Stabilizing *OH intermediate by fabricating Ni3N-MoN for scalable 5-hydroxymethylfurfural electrooxidation

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal 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

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引用次数: 0

Abstract

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.

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通过制备Ni3N-MoN来稳定*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，同时理解有机电氧化和析氧反应（OER）之间的竞争是一个重大挑战。在本研究中，采用高效异质结电催化剂Ni3N-MoN/NF作为阳极和阴极，在50 cm2的连续流反应器中，我们在2.6 V下获得了~20 a的总电流。这导致了最高的单道5-羟甲基糠醛转化效率（0.049 mmol cm−2 min−1）和克级2,5-呋喃二羧酸的生产。理论研究表明，MoN加速*OH的形成，增加其去质子能垒，导致*OH积聚，有效促进有机电氧化，抑制OER。我们期望我们在了解反应机理和催化剂设计策略方面的基础可以扩展到更广泛的阳极氧化反应。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.