基于Ag与NiFe-LDH协同作用实现电催化PET碱性水解产物选择性制备甲酸盐与乙醇酸盐

doi:10.1016/S1872-2067(25)64819-4

催化学报 ›› 2026, Vol. 80: 282-292.DOI: 10.1016/S1872-2067(25)64819-4

基于Ag与NiFe-LDH协同作用实现电催化PET碱性水解产物选择性制备甲酸盐与乙醇酸盐

马毅^a^,^b, 葛欢^a^,^b, 章勇^a^,^b, 简宁^a^,^b, 唐嘉陵^c, 胡宗坤^c, 于静^d^,^e, 李灿煌^d, 李露明^a, 李军山^a^,^b^,^d^,^*()

^a成都大学高等研究院, 四川成都 610106, 中国
^b成都大学机械工程学院, 四川成都 610106, 中国
^c成都大学建筑与土木工程学院, 四川成都 610106, 中国
^d加泰罗尼亚能源研究所(IREC), 巴塞罗那, 西班牙
^e加泰罗尼亚纳米科学与纳米技术研究所(ICN2), 巴塞罗那, 西班牙
^f加泰罗尼亚高等研究所(ICREA), 巴塞罗那, 西班牙

收稿日期:2025-06-24 接受日期:2025-07-27 出版日期:2026-01-05 发布日期:2026-01-05
通讯作者: 李军山
基金资助:
国家自然科学基金(22579020);四川省科技计划(2025ZNSFSC0139);中国博士后科学基金(2023MD734228)

Electrooxidation of PET alkaline hydrolysate to formate and glycolate enabled by the synergistic interaction of Ag and NiFe-LDH

Yi Ma^a^,^b, Huan Ge^a^,^b, Yong Zhang^a^,^b, Ning Jian^a^,^b, Jialing Tang^c, Zongkun Hu^c, Jing Yu^d^,^e, Jordi Arbiol^e^,^f, Canhuang Li^d, Luming Li^a, Andreu Cabot^d^,^f^,^*(), Junshan Li^a^,^b^,^d^,^*()

^aInstitute for Advanced Study, Chengdu University, Chengdu 610106, Sichuan, China
^bSchool of Mechanical Engineering, Chengdu University, Chengdu, 610106, Sichuan, China
^cDepartment of Environmental Engineering, School of Architecture and Civil Engineering, Chengdu University, Chengdu 610106, Sichuan, China
^dCatalonia Institute for Energy Research − IREC, Sant Adrià de Besòs, 08930 Barcelona, Catalonia, Spain.
^eCatalan Institute of Nanoscience and Nanotechnology-ICN2 (CSIC and BIST), Campus UAB, 08193 Bellaterra, Barcelona, Catalonia, Spain
^fICREA, Pg. Lluís Companys 23, 08010 Barcelona, Catalonia, Spain

Received:2025-06-24 Accepted:2025-07-27 Online:2026-01-05 Published:2026-01-05
Contact: Andreu Cabot, Junshan Li
Supported by:
National Natural Science Foundation of China(22579020);Sichuan Science and Technology Program(2025ZNSFSC0139);China Postdoctoral Science Foundation(2023MD734228)

摘要/Abstract

摘要：

废弃塑料对生态系统和人类健康构成重大威胁, 亟需开发高效、低成本的方法将其转化为高附加值产品.聚对苯二甲酸乙二醇酯(PET)作为广泛使用的塑料之一, 年产量约为7000万吨, 回收率不到20%. 通过传统的物理法回收PET塑料产生的附加值较低,因此, 化学方法回收升级再利用PET塑料显得尤为重要.相比之下, 化学回收对废弃塑料的升值回收有望在减轻塑料污染的同时, 实现塑料资源的高效利用. 其中, 碱性水解能在较温和条件下将PET废塑料降解为对苯二甲酸和乙二醇单体. 在此基础上, 结合电转化方法能够利用可再生电能生产高价值化学品和氢气的优势,这种耦合反应是PET废弃物资源化的重要研究方向之一. 然而, 现有技术中贵金属催化剂成本高、稳定性不足等问题限制了其工业化应用, 因此开发低成本、高性能的电催化剂具有重要的理论与实际意义.

