Zongxi Zhang, Mei Hong, Hui Cao, Yingxiong Wang, Shuai Chen, Yan Qiao
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引用次数: 0
Abstract
The electrooxidation of 5-hydroxymethylfurfural (HMF) to produce value-added chemicals provides an efficient and economical way for the sustainable development of society. However, the development of novel, cost-effective, and environmentally friendly techniques for the synthesis of electrocatalysts to improve HMF oxidation is still a challenge. Herein, we adopted a novel dual modulation strategy based on ionic liquid (IL) regulation to obtain F-doped amorphous nickel molybdenum oxides (NiMoOx/NF-IL). The acquired NiMoOx/NF-IL showed excellent catalytic activity (141.3 mA/cm2@1.40 V vs RHE), stability (20 successive cycles), and high yield and FEFDCA (all over 95%@1.40 V vs RHE) in electrocatalytic HMF oxidation reaction. Specifically, the introduction of an amorphous structure endowed numerous unsaturated sites for the generation of catalytic active sites. Several characterization techniques and theoretical calculation results demonstrated that F doping effectively modulates the coordination environment of the NiOOH active species through its electronegativity, further improving the adsorption behavior of the substrate. The combination of these innate advantages makes NiMoOx/NF-IL exhibit excellent performance in the electrocatalytic oxidation reaction of HMF to 2,5-furandicarboxylic acid.
5-羟甲基糠醛(HMF)电氧化生产增值化学品为社会的可持续发展提供了一条高效、经济的途径。然而,开发新颖、经济、环保的电催化剂合成技术来改善HMF氧化仍然是一个挑战。本文采用一种基于离子液体(IL)调控的新型双调制策略,获得了掺f的非晶镍钼氧化物(NiMoOx/NF-IL)。所获得的NiMoOx/NF-IL在电催化HMF氧化反应中表现出优异的催化活性(141.3 mA/cm2@1.40 V vs RHE)、稳定性(连续20次循环)、高产率和FEFDCA(均大于95%@1.40 V vs RHE)。具体来说,无定形结构的引入为催化活性位点的生成提供了大量的不饱和位点。多种表征技术和理论计算结果表明,F掺杂通过其电负性有效调节NiOOH活性物质的配位环境,进一步改善了底物的吸附行为。这些先天优势的结合使得NiMoOx/NF-IL在HMF的电催化氧化反应中表现出优异的性能。
期刊介绍:
ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment.
The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.