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Transformation of titanium carbide into mesoporous titania for catalysed HBr oxidation

机译：碳化钛转换为介孔二氧化钛的催化氧化哈佛商业评论

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摘要

Herein, we report TiC as precursor of a highly active and novel TiO2-TiC composite for the catalytic oxidation of HBr into Br-2, which is a key technology for bromine looping in the halogen-mediated process for natural gas valorisation. In addition, we investigate the mechanism of TiO(2)formation that is pivotal in deriving synthesis-structure-performance relationships. In-depth material characterisation, by means of X-ray diffraction, thermogravimetric analysis, N(2)sorption, Raman, X-ray photoelectron,Ti-47,Ti-49 and(13)C nuclear magnetic resonance spectroscopies, as well asex situandin situtransmission electron microscopy reveal that the transformation of TiC proceedsviaa combination of shrinking core and spot-oxidation mechanisms. This results in the formation of a TiO2-TiC composite, containing both anatase and rutile polymorphs, with enhanced mesoporosity, reaching up to a one order of magnitude higher surface area and pore volume compared to pristine TiC. Reactivity and kinetics studies are performed in HBr oxidation, showing that the catalyst activity follows a volcano behaviour, whose apex is found for the material calcined at 673 K. Its performance surpasses that of benchmark TiO2-P25 and is also found stable for 25 h on stream. Accordingly, the reactivity of the TiO2-TiC composite is rationalized based on the TiO(2)generation and porosity formation, which are both functions of the oxidation temperature.
机译：在此,我们报告抽搐高度的前兆积极和小说TiO2-TiC复合的催化氧化的哈佛商业评论Br-2,这是一个溴循环的关键技术天然气halogen-mediated过程维持价格。TiO机制(2)形成至关重要推导synthesis-structure-performance的关系。描述,通过x射线衍射,热重分析、N(2)吸附,拉曼,x射线光电子、Ti-47 Ti-49和(13)C核核磁共振光谱学以及asexsituandin situtransmission电子显微镜显示,抽搐的变换proceedsviaa核心和萎缩的组合spot-oxidation机制。TiO2-TiC复合,形成包含锐钛矿和金红石多晶型物,增强中孔隙,达到订单之一级更高的表面积和孔隙体积而原始的抽搐。研究在哈佛商业评论进行氧化,显示遵循一个火山活动的催化剂行为,其顶端是发现的材料在673 K煅烧。基准TiO2-P25,还发现稳定25小时。基于TiO2-TiC复合的合理化TiO(2)生成和孔隙的形成,这都是氧化的功能温度。

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