自支撑Ni(OH)2/NF催化剂高效电催化氧化5-羟甲基糠醛反应研究

催化学报 ›› 2024, Vol. 63: 282-291.

• 论文 • 上一篇

自支撑Ni(OH)₂/NF催化剂高效电催化氧化5-羟甲基糠醛反应研究

霍韵滢^a^,¹, 郭聪^a^,¹, 张永乐^a, 刘婧怡^a, 张巧^a^,^*(), 刘芝婷^a, 杨光星^a, 李仁贵^b^,^*(), 彭峰^a^,^*()

^a广州大学化学化工学院, 广东广州 510006
^b中国科学院大连化学物理研究所, 大连洁净能源国家实验室, 催化基础国家重点实验室, 辽宁大连 116023

收稿日期:2024-06-10 接受日期:2024-06-24 出版日期:2024-08-18 发布日期:2024-08-19
通讯作者: *电子信箱: zhangqiao@gzhu.edu.cn (张巧),rgli@dicp.ac.cn (李仁贵),
作者简介:
¹共同第一作者.
基金资助:
中国国家自然科学基金(51706231);广州市自然科学基金(202201020090);大连化学物理研究所催化基础国家重点实验室基金(N-22-10)

Realizing efficient electrochemical oxidation of 5-hydroxymethylfurfural on a freestanding Ni(OH)₂/nickel foam catalyst

Yunying Huo^a^,¹, Cong Guo^a^,¹, Yongle Zhang^a, Jingyi Liu^a, Qiao Zhang^a^,^*(), Zhiting Liu^a, Guangxing Yang^a, Rengui Li^b^,^*(), Feng Peng^a^,^*()

^aSchool of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, Guangdong, China
^bState Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2024-06-10 Accepted:2024-06-24 Online:2024-08-18 Published:2024-08-19
Contact: *E-mail: zhangqiao@gzhu.edu.cn (Q. Zhang), rgli@dicp.ac.cn (R. Li), fpeng@gzhu.edu.cn (F. Peng).
About author:
¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(51706231);Natural Science Foundation of Guangzhou City(202201020090);fund of the State Key Laboratory of Catalysis in DICP(N-22-10)

摘要/Abstract

摘要：

随着太阳能发电能力的不断提高, 如何有效利用可再生太阳能产生的电能对生物质进行电化学转化成为了一个研究热点. 5-羟甲基糠醛(HMF)通过电化学实验转化为生物燃料和高附加值的含氧化学品, 为将可再生电力转化为化学品提供了一条有前途的替代途径. HMF的电催化氧化过程可以产生多种有价值的化学产品, 包括2,5-二甲酰呋喃、5-羟甲基-2-呋喃甲酸、5-甲酰-2-呋喃甲酸和2.5-呋喃二甲酸(FDCA). 其中, FDCA是生物基聚合物如聚乙烯呋喃酸酯的关键单体, 展现出取代石油衍生的聚对苯二甲酸乙二醇酯的潜力. 然而, 尽管镍基催化剂广泛应用于HMF电催化氧化反应, 但其相对较差的导电性和稳定性仍然限制了其潜在的应用.

本文报道了新颖的酸腐蚀诱导策略, 原位构建了自支撑式Ni(OH)₂/NF电极, 研究了腐蚀溶液的浓度和酸蚀时间对泡沫镍电催化氧化HMF性能的影响. 结果表明, 较高的酸浓度和较长的酸蚀时间有利于HMF电化学氧化反应. 酸诱导刻蚀Ni(OH)₂/NF电催化剂表现出稳定、高效的电化学氧化HMF性能, HMF转化率接近100%, FDCA产率与法拉第效率都在90%左右, 催化剂具有良好的稳定性, 连续5次电解循环的Ni(OH)₂/NF催化活性仍然保持稳定. 原位形成策略使Ni(OH)₂与NF之间形成致密的界面, 有助于在电化学反应中保持良好的导电性和稳定性. 原位电化学阻抗测试、原位拉曼和开路电位测试结果表明, 较好的催化性能得益于Ni(OH)₂在HMF氧化过程中动态循环演化为NiOOH, 而HMF分子迅速消耗原位形成的NiOOH物种, 生成FDCA, 同时NiOOH在此过程中被还原为最初的Ni(OH)₂. 将反应体系应用于连续流动电解池装置, 探究了流速、电压对HMF电化学流动池反应体系的影响, 在160 mL min^-1和1.65 V (vs. RHE)的条件下, 该装置能够稳定运行60 h, FDCA的产率高达27 mg h^-1 cm^-2, 表现出较好的应用潜力.

综上, 本文提供了一种简单、经济、易于实施的设计策略, 利用酸腐蚀诱导策略在泡沫镍上原位构建出Ni(OH)₂催化剂并应用于电催化氧化HMF反应中, 探索了镍基催化剂电催化氧化HMF性能, 实现了HMF分子的高效转化, 同时将其应用于小型连续流动电解池体系, 为HMF电化学工业化提供可能性.

