题目： | Synergistic Active Heterostructure Design for Enhanced Two Electron Oxygen Reduction via Chemical and Electrochemical Reconstruction of Heterosulfides |
作者： | Kai Yu1#, Hongyuan Yang3#, Jie Xu1,4*, Weijie Yuan1, Ruotao Yang1, Meiling Hou5, Zhenhui Kang1*, Yang Liu1, Prashanth W. Menezes2,3* and Ziliang Chen1,2* |
单位： | 1Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-based Functional Materials and Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou 215123, P. R. China. 2Materials Chemistry Group for Thin Film Catalysis–CatLab, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-EinsteinStr. 15, 12489 Berlin, Germany. 3Department of Chemistry: Metalorganics and Inorganic Materials, Technical University of Berlin, Straße des 17 Juni 135. Sekr. C2, 10623 Berlin, Germany. 4College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang, 325035, China. 5College of Engineering, Hebei Normal University, Shijiazhuang, 050024, P. R. China. |
摘要： | Transition metal sulfides, particularly heterostructures, represent a promising class of electrocatalysts for two electron oxygen reduction (2e- ORR), however, understanding the dynamic structural evolution of these catalysts during alkaline ORR remains relatively unexplored. Herein, NiS2/In2.77S4 heterostructure was synthesized as a precatalyst and through a series of comprehensive ex situ and in situ characterizations, including X-ray absorption spectroscopy, Raman spectroscopy, transient photo-induced voltage measurements, electron energy loss spectroscopy, and spherical aberration-corrected electron microscopy, it was revealed that nickel/indium (oxy)hydroxides (NiOOH/In(OH)3) could be evolved from the initial NiS2/In2.77S4 via both electrochemical and chemical-driven methods. The electrochemicaldriven phase featured abundant bridging oxygen-deficient [NiO6]-[InO6] units at the interfaces of NiOOH/In(OH)3, facilitating a synergistic effect between active Ni and In sites, thus enabling an enhanced alkaline 2e- ORR capability than that of chemical-driven process. Remarkably, electrochemically induced NiOOH/In(OH)3 exhibited exceptional performance, achieving H2O2 selectivity of >90% across the wide potential window (up to 0.4 V) with a peak selectivity of >99%. Notably, within the three-electrode flow cell, a current density of 200 mA cm-2 was sustained over 20 h, together with an impressive Faradaic efficiency of ~90% during the whole cycle process. |
影响因子： | 16.1 |
分区情况： | 一区 |
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