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Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic-Nitrogen-Carbon

机译：通过可调谐吡咯基 - 氮碳剪裁电化学过氧化氢的选择性

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摘要

The electrochemical reduction of O-2 via a two-electron reaction pathway to H2O2 provides a possibility for replacing the current anthraquinone process, enabling sustainable and decentralized H2O2 production. Here, a nitrogen-rich few-layered graphene (N-FLG) with a tunable nitrogen configuration is developed for electrochemical H2O2 generation. A positive correlation between the content of pyrrolic-N and the H2O2 selectivity is experimentally observed. The critical role of pyrrolic-N is elucidated by the variable intermediate adsorption profiles as well as the dependent negative shifts of the pyrrolic-N peak on X-ray adsorption near edge structure spectra. By virtue of the optimized N doping configuration and the unique porous structure, the as-fabricated N-FLG electrocatalyst exhibits high selectivity toward electrochemical H2O2 synthesis as well as superior long-term stability. To achieve high-value products on both the anode and cathode with optimized energy efficiency, a practical device coupling electrochemical H2O2 generation and furfural oxidation is assembled, simultaneously enabling a high yield rate of H2O2 at the cathode (9.66 mol h(-1) g(cat)(-1)) and 2-furoic acid at the anode (2.076 mol m(-2) h(-1)) under a small cell voltage of 1.8 V.
机译：通过双电子反应途径对H 2 O 2的O-2电化学还原提供了更换当前的蒽醌工艺，使可持续和分散的H2O2产生的可能性。这里，为电化学H2O2产生开发具有可调谐氮构型的富含富含氮的少数层状石墨烯（N-FLG）。实验观察到吡咯射线-N含量与H2O2选择性之间的正相关性。通过可变中间吸附曲线阐明吡咯的关键作用以及吡咯的滤波器-N峰值在X射线吸附附近近边缘结构光谱附近的依赖性负偏移。借助于优化的N掺杂构造和独特的多孔结构，所制造的N-FLG电催化剂对电化学H2O2合成具有高选择性以及优异的长期稳定性。为了在优化能量效率上实现阳极和阴极上的高价值产物，组装了一种实用的装置耦合电化学H2O2代和糠醛氧化，同时在阴极处能够高产率（9.66molH（-1）g （猫）（ - 1））和在阳极（2.076mol m（-2）h（-1）的2-糠酸下，小电池电压为1.8V。

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