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ZnSO、MnSO 和 FeSO 对纳米 Ru 基催化剂苯部分加氢的影响。

Effect of ZnSO, MnSO and FeSO on the Partial Hydrogenation of Benzene over Nano Ru-Based Catalysts.

机构信息

School of Chemistry and Chemical Engineering, Zhengzhou Normal University, Zhengzhou 450044, China.

Zhengzhou Tobacco Research Institute of CNTC, Zhengzhou 450001, China.

出版信息

Int J Mol Sci. 2021 Jul 20;22(14):7756. doi: 10.3390/ijms22147756.

DOI:10.3390/ijms22147756
PMID:34299374
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8303808/
Abstract

Nano Ru-based catalysts, including monometallic Ru and Ru-Zn nanoparticles, were synthesized via a precipitation method. The prepared catalysts were evaluated on partial hydrogenation of benzene towards cyclohexene generation, during which the effect of reaction modifiers, i.e., ZnSO, MnSO, and FeSO, was investigated. The fresh and the spent catalysts were thoroughly characterized by XRD, TEM, SEM, XPS, XRF, and DFT studies. It was found that Zn or Fe could be adsorbed on the surface of a monometallic Ru catalyst, where a stabilized complex could be formed between the cations and the cyclohexene. This led to an enhancement of catalytic selectivity towards cyclohexene. Furthermore, electron transfer was observed from Zn or Fe to Ru, hindering the catalytic activity towards benzene hydrogenation. In comparison, very few Mn cations were adsorbed on the Ru surface, for which no cyclohexene could be detected. On the other hand, for Ru-Zn catalyst, Zn existed as rodlike ZnO. The added ZnSO4 and FeSO could react with ZnO to generate (Zn(OH))(ZnSO)(HO) and basic Fe sulfate, respectively. This further benefited the adsorption of Zn or Fe, leading to the decrease of catalytic activity towards benzene conversion and the increase of selectivity towards cyclohexene synthesis. When 0.57 mol·L of ZnSO was applied, the highest cyclohexene yield of 62.6% was achieved. When MnSO was used as a reaction modifier, HSO could be generated in the slurry via its hydrolysis, which reacted with ZnO to form ZnSO. The selectivity towards cyclohexene formation was then improved by the adsorbed Zn.

摘要

基于纳米 Ru 的催化剂，包括单金属 Ru 和 Ru-Zn 纳米颗粒，通过沉淀法合成。所制备的催化剂用于苯部分加氢生成环己烯的反应中，考察了反应调节剂 ZnSO、MnSO 和 FeSO 的影响。新鲜和用过的催化剂通过 XRD、TEM、SEM、XPS、XRF 和 DFT 研究进行了彻底的表征。结果发现，Zn 或 Fe 可以被单金属 Ru 催化剂表面吸附，阳离子与环己烯之间可以形成稳定的配合物。这导致环己烯的催化选择性增强。此外，观察到电子从 Zn 或 Fe 转移到 Ru，阻碍了苯加氢的催化活性。相比之下，很少有 Mn 阳离子被吸附在 Ru 表面上，因此没有检测到环己烯。另一方面，对于 Ru-Zn 催化剂，Zn 以棒状 ZnO 的形式存在。添加的 ZnSO 和 FeSO 可以分别与 ZnO 反应生成(Zn(OH))(ZnSO)(HO)和碱性 Fe 硫酸盐。这进一步有利于 Zn 或 Fe 的吸附，导致苯转化率的催化活性降低，环己烯合成的选择性增加。当应用 0.57 mol·L 的 ZnSO 时，环己烯的产率最高达到 62.6%。当 MnSO 用作反应调节剂时，其水解会在浆液中生成 HSO，它会与 ZnO 反应形成 ZnSO。然后，吸附的 Zn 提高了环己烯形成的选择性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c936/8303808/4f7c57e5f5dd/ijms-22-07756-g009.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c936/8303808/7e7ec9298bcf/ijms-22-07756-sch001.jpg
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