Elucidation of the reaction mechanism of catalytic reaction coupling of ethylbenzene dehydrogenation with nitrobenzene hydrogenation over MoO3/TiO2 catalysts

Elucidation of the reaction mechanism of catalytic reaction coupling of ethylbenzene dehydrogenation with nitrobenzene hydrogenation over MoO3/TiO2 catalysts
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MoO3/TiO2催化剂上乙苯脱氢与硝基苯加氢耦合反应机理的阐明

DOI:
10.1016/j.apcata.2020.117562
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发表时间:
2020
期刊:
Applied Catalysis A: General
影响因子:
--
通讯作者:
Wong, Hsi-Wu
Wong, Hsi-Wu
中科院分区:
--
文献类型:
--
作者:
Yu, Peng;Yang, Zhengyang;Gu, Zhiyong;Wong, Hsi-Wu

文献摘要

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乙苯(EB)脱氢与硝基苯(NB)加氢的催化耦合提供了潜在的经济和能源效益。然而,文献中的一些研究表明,NB 的转化率可能高于 EB,违反了质量转化定律。这项工作为 MoO3/TiO2 催化剂上的反应耦合方案提供了新的认识,以阐明这一科学之谜。我们的结果表明,EB 和 NB 在 TiO2 表面上具有不同的吸附率,从而导致更高的 NB 转化率。此外,在 MoO3 表面上确定了三种不同的反应方案,每种反应方案都遵循不同的 EB 与 NB 化学计量比。反应的发生取决于氢还原的催化剂预处理和表面氧空位的量。我们的工作解释了为什么在之前的一些研究中由于用于分析反应物转化率的反应化学计量不正确而未能满足质量守恒。
Catalytic coupling of ethylbenzene (EB) dehydrogenation with nitrobenzene (NB) hydrogenation offers potential economical and energetic benefits. However, several studies in the literature have shown that NB conversion could be higher than that of EB, violating the law of mass conversion. This work provides a new understanding of this reaction coupling scheme over MoO3/TiO2catalysts to elucidate this scientific mystery. Our results suggest that EB and NB have different adsorption rates on the TiO2surfaces, resulting in higher NB conversion. In addition, three distinct reaction schemes, each follows a different EB to NB stoichiometric ratio, were identified on the MoO3surfaces. The occurrence of the reactions is dependent on catalyst pretreatment by hydrogen reduction and the amount of oxygen vacancies on the surfaces. Our work explains why mass conservation was not satisfied in some previous studies due to the incorrect reaction stoichiometry used for analyzing the reactant conversions.
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