One-step in-situ synthesis of nickel–cobalt sulfide catalysts for ultra-efficient electrooxidation of 5-hydroxymethylfurfural

IF 4.1 2区 工程技术 Q2 ENGINEERING, CHEMICAL Chemical Engineering Science Pub Date : 2024-11-08 DOI:10.1016/j.ces.2024.120919
Lili Geng , Sen Li , Haifeng Shi , Ruijie Li , Yongming Zeng , Ley Boon Sim , Binghui Chen
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Abstract

This study presents Ni7Co3-S achieving 99.2 % HMF conversion, 96.1 % FDCA yield, and 98.5 % Faradaic efficiency at 1.45 V, with FDCA rates at 266.7 µmol cm-2h−1 in a 30 mL, 20 mM HMF electrolyte. At the same operational potential, this catalyst achieved a current density of 105 mA cm−2 in 1 M KOH with 20 mM HMF, outperforming 26mA cm−2 of Ni7Co3-O. Linear sweep voltammetry (LSV) analysis reveals that Ni7Co3-S has an onset potential of 1.16 V, which is 90 mV lower than Ni7Co3-O. With a Tafel slope of 89.1 mV dec-1, versus 110.3 mV dec-1 for Ni7Co3-O, Ni7Co3-S exhibits quicker reaction kinetics. Additionally, Ni7Co3-S boasts double-layer capacitance twice that of Ni7Co3-O, while sulfidation decreases in Ni2+ and Co3+ alongside an increase in Ni3+ and Co2+, suggesting enhanced electron transfer from Ni to Co. These insights offer a strategy for developing high-performance, non-precious catalysts for HMF electrooxidation.

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一步原位合成用于 5-羟甲基糠醛超高效电氧化的硫化镍钴催化剂
本研究显示,在 30 mL、20 mM HMF 电解液中,Ni7Co3-S 在 1.45 V 电压下可实现 99.2 % 的 HMF 转化率、96.1 % 的 FDCA 产率和 98.5 % 的 Faradaic 效率,FDCA 速率为 266.7 µmol cm-2h-1。在相同的操作电位下,这种催化剂在 1 M KOH 和 20 mM HMF 溶液中的电流密度达到 105 mA cm-2,超过了 Ni7Co3-O 的 26mA cm-2。线性扫描伏安法(LSV)分析表明,Ni7Co3-S 的起始电位为 1.16 V,比 Ni7Co3-O 低 90 mV。Ni7Co3-S 的塔菲尔斜率为 89.1 mV dec-1,而 Ni7Co3-O 为 110.3 mV dec-1,因此 Ni7Co3-S 的反应动力学更快。此外,Ni7Co3-S 的双层电容是 Ni7Co3-O 的两倍,而 Ni2+ 和 Co3+ 的硫化程度降低,同时 Ni3+ 和 Co2+ 的硫化程度升高,这表明从 Ni 到 Co 的电子转移得到了加强。这些见解为开发用于 HMF 电氧化的高性能非贵金属催化剂提供了一种策略。
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来源期刊
Chemical Engineering Science
Chemical Engineering Science 工程技术-工程:化工
CiteScore
7.50
自引率
8.50%
发文量
1025
审稿时长
50 days
期刊介绍: Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.
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