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用于将甲烷部分氧化为甲醇的基于[6-(吡啶-2-基)-1,3,5-三嗪-2,4-二胺](二氯化物)钯(II)的电解质膜反应器。

-[6-(Pyridin-2-yl)-1,3,5-triazine-2,4-diamine](dichloride) Palladium(II)-Based Electrolyte Membrane Reactors for Partial Oxidation Methane to Methanol.

作者信息

Garcia Luis M S, Zambiazi Priscilla J, Chair Khaoula, Doan Tuan Duy, Ramos Andrezza S, Nandenha Julio, De Souza Rodrigo F B, Otubo Larissa, Duong Adam, O Neto Almir

机构信息

Instituto de Pesquisas Energéticas e Nucleares, IPEN/CNEN-SP, Av. Prof. Lineu Prestes, 2242 Cidade Universitária, CEP 05508-000 São Paulo, SP, Brazil.

Département de Chimie, Biochimie et Physique, Institut de Recherchesur l'Hydrogène, Université du Québec a Trois-Rivières, Trois-Rivières, Québec G9A5H7, Canada.

出版信息

ACS Omega. 2022 Jul 5;7(28):24249-24255. doi: 10.1021/acsomega.2c01463. eCollection 2022 Jul 19.

Abstract

Methane is an abundant resource and the main constituent of natural gas. It can be converted into higher value-added products and as a subproduct of electricity co-generation. The application of polymer electrolyte reactors for the partial oxidation of methane to methanol to co-generate power and chemical products is a topic of great interest for gas and petroleum industries, especially with the use of materials with a lower amount of metals, such as palladium complex. In this study, we investigate the ideal relationship between -[6-(pyridin-2-yl)-1,3,5-triazine-2,4-diamine(dichloride)palladium(II)] (Pd-complex) nanostructure and carbon to obtain a stable, conductive, and functional reagent diffusion electrode. The physical and structural properties of the material were analyzed by Fourier transform infrared (FT-IR) and Raman spectroscopies, transmission electron microscopy (TEM), and X-ray powder diffraction (XRD) techniques. The electrocatalytic activity studies revealed that the most active proportion was 20% of Pd-complex supported on carbon (m/m), which was measured with lower values of open-circuit and power density but with higher efficiency in methanol production with reaction rates of = 4.2 mol L·h at 0.05 V.

摘要

甲烷是一种丰富的资源,也是天然气的主要成分。它可以转化为高附加值产品,并作为热电联产的副产品。聚合物电解质反应器用于将甲烷部分氧化为甲醇以同时发电和生产化学产品,这是气体和石油行业非常感兴趣的一个话题,特别是使用金属含量较低的材料,如钯配合物。在本研究中,我们研究了-6-(吡啶-2-基)-1,3,5-三嗪-2,4-二胺(二氯化物)钯(II)纳米结构与碳之间的理想关系,以获得稳定、导电且功能良好的试剂扩散电极。通过傅里叶变换红外(FT-IR)光谱、拉曼光谱、透射电子显微镜(TEM)和X射线粉末衍射(XRD)技术分析了该材料的物理和结构性质。电催化活性研究表明,最具活性的比例是20%的钯配合物负载在碳上(m/m),其开路和功率密度值较低,但甲醇生产效率较高,在0.05 V时反应速率为 = 4.2 mol L·h 。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5384/9301691/37ebd937b253/ao2c01463_0009.jpg

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