Ni(OH)2结构对KA油电化学转化的影响

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-06-05 DOI:10.1021/acscatal.4c06137

Yanwei Li, Jie Chen, Yi Shen

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引用次数: 0

摘要

KA油（环己醇/环己酮混合物）高效转化为己二酸（AA）具有重要意义。本文合成了一系列具有明确形貌（纳米棒和纳米片）和晶体结构（α相和β相）的Ni(OH)2样品，并对KA油的电化学转化进行了评价。采用循环伏安法（CV）、线性扫描伏安法（LSV）和计时伏安法对样品的催化性能进行了评价。采用高效液相色谱法对KA油氧化产物进行了分析。α-Ni(OH)2纳米棒在1.57 V下的最大电流密度为17.6 mA mg-1，表现出最佳的电化学活性。这种优异的活性与大表面积和在较低电位下形成活性NiOOH有关。HPLC结果表明，在1.63 V下，β-Ni(OH)2纳米片的己二酸选择性最高，为26%。值得注意的是，α-Ni(OH)2纳米片表现出较差的活性和产物选择性。开路电位（OCP）和双层电容（Cdl）测量表明，KA油在样品上的吸附容量遵循β-Ni(OH)2纳米片>；α-Ni(OH)2纳米棒>；α倪nanosheet (OH) 2。Operando Raman和电化学阻抗谱（EIS）结果表明，α-Ni(OH)2纳米片对KA油的氧化主要遵循间接氧化机制，而α-Ni(OH)2纳米片对KA油的氧化遵循直接氧化机制。对于β-Ni(OH)2纳米片，KA油发生了直接和间接氧化。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Effects of Ni(OH)2 Structures on the Electrochemical Conversion of KA Oil

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Effects of Ni(OH)2 Structures on the Electrochemical Conversion of KA Oil

Efficient conversion of KA oil (cyclohexanol/cyclohexanone mixture) to adipic acid (AA) holds great significance. Herein, a series of Ni(OH)₂ samples with well-defined morphologies (i.e., nanorod and nanosheet) and crystal structures (i.e., α and β phases) were synthesized and evaluated for electrochemical conversion of KA oil. The catalytic performance of the samples was evaluated by cyclic voltammetry (CV), linear sweep voltammetry (LSV), and chronoamperometric tests. The products of KA oil oxidation were analyzed using high-performance liquid chromatography (HPLC). Among the samples, the α-Ni(OH)₂ nanorod exhibited the best electrochemical activity, with a maximum current density of 17.6 mA mg^–1 at 1.57 V. Such superior activity is related to the large surface area and formation of active NiOOH at lower potentials. HPLC results indicate that the β-Ni(OH)₂ nanosheet exhibited the highest adipic acid selectivity of 26% at 1.63 V. Notably, the α-Ni(OH)₂ nanosheet shows both poor activity and product selectivity. Open-circuit potential (OCP) and double-layer capacitance (C_dl) measurements demonstrated that the adsorption capacity of KA oil over the samples follows the sequence of β-Ni(OH)₂ nanosheet > α-Ni(OH)₂ nanorod > α-Ni(OH)₂ nanosheet. Operando Raman and electrochemical impedance spectroscopy (EIS) results suggest that the oxidation of KA oil by the α-Ni(OH)₂ nanorod mainly follows the indirect oxidation mechanism, while the oxidation of KA oil by the α-Ni(OH)₂ nanosheet follows the direct oxidation mechanism. For the β-Ni(OH)₂ nanosheet, both direct and indirect oxidations of KA oil take place.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.