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康振辉教授、陈子亮副教授及其合作者在Adv. Funct. Mater上发表论文
发布时间:2024-11-08 点击:195

题目:

Phase Reconstruction-Directed Synthesis of Oxalate-Functionalized Nickel Hydroxide Electrocatalyst for High-Yield H2O2Generation 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 CatalysisCatLab Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.

摘要:

The electrochemical oxygen reduction reaction (2eORR) offers a promising approach for H2O2production, 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 H2O2yield at elevated current densities. Remarkably, Ni(OH)2-C2O4exhibits a 2eselectivity 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-C2O4catalyst demonstrates stable operation for 50 h at 200 mA cm−2, with a Faradaic efficiency surpassing 90% and a peak H2O2yield of 6.2 mol g−1cath−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)2enhance 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 H2O2production.

影响因子:

18.5

分区情况:

一区

链接:

https://doi.org/10.1002/adfm.202412198


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