State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Institute of Functional Materials, Donghua University, 201620, Shanghai, China.
Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202303563. doi: 10.1002/anie.202303563. Epub 2023 Apr 28.
Electrocatalytic water splitting powered by renewable energy is a sustainable approach for hydrogen production. However, conventional water electrolysis may suffer from gas mixing, and the different kinetics between hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) will limit the direct use of unstable renewable energies, leading to increased cost of H production. Herein, a novel phenazine-based compound is synthesized to develop the solid-state redox mediator associated water splititng process, and thus decoupling the H and O production in acid solution without the use of membrane. Excitingly, this organic redox mediator exhibits high specific capacity (290 mAh g at 0.5 A g ), excellent rate performance (186 mAh g at 30 A g ) and long cycle life (3000 cycles) due to its π-conjugated aromatic structure and the fast kinetics of H storage/release process. Furthermore, a membrane-free decoupled water electrolysis architecture driven by solar energy is achieved, demonstrating high-purity H production at different times.
可再生能源驱动的电催化水分解是一种可持续的制氢方法。然而，传统的水电解可能会遭受气体混合的影响，并且析氢反应（HER）和析氧反应（OER）之间的不同动力学特性会限制不稳定可再生能源的直接利用，从而增加 H 生产的成本。在此，合成了一种新型的吩嗪基化合物，以开发与固态氧化还原介体相关的水分解过程，从而在不使用膜的情况下在酸性溶液中解耦 H 和 O 的生产。令人兴奋的是，由于其共轭芳香结构和快速的 H 存储/释放过程动力学，这种有机氧化还原介体表现出高比容量（在 0.5 A g 时为 290 mAh g）、优异的倍率性能（在 30 A g 时为 186 mAh g）和长循环寿命（3000 次循环）。此外，还实现了一种由太阳能驱动的无膜解耦水电解架构，证明了在不同时间内可以高纯度地生产 H。