关键词: 酸腐蚀诱导, 5-羟甲基糠醛, 电催化氧化, 镍基催化剂

Abstract:

With the continuous improvement of solar energy production capacity, how to effectively use the electricity generated by renewable solar energy for electrochemical conversion of biomass is a hot topic. Electrochemical conversion of 5-hydroxymethylfurfural (HMF) to biofuels and value-added oxygenated commodity chemicals provides a promising and alternative pathway to convert renewable electricity into chemicals. Although nickel-based eletrocatalysts are well-known for HMF oxidation, their relatively low intrinsic activity, poor conductivity and stability still limit the potential applications. Here, we report the fabrication of a freestanding nickel-based electrode, in which Ni(OH)₂ species were in-situ constructed on Ni foam (NF) support using a facile acid-corrosion-induced strategy. The Ni(OH)₂/NF electrocatalyst exhibits stable and efficient electrochemical HMF oxidation into 2,5-furandicarboxylic acid (FDCA) with HMF conversion close to 100% with high Faraday efficiency. In-situ formation strategy results in a compact interface between Ni(OH)₂ and NF, which contributes to good conductivity and stability during electrochemical reactions. The superior performance benefits from dynamic cyclic evolution of Ni(OH)₂ to NiOOH, which acts as the reactive species for HMF oxidation to FDCA. A scaled-up device based on a continuous-flow electrolytic cell was also established, giving stable operation with a high FDCA production rate of 27 mg h^-1 cm^-2. This job offers a straightforward, economical, and scalable design strategy to design efficient and durable catalysts for electrochemical conversion of valuable chemicals.

Key words: Acid-corrosion-induced, 5-Hydroxymethylfurfural, Electrocatalytic oxidation, Ni electrocatalysis

霍韵滢, 郭聪, 张永乐, 刘婧怡, 张巧, 刘芝婷, 杨光星, 李仁贵, 彭峰. 自支撑Ni(OH)₂/NF催化剂高效电催化氧化5-羟甲基糠醛反应研究[J]. 催化学报, 2024, 63: 282-291.

Yunying Huo, Cong Guo, Yongle Zhang, Jingyi Liu, Qiao Zhang, Zhiting Liu, Guangxing Yang, Rengui Li, Feng Peng. Realizing efficient electrochemical oxidation of 5-hydroxymethylfurfural on a freestanding Ni(OH)₂/nickel foam catalyst[J]. Chinese Journal of Catalysis, 2024, 63: 282-291.

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图/表 5

Fig. 1. (a) The schematic diagram of nickel foam. SEM (b) and TEM (c,d) images of Ni(OH)2/NF. The EDS mapping images (e), Ni 2p (f) and O 1s (g) peaks of NF and Ni(OH)2/NF.

Fig. 2. (a) CV curves of NF and Ni(OH)2/NF in 1 mol L-1 KOH at a scan rate of 10 mV s-1. (b) LSV curves of Ni(OH)2/NF in 1 mol L-1 KOH with and without HMF (10 mmol L-1). (c,d) Tafel plot and the electrochemical double-layer capacitance of NF and Ni(OH)2/NF electrodes. (e) HPLC traces of electrochemical HMF oxidation catalyzed by Ni(OH)2/NF at 1.45 V (vs. RHE). (f) Reactant and products concentration-reaction time plots for electrochemical HMF oxidation catalyzed by Ni(OH)2/NF under a 1.45 V (vs. RHE). (g) The HMF conversion, the yield and Faradaic efficiency FDCA based on Ni(OH)2/NF electrode at different potentials. (h) The HMF conversion, the yield and the Faradaic efficiency of FDCA based on NF and Ni(OH)2/NF at 1.45 V (vs. RHE). (i) The HMF conversion, the yield and Faradaic efficiency of FDCA obtained by Ni(OH)2/NF electrode for five consecutive cycles of HMFOR.

Fig. 3. SEM (a), EDS mapping (b) and HRTEM (c) images of Ni(OH)2/NF after reaction. XRD patterns (d), Ni 2p (e) and O 1s (f) peak of Ni(OH)2/NF before and after electrochemical reaction.

Fig. 4. Bode phase plots of the in-situ EIS on Ni(OH)2/NF without 10 mmol L-1 HMF (a) and with 10 mmol L-1 HMF (b). In situ Raman spectra of Ni(OH)2/NF electrode during OER (without 10 mmol L-1 HMF) (c) and HMFOR (with 10 mmol L-1 HMF) (d) under increasing potential from OCP to 1.55 V. (e) Multipotential step curves of the Ni(OH)2/NF electrode. (f) Schematic illustration of the surface reconstruction and reaction mechanism.

Fig. 5. Continuous-flow electrolysis. (a) Electrolysis setup for HMFOR in a continuous-flow electrolytic cell. (b) FDCA productivity based on Ni(OH)2/NF at different potentials, different volume flows in a continuous-flow electrolytic cell. (c,d) HMF conversion, the yield and the productivity of FDCA obtained by Ni(OH)2/NF electrode for six consecutive cycles of HMFOR in a continuous-flow electrolytic cell.

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自支撑Ni(OH)₂/NF催化剂高效电催化氧化5-羟甲基糠醛反应研究

Realizing efficient electrochemical oxidation of 5-hydroxymethylfurfural on a freestanding Ni(OH)₂/nickel foam catalyst

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