用于高效 5-hydroxymethylfurfural 电氧化的二维 NiFe LDH/NiFeS 异质结构的界面工程设计

IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Lili Wang , Ya Yan , Rulin Li , Xujie Han , Jiahui Li , Ting Ran , Jialu Li , Baichuan Xiong , Xiaorong Song , Zhaohui Yin , Hong Wang , Qingjun Zhu , Bowen Cheng , Zhen Yin
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引用次数: 0

摘要

将 5-hydroxymethylfurfural (HMF) 电化学氧化为有价值的化学品是提升生物质分子等级和取代传统催化合成的有效方法。开发高效、低成本的富土电催化剂以提高 HMF 氧化的催化性能至关重要。本文通过界面工程构建了一种由镍铁层双氢氧化物(LDH)纳米片和双金属硫化物(NiFeS)组成的新型二维(2D)混合阵列,用于将 HMF 高效电催化氧化为 2,5-呋喃二甲酸(FDCA)。具有超薄异质结构的二维 NiFe LDH/NiFeS 的制备过程包括:通过原位生长将 Co 基金属有机框架(Co MOF)作为模板锚定在碳布(CC)上,在 Co MOF 表面形成 NiFe LDH,然后进行部分硫化。NiFe LDH/NiFeS 电催化剂在 HMF 氧化方面表现出卓越的性能,在 10 mmol/L HMF 的碱性电解液中,FDCA 收率约为 98.5%,法拉第效率(FE)约为 97.2%。此外,即使 HMF 浓度为 100 mmol/L,FDCA 的产率和 FE 仍然很高,分别为 83.6% 和 93.6%。这些发现突出表明,镍铁合金 LDH 纳米片与镍铁合金之间含有丰富界面的二维异质结构可以提高 LDH 的内在活性,从而促进氧化反应动力学。此外,双金属镍铁化合物的协同效应还提高了 HMF 转化为 FDCA 的选择性。我们目前的工作表明,通过界面工程构建镍铁合金 LDH/NiFeS 二维超薄异质结构是提高 LDH 电催化剂内在活性的一种简便策略,这将为低成本、先进的二维纳米催化剂开辟新的途径,从而实现可持续能源转换和生物质衍生物的电化学增值。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Interface engineering of 2D NiFe LDH/NiFeS heterostructure for highly efficient 5-hydroxymethylfurfural electrooxidation

Interface engineering of 2D NiFe LDH/NiFeS heterostructure for highly efficient 5-hydroxymethylfurfural electrooxidation

The electrochemical oxidation of 5-hydroxymethylfurfural (HMF) to valuable chemicals is an efficient way to upgrade biomass molecules and replace traditional catalytic synthesis. It is crucial to develop efficient and low-cost earth-abundant electrocatalysts to enhance catalytic performance of HMF oxidation. Herein, a new type of two-dimensional (2D) hybrid arrays consisting of NiFe layered double hydroxides (LDH) nanosheets and bimetallic sulfide (NiFeS) is constructed via interface engineering for efficient electrocatalytic oxidation of HMF to 2,5-furandicarboxylic acid (FDCA). The preparation process of 2D NiFe LDH/NiFeS with ultrathin heterostructure involves in anchoring a Co-based metal-organic framework (Co MOF) as template onto the carbon cloth (CC) via in-situ growth, formation of NiFe LDH on the surface of Co MOF and subsequent partial sulfidation. The electrocatalyst of NiFe LDH/NiFeS exhibits outstanding performance towards HMF oxidation, about 98.5% yield for FDCA and 97.2% Faraday efficiency (FE) in the alkaline electrolyte with 10 mmol/L HMF, as well as excellent stability retaining 90.1% FE for FDCA after six cycles test. Moreover, even at an HMF concentration of 100 mmol/L, the yield and FE for FDCA remain high at 83.6% and 93.6%, respectively. These findings highlight that 2D heterostructure containing abundant interfaces between NiFe LDH nanosheets and NiFeS can enhance the intrinsic activity of LDH and thus promote the oxidation reaction kinetics. Additionally, the synergistic effect of the bimetallic NiFe compounds also improved the selectivity of HMF conversion to FDCA. Our present work demonstrates that constructing 2D ultrathin heterostructure of NiFe LDH/NiFeS is a facile strategy via interface engineering to enhance the intrinsic activity of LDH electrocatalysts, which would open new avenues toward low-cost and advanced 2D nanocatalysts for sustainable energy conversion and electrochemical valorization of biomass derivatives.

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来源期刊
Chinese Chemical Letters
Chinese Chemical Letters 化学-化学综合
CiteScore
14.10
自引率
15.40%
发文量
8969
审稿时长
1.6 months
期刊介绍: Chinese Chemical Letters (CCL) (ISSN 1001-8417) was founded in July 1990. The journal publishes preliminary accounts in the whole field of chemistry, including inorganic chemistry, organic chemistry, analytical chemistry, physical chemistry, polymer chemistry, applied chemistry, etc.Chinese Chemical Letters does not accept articles previously published or scheduled to be published. To verify originality, your article may be checked by the originality detection service CrossCheck.
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