题目： | Phase Reconstruction-Directed Synthesis of Oxalate-Functionalized Nickel Hydroxide Electrocatalyst for High-Yield H2O2 Generation at Industrial Currents |
作者： | Zhiwei Liu1, Weijie Yuan1, Hongyuan Yang2, Zhenhui Kang1*, Mengjie Ma1, Prashanth W. Menezes2,3* & Ziliang Chen1,3* |
单位： | 1Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, 199 Ren’ai Road, Suzhou, Jiangsu 215123, China. 2Department of Chemistry: Metalorganics and Inorganic Materials Technische Universität Berlin, Straße des 17 Juni 135, Sekr. C2, 10623 Berlin, Germany. 3Material Chemistry Group for Thin Film Catalysis–CatLab Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany. |
摘要： | The electrochemical oxygen reduction reaction (2e− ORR) offers a promising approach for H2O2 production, yet developing highly active, selective, and stable electrocatalysts remains a challenge. In this work, a phase reconstruction strategy is presented to synthesize an oxalate-adsorbed nickel hydroxide electrocatalyst (Ni(OH)2-C2O4) through the self-dissociation of nickel oxalate in an alkaline medium, leading to a notable enhancement in H2O2 yield at elevated current densities. Remarkably, Ni(OH)2-C2O4 exhibits a 2e− selectivity exceeding 93% across a broad voltage range (0.0 to 0.5 V vs. RHE) in 0.1 M KOH, outperforming pristine Ni(OH)2. When deployed as a gas diffusion electrode in a flow cell, the Ni(OH)2-C2O4 catalyst demonstrates stable operation for 50 h at 200 mA cm−2, with a Faradaic efficiency surpassing 90% and a peak H2O2 yield of 6.2 mol g−1cat h−1. Comprehensive advanced characterizations, including in situ Raman spectroscopy, transient photovoltage spectra, and transient potential scanning spectra, coupled with post-ORR analyses, reveal that surface-adsorbed oxalate groups on Ni(OH)2 enhance the interfacial reaction kinetics between active Ni sites and reactants by inducing a charge trapping effect and forming a hydrogen-bonded network, facilitating robust and high-yield H2O2 production. |
影响因子： | 18.5 |
分区情况： | 一区 |
链接： | https://doi.org/10.1002/adfm.202412198 责任编辑：杜欣 |