本文以设计和合成先进的电催化材料为切入点, 旨在大电流密度下实现PET水解产物在阳极(正极)的选择性氧化为高附件值产物, 并耦合阴极(负极)的电解水制氢过程. 因此, 本研究设计了一种新型异质结构催化剂, 通过水热法与光沉淀法在泡沫镍(NF)基底上合成了银(Ag)纳米颗粒锚定在镍铁层状双氢氧化物(NiFe-LDH)纳米片阵列上的复合催化剂(Ag/NiFe-LDH/NF), 利用Ag与NiFe-LDH的协同作用实现PET水解产物EG的高效电氧化. 结果表明, 该催化剂在PET碱性水解体系中表现出优异的乙二醇氧化反应性能: 在1.5 V (vs. RHE)的低电位下, 电流密度高达120 mA cm^-², 且稳定性良好; 对目标产物甲酸根和乙醇酸根的法拉第效率分别达到85%和13%, 展现出较高的选择性. 密度泛函理论计算揭示了其催化机制: Ag与NiFe-LDH形成的Ag/NiFe-OOH界面促进了电荷积累, 不仅优化了EG在催化位点的吸附能力, 还降低了反应决速步的过电势, 从而协同提升了催化剂的活性、选择性与稳定性. 由此可见, Ag的引入有效平衡了催化活性与成本, 结合NiFe-LDH的层状结构为反应提供了丰富的活性位点, 二者的协同作用是实现高效转化以及选择性氧化的核心.

综上, 本文开发的Ag/NiFe-LDH/NF催化剂为废弃PET的高值化利用提供了可持续策略, 不仅实现了塑料废弃物到甲酸根等高价值化学品的转化, 还可同步产氢, 为“废弃物-能源-化学品”闭环体系的构建奠定了基础. 该工作为设计低成本、高性能电催化剂提供了新思路, 有望推动塑料废弃物电化学资源化技术的工业化发展.

关键词: 乙二醇氧化反应, 电催化重整, 聚对苯二甲酸乙二醇酯, 塑料回收, 甲酸, 协同效应

Abstract:

Waste plastics present a significant threat to ecosystems and human health, necessitating efficient and cost-effective solutions for their conversion into high-value products. This study introduces a novel electrochemical reforming strategy to upgrade polyethylene terephthalate (PET) into valuable chemicals, primarily formic acid, while simultaneously generating hydrogen. A highly efficient electrocatalyst composed of nano-arrays of silver and NiFe layered double hydroxide (LDH) is synthesized via a hydrothermal and photo-precipitation process on a nickel foam substrate. This advanced catalyst achieves selective electrochemical conversion of ethylene glycol (EG) as PET hydrolysate to formate and glycolate with Faradaic efficiencies of 85% and 13% at 1.5 V vs. the reversible hydrogen electrode, with a stable and high current density. Density functional theory calculations reveal that the synergistic interaction between Ag and NiFe-LDH optimizes the adsorption and desorption of key intermediates on the catalytic sites, resulting in superior activity, selectivity, and stability for the electrochemical EG oxidation reaction. These findings highlight the potential of this catalyst for sustainable plastic waste valorization and renewable hydrogen production.

Key words: Ethylene glycol oxidation reaction, Electrocatalytic reforming, Polyethylene terephthalate, Plastic removal, Formic acid, Synergistic effect

马毅, 葛欢, 章勇, 简宁, 唐嘉陵, 胡宗坤, 于静, 李灿煌, 李露明, 李军山. 基于Ag与NiFe-LDH协同作用实现电催化PET碱性水解产物选择性制备甲酸盐与乙醇酸盐[J]. 催化学报, 2026, 80: 282-292.

