Nanoscale Heterogeneities of Non-Noble Iron-Based Metallic Glasses toward Efficient Water Oxidation at Industrial-Level Current Densities

作者：Jia, Zhe; Zhao, Yilu; Wang, Qing; Lyu, Fucong; Tian, Xiaobao; Liang, Shun-Xing; Zhang, Lai-Chang; Luan, Junhua; Wang, Qianqian; Sun, Ligang^*; Yang, Tao^*; Shen, Baolong^*

来源：ACS applied materials & interfaces, 2022, 14(8): 10288-10297.

DOI：10.1021/acsami.1c22294

• metallic glasses
• heterogeneity
• chemical complexity
• water oxidation
• metallurgy

Scaling up the production of cost-effective electrocatalysts for efficient water splitting at the industrial level is critically important to achieve carbon neutrality in our society. While noble-metal-based materials represent a high-performance benchmark with superb activities for hydrogen and oxygen evolution reactions, their high cost, poor scalability, and scarcity are major impediments to achieve widespread commercialization. Herein, a flexible freestanding Fe-based metallic glass (MG) with an atomic composition of Fe50Ni30P13C7 was prepared by a large-scale metallurgical technique that can be employed directly as a bifunctional electrode for water splitting. The surface hydroxylation process created unique structural and chemical heterogeneities in the presence of amorphous FeOOH and Ni2P as well as nanocrystalline Ni2P that offered various active sites to optimize each rate-determining step for water oxidation. The achieved overpotentials for the oxygen evolution reaction were 327 and 382 mV at high current densities of 100 and 500 mA cm(-2) in alkaline media, respectively, and a cell voltage of 1.59 V was obtained when using the MG as both the anode and the cathode for overall water splitting at a current density of 10 mA cm(-2). Theoretical calculations unveiled that amorphous FeOOH makes a significant contribution to water molecule adsorption and oxygen evolution processes, while the amorphous and nanocrystalline Ni2P stabilize the free energy of hydrogen protons (Delta G(H*)) in the hydrogen evolution process. This MG alloy design concept is expected to stimulate the discovery of many more high-performance catalytic materials that can be produced at an industrial scale with customized properties in the near future.

• 单位
  四川大学; 上海大学