Junda Lu, Chao Hong, Guoyang Li, Xuerong Zheng, Zexiang Yin, Jinfeng Zhang, Yan Dong, Haozhi Wang, Yang Wang, Yida Deng
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引用次数: 0
摘要
海水电池(SWB)作为海洋电气设备的下一代能源供应系统具有巨大潜力。然而,海水中的低氧浓度和有害的 Cl- 吸附及腐蚀阻碍了其效率和耐用性。本文开发了一种主-客策略,在掺氮碳上制造具有相邻 Co 和 Ni 位点的二原子催化剂(CoNi-DAC),其中 Co 和 Ni 原子分别与三个氮原子配位。理论计算和原位表征显示,Co 和 Ni 价态的同步还原通过优化 O2 吸附能垒、促进 O─O 键的直接裂解和防止 *OOH 中间体的形成,增强了 ORR 动力学。这种电子调制增强了亲氧性和抗 Cl- 腐蚀性。Co/Ni 二原子位点协同提高了 ORR 催化活性,使半波电位(E1/2)达到 0.79 V,并在天然海水中实现了近 700 小时的超长耐久性。使用 CoNi-DAC 涂层碳刷电极组装的 SWB 达到了 3.3 W L-1 的峰值功率密度。这项研究为设计和开发适用于天然海水环境的先进 ORR 电催化剂提供了宝贵的启示。
Building Cobalt-Nickel Diatomic Sites as Oxygenophilic ORR Catalyst with Strong Cl−-Corrosion Resistance for Seawater Batteries
The seawater battery (SWB) holds great potential as the next-generation energy supply system for marine electrical equipment. However, its efficiency and durability are hindered by low oxygen concentration and harmful Cl− adsorption and corrosion in seawater. Herein, a host-guest strategy is developed to fabricate diatomic catalysts with adjacent Co and Ni sites on nitrogen-doped carbon (CoNi-DAC), where Co and Ni atoms are each coordinated to three nitrogen atoms. Theoretical calculations and in situ characterization reveal that the synchronized reduction of Co and Ni valence states enhances ORR kinetics by optimizing the O2 adsorption energy barrier, facilitating direct O─O bond cleavage and preventing *OOH intermediate formation. This electronic modulation enhances oxygenophilicity and Cl− corrosion resistance. The Co/Ni diatomic sites synergistically improve ORR catalytic activity, achieving a half-wave potential (E1/2) of 0.79 V and exceptional long-term durability of nearly 700 h in natural seawater. The assembled SWB with CoNi-DAC coated carbon brush electrode attains a peak power density of 3.3 W L−1. This work offers valuable insights into the design and development of advanced ORR electrocatalysts for natural seawater environments.
期刊介绍:
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