Provincial Key Laboratory of Functional Coordination Compounds and Nanomaterials, School of Chemistry and Chemical Engineering , Anqing Normal University , Anqing 246001 , P. R. China.
Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM) , Soochow University , Suzhou 215123 , P. R. China.
ACS Appl Mater Interfaces. 2018 Nov 14;10(45):39161-39167. doi: 10.1021/acsami.8b11970. Epub 2018 Oct 30.
Nitrogen-doped graphene (NG) chemically coupled with graphitic carbon nitride (g-CN) may facilitate the kinetics of overall electrochemical water splitting. Herein, a facile strategy is adopted to synthesize monodispersed Ir nanoparticles on g-CN/NG layers. Benefiting from the synergistic effect between different components of the catalyst, the optimal Ir/g-CN/NG catalyst with a low content of Ir (5.9 wt %) exhibits highly active for electrochemical water splitting in acidic electrolyte. Specifically, as a hydrogen evolution reaction catalyst, the optimal Ir/g-CN/NG exhibits a Tafel slope of 22 mV·dec. The optimal catalyst requires an overpotential of 22 mV to reach the current density of 10 mA·cm, the value of which is superior to Ir/NG (32 mV) and 20 wt % Pt/C (28 mV) catalysts; as an oxygen evolution reaction catalyst, it also achieve the Tafel slope of only 72.8 mV·dec. At the overpotential of 300 mV, the mass activity of the optimal Ir/g-CN/NG catalyst is 2.8 times as large as that of 5.7 wt % Ir/NG catalyst. More significantly, as a bifunctional catalyst, the optimal Ir/g-CN/NG achieves a current density of 10 mA·cm with a potential of only 1.56 V and displays good stability for overall water splitting. This work provides a new strategy to design highly efficient acidic catalysts for electrochemical overall water splitting.
氮掺杂石墨烯(NG)与石墨相氮化碳(g-CN)的化学耦合可能会促进整体电化学水分解的动力学。在此,采用一种简便的策略在 g-CN/NG 层上合成了单分散的 Ir 纳米颗粒。得益于催化剂中不同组分的协同作用,含有低含量 Ir(5.9wt%)的最佳 Ir/g-CN/NG 催化剂在酸性电解质中对电化学水分解具有高活性。具体而言,作为析氢反应催化剂,最佳的 Ir/g-CN/NG 表现出 22 mV·dec 的塔菲尔斜率。最佳催化剂需要 22 mV 的过电势才能达到 10 mA·cm 的电流密度,其值优于 Ir/NG(32 mV)和 20wt%Pt/C(28 mV)催化剂;作为析氧反应催化剂,它也实现了仅 72.8 mV·dec 的塔菲尔斜率。在 300 mV 的过电势下,最佳 Ir/g-CN/NG 催化剂的质量活性是 5.7wt%Ir/NG 催化剂的 2.8 倍。更重要的是,作为一种双功能催化剂,最佳的 Ir/g-CN/NG 在仅 1.56 V 的电势下实现了 10 mA·cm 的电流密度,并显示出良好的整体水分解稳定性。这项工作为设计高效的酸性电化学整体水分解催化剂提供了一种新策略。