pH-Universal Decoupled Water Electrolysis Enabled by Electrocatalytic Hydrogen Gas Capacitive Chemistry

[Image: see text] In conventional water electrolysis (CWE), the H(2) and O(2) evolution reactions (HER/OER) are tightly coupled, making the generated H(2) and O(2) difficult to separate, thus resulting in complex separation technology and potential safety issues. Previous efforts on the design of decoupled water electrolysis mainly concentrated on multi-electrode or multi-cell configurations; however, these strategies have the limitation of involving complicated operations. Here, we propose and demonstrate a pH-universal, two-electrode capacitive decoupled water electrolyzer (referred to as all-pH-CDWE) in a single-cell configuration by utilizing a low-cost capacitive electrode and a bifunctional HER/OER electrode to separate H(2) and O(2) generation for decoupling water electrolysis. In the all-pH-CDWE, high-purity H(2) and O(2) generation alternately occur at the electrocatalytic gas electrode only by reversing the current polarity. The designed all-pH-CDWE can maintain a continuous round-trip water electrolysis for over 800 consecutive cycles with an electrolyte utilization ratio of nearly 100%. As compared to CWE, the all-pH-CDWE achieves energy efficiencies of 94% in acidic electrolytes and 97% in alkaline electrolytes at a current density of 5 mA cm(–2). Further, the designed all-pH-CDWE can be scaled up to a capacity of 720 C in a high current of 1 A for each cycle with a stable HER average voltage of 0.99 V. This work provides a new strategy toward the mass production of H(2) in a facilely rechargeable process with high efficiency, good robustness, and large-scale applications.