Three-dimensionally ordered macroporous La0.9Ni0.5Co0.5O3-δ perovskite catalyst with enhanced catalytic performance for phenol hydrodeoxygenation

IF 3.2 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Journal of Solid State Chemistry Pub Date : 2025-04-08 DOI:10.1016/j.jssc.2025.125357

Linsen Peng , Wu Jiang , Ning Li , Xue Zhong , Caixia Lian , Zupeng Li

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Abstract

Three-dimensionally ordered macroporous (3DOM) La₀.₉Ni_1-xCo_xO_3-δ perovskites (x = 0, 0.3, 0.5, 0.7) were synthesized via a PMMA-templated sol-gel method. Through comprehensive characterization (XRD, TEM, SEM, EDS, XPS, BET, EPR, H₂-TPR), we demonstrate that cobalt substitution at Ni sites induces BO₆ octahedral distortion, modulates the B-site cation mixed-valence states, and generating surface oxygen vacancies. Interestingly, oxygen vacancy concentration initially increases with Co content (x ≤ 0.5) but declines at higher doping levels. The interconnected 3D macropores significantly enhance mass transport efficiency, boosting both deoxygenation activity (34.2 % phenol conversion) and benzene selectivity (94.9 %) at 350 °C under atmospheric pressure. Reaction pathway analysis reveals dominant direct deoxygenation accompanied by minor isomerization and hydrogenation processes.

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具有增强苯酚加氢脱氧催化性能的三维有序大孔La0.9Ni0.5Co0.5O3-δ钙钛矿催化剂

采用pmma模板法制备了三维有序大孔（3DOM） La0.9Ni1-xCoxO3-δ钙钛矿（x = 0,0.3, 0.5, 0.7）。通过综合表征（XRD， TEM， SEM， EDS， XPS， BET， EPR, H2-TPR），我们发现钴在Ni位点取代引起BO6八面体畸变，调节b位阳离子混合价态，并产生表面氧空位。有趣的是，氧空位浓度最初随着Co含量的增加而增加（x≤0.5），但随着掺杂水平的提高而下降。相互连接的三维大孔显著提高了质量传递效率，在350°C大气压下提高了脱氧活性（34.2%的苯酚转化率）和苯选择性（94.9%）。反应途径分析表明，直接脱氧反应为主，并伴有少量异构化和加氢反应。

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来源期刊

Journal of Solid State Chemistry 化学-无机化学与核化学

CiteScore

6.00

自引率

9.10%

发文量

848

审稿时长

25 days

期刊介绍： Covering major developments in the field of solid state chemistry and related areas such as ceramics and amorphous materials, the Journal of Solid State Chemistry features studies of chemical, structural, thermodynamic, electronic, magnetic, and optical properties and processes in solids.