Atomic Ru‐Mediated Spontaneous Heterointerface Phase Transition Enables Ampere‐Level Catalytic Performance in Paired Electrolysis
Zhouhong Yu, Xiaonan Zheng, Cong Lin, Han Cheng, Kun Chen, Yun Xiang Tong, Pengzuo Chen, Changzheng Wu
Abstract
Abstract Phase transition regulation is a promising strategy to optimize the catalytic properties of catalysts, playing a crucial role in enhancing electrocatalytic efficiency. However, the intrinsic relationship between atomic‐scale interface phase transitions and catalytic performance remains unclear. Herein, we report a heteroatomic interfacial phase transition of Co 3 S 4 /Co heterostructured nanosheets to Co 9 S 8 /Co by anchoring single‐atom Ru under thermal treatment (Ru SA –Co 9 S 8 /Co–T), resulting in ampere‐level catalytic performance for the sustained paired electrosynthesis. Theoretical calculations and in situ spectroscopy confirm the spontaneous transition to a more stable structure triggered by atomic Ru, which synergistically optimizes the formation kinetics of key intermediates and reduces the energy barrier of the rate‐determining steps on Ru SA ‐Co 9 S 8 /Co–T. Impressively, this catalyst can be directly applied in membrane electrode assembly electrolyzers for nitrite‐glycerol co‐electrolysis. Within a wide potential window of 1.2–2.0 V, the average Faradaic efficiencies of NH 3 and formate exceed 90%, with the highest yields reaching 95.83 mg h −1 cm −2 and 567.38 mg h −1 cm −2 at 2.0 V, respectively, alongside stable operation for 100 h at an industrial current density of 500 mA cm −2 . Our work provides new insights into the development of high‐performance catalysts.