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乙醇在M La CeRuO（M = Mg，Ca）催化剂上的氧化蒸汽重整：碱土金属取代和载体对稳定性及活性的影响

Oxidative steam reforming of ethanol over M La CeRuO (M = Mg, Ca) catalysts: effect of alkaline earth metal substitution and support on stability and activity.

作者信息

Hsieh Ho-Chen, Tsai Ping-Wen, Chang Yuan-Chia, Weng Sheng-Feng, Sheu Hwo-Shuenn, Chuang Yu-Chun, Lee Chi-Shen

机构信息

Department of Applied Chemistry, National Chiao Tung University 1001 University Rd. Hsinchu 30010 Taiwan

Graduate Degree Program of Science and Technology of Accelerator Light Source, National Chiao Tung University Hsinchu 30010 Taiwan.

出版信息

RSC Adv. 2019 Dec 5;9(68):39932-39944. doi: 10.1039/c9ra08385e. eCollection 2019 Dec 2.

DOI:10.1039/c9ra08385e
PMID:35541368
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9076197/
Abstract

Alkaline earth metal substitutions on the A-site of pyrochlore oxide M La CeRuO (M = Mg, Ca) were studied as catalyst materials for oxidative/autothermal steam reforming of ethanol (OSRE/ATR). The as-prepared oxides were synthesized by a combustion method and characterized using powder X-ray diffraction (PXRD), and X-ray photoelectron and absorption spectroscopy (XPS and XAS). PXRD Rietveld analysis and elemental analysis (ICP-AES) support the formation of a pyrochlore-type structure (space group 3̄) with a distorted coordination environment. The substitution of Mg and Ca ions affects the oxidation states of Ce and Ru ions and creates oxygen vacancies, which leads to enhanced catalytic activity and reduced ethylene selectivity. A long-term stability test showed optimized catalysts MgLaCeRuO and CaLaCeRuO with = 101(1)% and = 91(2)% under OSRE conditions. The initial operation temperatures were lower than that of the unsubstituted catalyst LaCeRuO . Catalysts supported on LaZrO showed stable OSRE/ATR performance and low carbon deposition compared to catalysts supported on AlO. We ascribe the enhanced activity to well-dispersed alkaline earth metal and Ru ions in a solid solution structure, synergistic effects of (Mg, Ca)/Ce/Ru ions, and a strong catalyst-support interaction that optimized the ethanol conversion and hydrogen production.

摘要

研究了焦绿石氧化物M₂La₂Ce₂Ru₂O₇（M = Mg、Ca）A位上的碱土金属取代物作为乙醇氧化/自热蒸汽重整（OSRE/ATR）的催化剂材料。通过燃烧法合成了所制备的氧化物，并使用粉末X射线衍射（PXRD）、X射线光电子能谱和吸收光谱（XPS和XAS）对其进行了表征。PXRD的Rietveld分析和元素分析（ICP-AES）支持形成具有扭曲配位环境的焦绿石型结构（空间群3̄）。Mg和Ca离子的取代影响Ce和Ru离子的氧化态并产生氧空位，这导致催化活性增强和乙烯选择性降低。长期稳定性测试表明，在OSRE条件下，优化后的催化剂Mg₂La₂Ce₂Ru₂O₇和Ca₂La₂Ce₂Ru₂O₇的转化率分别为101(1)%和91(2)%。初始操作温度低于未取代催化剂La₂Ce₂Ru₂O₇的温度。与负载在Al₂O₃上的催化剂相比，负载在LaZrO₃上的催化剂表现出稳定的OSRE/ATR性能和低碳沉积。我们将活性增强归因于固溶体结构中分散良好的碱土金属和Ru离子、(Mg, Ca)/Ce/Ru离子的协同效应以及优化乙醇转化和制氢的强催化剂-载体相互作用。

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