Reactive metals hydrolysis offers significant advantages for hydrogen storage and production. However, the regeneration of common reactive metals (e.g., Mg, Al, etc.) is energy-intensive and produces unwanted byproducts such as CO and Cl. Herein, we employ Zn as a reactive mediator that can be easily regenerated by electrolysis of ZnO in an alkaline solution with a Faradaic efficiency of >99.9 %. H is produced in the same electrolyte by constructing a Zn-HO hydrolysis battery consisting of a Zn anode and a Raney-Ni cathode to unlock the Zn-HO reaction. The entire two-step water splitting reaction with a net energy efficiency of 70.4 % at 80 °C and 50 mA cm. Additionally, the Zn-HO system can be charged using renewable energy to produce H on demand and runs for 600 cycles only sacrificing 3.76 % energy efficiency. DFT calculations reveal that the desorption of H* on Raney-Ni (-0.30 eV) is closer to zero compared with that on Zn (-0.87 eV), indicating a faster desorption of H* at low overpotential. Further, a 24 Ah electrolyzer is demonstrated to produce H with a net energy efficiency of 65.5 %, which holds promise for its real application.
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http://dx.doi.org/10.1002/anie.202404025 | DOI Listing |
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