Highly Efficient Electrochemical Synthesis of Hydrogen Peroxide (H2O2) Enabled by Amino Acid Glycine-Derived Metal-Free Nitrogen-Doped Ordered Mesoporous Carbon

过氧化氢 甘氨酸 电化学 碳纤维 无机化学 化学 介孔材料 氮气 金属 氨基酸 材料科学 组合化学 催化作用 有机化学 电极 生物化学 物理化学 复合数 复合材料
作者
Basil Sabri Rawah,Mohammad Albloushi,Wenzhen Li
出处
期刊:ACS Sustainable Chemistry & Engineering [American Chemical Society]
卷期号:10 (17): 5453-5462 被引量:16
标识
DOI:10.1021/acssuschemeng.1c08285
摘要

Electrocatalytic partial oxygen reduction has been considered a more sustainable approach to the synthesis of hydrogen peroxide (H2O2), as compared with current industrial anthraquinone processes. One key research need is to explore low-cost active electrocatalysts. Here, we report a facile, solvent-free method to synthesize a metal-free nitrogen-doped ordered mesoporous carbon (N-OMC) by in situ transforming of glycine (carbon and nitrogen precursors) in the mesoporous SiO2 template (KIT-6) followed by subsequent thermal treatment at different temperatures. Among all samples, the catalyst treated at 800 °C (N-OMC-800), the nitrogen-rich carbon, exhibits outstanding structural properties and porosity, showing the dominant formation of pyrrolic-N and graphitic-N. With combined improved structural properties with the optimal ratio of N-pyrrolic/N-graphitic, P/G carbon provided an outstanding electrocatalytic activity, promoting H2O2 with high selectivity and production rate in alkaline mediums. The N-OMC-800 can achieve a faradaic efficiency (FE) of ∼100% to H2O2 at (0.6 VRHE to 0.4 VRHE) in a H-cell containing 0.1 M KOH. Furthermore, its bulk H2O2 electrosynthesis in our self-designed flow cell confirmed its practical capability by showing a remarkable H2O2 production rate of 9.43 mol gcat–1 h–1 at 0.35 VRHE and maintaining nearly 100% FE at the cathode potential of 0.6 VRHE for 12 h without any degradation.
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