Kirkendall Effect‐Driven Interface Engineering Facilitates Water Dissociation for Dual‐Site H2O2 Electrosynthesis Simultaneously at the Anode and Cathode

作者：Xinhao Cai, Lu Peng, Ping Zhu, Peng Liu, Yuan‐Chu Qin, Zibo Jing, Hao‐Jie Zhu, Chengcheng Huang, Junghyun Son, Ju‐Won Lee, Yanlin Chen, Wenlong Wang, Qian‐Yuan Wu · 发表于：Angewandte Chemie International Edition · 年份：2025 · DOI：10.1002/anie.202512046 · 被引用次数：7 · 研究领域：Electrocatalysts for Energy Conversion、Advanced oxidation water treatment、Electrochemical Analysis and Applications

Abstract The direct integration of renewable energy into H 2 O 2 electrosynthesis systems offers a promising strategy to minimize energy losses and costs. Due to the intermittency of renewable energy, the dual‐site catalysts must efficiently enable both the two‐electron oxygen reduction reaction (2e − ORR) and water oxidation reaction (2e − WOR). The Kirkendall effect was employed to engineer interfaces and construct a NiZnO x ─C catalyst with exposed (100) facets. The hetero‐cluster NiO x induces oxygen vacancies and built‐in electric fields, which facilitate water activation and subsequent formation of hydrogen and hydroxyl radicals, thereby enabling a single catalyst to rapidly electrosynthesize H 2 O 2 at both the anode and cathode. Notably, 2e − ORR on the cathode enabled rapid synthesis of high‐concentration H 2 O 2 (33987 mg L −1 , 33.18 mol g catalyst −1 h −1 ). NiZnO x ─C achieves stable 2e − ORR/WOR coupling in a continuous‐flow reactor, operating reliably for 4 h under simulated alternating current (AC) and peaking at a total Faradaic efficiency of 150.9% under amperage‐level direct currents. This work provides insights into interface engineering based on the Kirkendall effect, demonstrating the feasibility of directly integrating intermittent renewable energy into H 2 O 2 electrosynthesis systems.