. To investigate the mechanisms of oxygen transport inside the PEMWE at high current density and its relation to electrolytic performance. Operational in situ x‐ray imaging is utilized to simultaneously characterize the bubble behavior and voltage response in a novel designed visual mini‐cell, and it is identified that oxygen evolution and transport in the PEMWE follow the process of bubble nucleation, growth, and detachment. Based on the results of mini‐cells with three porous transport layers (PTLs) up to 9 A cm−2 operation, it revealed that critical current densities exist for both carbon‐based and titanium‐based PTLs. Once exceeding the critical current density, the cell voltage can no longer be stabilized and the cell exhibits a significant oxygen overpotential. To illustrate this, the concept of interfacial separation zone (ISZ) is first proposed, which is an effective pathway for bubble growth and separation and the pattern of the ISZ exhibits specific regimes with the critical current density. Ultimately, a new approach for better understanding the mechanisms of oxygen transport is revealed.
The proton exchange membrane water electrolyzer (PEMWE) is one of the most promising electrochemical energy conversion devices for hydrogen production, while still limited by performance bottlenecks at high current densities, due to the lack of mass transfer insights. To investigate the mechanisms of oxygen transport inside the PEMWE at high current density and its relation to electrolytic performance. Operational in situ x‐ray imaging is utilized to simultaneously characterize the bubble behavior and voltage response in a novel designed visual mini‐cell, and it is identified that oxygen evolution and transport in the PEMWE follow the process of bubble nucleation, growth, and detachment. Based on the results of mini‐cells with three porous transport layers (PTLs) up to 9 A cm−2 operation, it revealed that critical current densities exist for both carbon‐based and titanium‐based PTLs. Once exceeding the critical current density, the cell voltage can no longer be stabilized and the cell exhibits a significant oxygen overpotential. To illustrate this, the concept of interfacial separation zone (ISZ) is first proposed, which is an effective pathway for bubble growth and separation and the pattern of the ISZ exhibits specific regimes with the critical current density. Ultimately, a new approach for better understanding the mechanisms of oxygen transport is revealed.
In recent years, catalysts based on transition metal sulfides have garnered extensive attention due to their low cost and excellent electrocatalytic activity in the alkaline oxygen evolution reaction. Here, the preparation of Fe‐doped Ni3S2 via a one‐step hydrothermal approach is reported by utilizing inexpensive transition metals Ni and Fe. In an alkaline medium, Fe–Ni3S2 exhibits outstanding electrocatalytic activity and stability for the OER, and the current density can reach 10 mA cm−2 with an overpotential of 163 mV. In addition, Pt/C||Fe–Ni3S2 is used as the membrane electrode of the anion exchange membrane water electrolyzer, which is capable of providing a current density of 650 mA cm−2 at a cell voltage of 2.0 V, outperforming the benchmark Ir/C. The principle is revealed that the doping of Fe enhances the electrocatalytic water decomposition ability of Ni3S2 by in situ Raman and in situ X‐ray absorption fine structure. The results indicate that the doping of Fe decreases the charge density near Ni atoms, which renders Fe–Ni3S2 more favorable for the adsorption of OH− and the formation of *OO− intermediates. This work puts forward an effective strategy to significantly improve both the alkaline OER activity and stability of low‐cost electrocatalysts.
Developing efficient electrocatalysts is significant for the commercial application of electrocatalytic water splitting. 2D materials have presented great prospects in electrocatalysis for their high surface‐to‐volume ratio and tunable electronic properties. Particularly, MXene emerges as one of the most promising candidates for electrocatalysts, exhibiting unique advantages of hydrophilicity, outstanding conductivity, and exceptional stability. However, it suffers from lacking catalytic active sites, poor oxidation resistance, and easy stacking, leading to a significant suppression of the catalytic performance. Combining MXene with other 2D materials is an effective way to tackle the aforementioned drawbacks. In this review, the focus is on the accurate synthesis of 2D/2D MXene‐based catalysts toward electrocatalytic water splitting. First, the mechanisms of electrocatalytic water splitting and the relative properties and preparation methods of MXenes are introduced to offer the basis for accurate synthesis of 2D/2D MXene‐based catalysts. Then, the accurate synthesis methods for various categories of 2D/2D MXene‐based catalysts, such as wet‐chemical, phase‐transformation, electrodeposition, etc., are systematically elaborated. Furthermore, in‐depth investigations are conducted into the internal interactions and structure‐performance relationship of 2D/2D MXene‐based catalysts. Finally, the current challenges and future opportunities are proposed for the development of 2D/2D MXene‐based catalysts, aiming to enlighten these promising nanomaterials for electrocatalytic water splitting.
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