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Stabilizing *OH intermediate by fabricating Ni3N‐MoN for scalable 5‐hydroxymethylfurfural electrooxidation
AIChE Journal ( IF 3.5 ) Pub Date : 2024-12-13 , DOI: 10.1002/aic.18690
Shaowei Yang, Ying Guo, Jie Yang, Runze Gao, Zhibei Liao, Haidong Shen, Haoxi Wang, Lifeng Jiang, Buxing Han, Qiuyu Zhang, Hepeng Zhang

Achieving large‐scale coupling of organic electrooxidation and the hydrogen evolution reaction, while understanding the competition between organic electrooxidation and oxygen evolution reaction (OER), is a significant challenge. In this study, using Ni3N‐MoN/NF, an efficient heterojunction electrocatalyst as both anode and cathode in a 50 cm2 continuous flow reactor, we achieved a total current of ~20 A at 2.6 V. This resulted in the highest single‐pass 5‐hydroxymethylfurfural conversion efficiency (0.049 mmol cm−2 min−1) and gram‐level production of 2,5‐furandicarboxylic acid. Theoretical studies revealed that MoN accelerated *OH formation and increased its deprotonation energy barrier, leading to *OH accumulation, effectively promoting organic electrooxidation and inhibiting OER. We anticipate that our foundation in understanding the reaction mechanism and catalyst design strategy can be extended to a wider range of anodic oxidation reactions.

中文翻译:


通过制备 Ni3N-MoN 稳定 *OH 中间体,用于可扩展的 5-羟甲基糠醛电氧化



实现有机电氧化和析氢反应的大规模耦合,同时了解有机电氧化和析氧反应 (OER) 之间的竞争,是一项重大挑战。在这项研究中,在 50 cm2 连续流反应器中使用 Ni3N-MoN/NF(一种高效的异质结电催化剂)作为阳极和阴极,我们在 2.6 V 下实现了 ~20 A 的总电流。这导致最高的单通道 5-羟甲基糠醛转化效率 (0.049 mmol cm-2 min-1) 和 2,5-呋喃二羧酸的克级产生。理论研究表明,MoN 加速了 *OH 的形成,增加了其去质子化能垒,导致 *OH 积累,有效促进有机电氧化和抑制 OER。我们预计,我们理解反应机理和催化剂设计策略的基础可以扩展到更广泛的阳极氧化反应。
更新日期:2024-12-13
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