Yi Ma, Huan Ge, Yong Zhang, Ning Jian, Jialing Tang, Zongkun Hu, Jing Yu, Jordi Arbiol, Canhuang Li, Luming Li, Andreu Cabot, Junshan Li. Electrooxidation of PET alkaline hydrolysate to formate and glycolate enabled by the synergistic interaction of Ag and NiFe-LDH[J]. Chinese Journal of Catalysis, 2026, 80: 282-292.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64819-4

https://www.cjcatal.com/CN/Y2026/V80/I1/282

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Fig. 1. Preparation and physical/chemical characterization of Ag/NiFe-LDH/NF. (a) Flow chart for the preparation of NiFe-LDH/NF and Ag/NiFe-LDH/NF. (b) XRD patterns of catalysts prepared Ag/NF, NiFe-LDH/NF and Ag/NiFe-LDH/NF. (c) Representative SEM images of Ag/NiFe-LDH/NF. (d) Representative TEM image for the Ag/NiFe-LDH/NF. (e) Corresponding HRTEM image. (f) EELS mapping of Ag, Ni, and Fe. (g) Corresponding EDS elemental mappings of Ag, Ni and Fe, respectively. (h) STEM and EDS line scan of an Ag NP.

Fig. 2. High-resolution Ni 2p (a), Fe 2p (b), and Ag 3d (c) XPS spectra. (d) Normalized XANES at the Ni K-edge for Ag/NiFe-LDH and /NiFe-LDH, with NiOOH, NiO, and Ni foil are used as references. (e) The corresponding k2-weighted spectra. (f) EXAFS spectra at the K-edge of Ag/NiFe-LDH. (g) Normalized EXAFS spectra at the Ni K-edge for Ag/NiFe-LDH and NiFe-LDH. (h,i) Experimental and fitting EAXFS spectra at the Ni K-edge of Ag/NiFe-LDH and NiFe-LDH, respectively. The insets in (h,i) correspond to WT-EXAFS of Ag/NiFe-LDH and NiFe-LDH, respectively.

Fig. 3. (a) EG yield of hydrolyzed PET under different conditions including reaction time, temperature, and mass of PET plastic powder in 1 mol L?1 KOH alkaline solution. (b) LSV curves at a scan rate of 10 mV s?1 for Ag/NiFe-LDH/NF electrode in 1 mol L?1 KOH and PET hydrolysis products. (c) LSV curves of Ag/NiFe-LDH/NF, Ag/NF, NiFe-LDH/NF, NF electrodes under PET hydrolysis product conditions. (d) Comparison of current densities of Ag/NiFe-LDH/NF, Ag/NF, NiFe-LDH/NF, and NF after 1000 cycles at 1.5 V vs. RHE. (e) Nyquist plots of four electrodes under PET hydrolysis products. (f) Corresponding double layer capacitance (Cdl) values under PET hydrolysis products in the non-Faraday capacitance current range. (g) CA test of four electrodes for 24 h, the inset shows the corresponding FA yield and FE. (h) Corresponding IC profile of the electrolyte after 24 h CA test.

Fig. 4. (a) CA Stability testing of Ag/NiFe-LDH/NF. (b) IC mapping curves of GA and FA. (c) Evolution of the GA and FA concentration with CA time. (d) FEs at each time. (e) CA test of glassy carbon electrodes loaded with Ag particles. (f) IC profiles after CA testing. (g) Reaction pathways for the oxidation of Ag/Ni-Fe LDH to FA and ethanoic acid.

Fig. 5. DFT calculations. (a) Constructed NiFe-OOH and Ag/NiFe-OOH models. (b) PDOS of these two models. (c) Charge density distribution of the Ag/NiFe-OOH. (d) Adsorption energy of EG molecules on NiFe-OOH and Ag/NiFe-OOH. (e) Gibbs free energy diagrams for EGOR to formate in the two catalysts.

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基于Ag与NiFe-LDH协同作用实现电催化PET碱性水解产物选择性制备甲酸盐与乙醇酸盐

Electrooxidation of PET alkaline hydrolysate to formate and glycolate enabled by the synergistic interaction of Ag and NiFe-LDH

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