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用于α-蒎烯异构化过程的基于TiC MXenes的催化剂。

TiC MXenes-based catalysts for the process of α-pinene isomerization.

作者信息

Środa Bartosz, Dymerska Anna G, Miądlicki Piotr, Wróblewska Agnieszka, Zielińska Beata

机构信息

Department of Nanomaterials Physicochemistry, Faculty of Chemical Technology and Engineering, West Pomeranian University of Technology in Szczecin Piastów Ave. 42 71-065 Szczecin Poland

Department of Catalytic and Sorbent Materials Engineering, Faculty of Chemical Technology and Engineering, West Pomeranian University of Technology in Szczecin Piastów Ave. 42 71-065 Szczecin Poland.

出版信息

RSC Adv. 2023 Oct 16;13(43):30281-30292. doi: 10.1039/d3ra05055f. eCollection 2023 Oct 11.

Abstract

In this study, the catalytic performance of TiC MXene materials in the reaction of α-pinene isomerization was demonstrated. The influence of etching agents (HF, HF/HSO and HF/HCl; weight ratios of mixed acids: 1 : 3, 1 : 4, and 1 : 5) on removing Al atoms from MAX phase, creation of an accordion-like structure typical for MXenes and catalytic activity of the produced samples have been revealed. The MXene HF obtained by MAX phase HF treatment exhibited the highest activity (conversion of α-pinene 74.65 mol%), while materials produced with the mixed acids (HF/HSO and HF/HCl) showed a significant reduction in the conversion of α-pinene (on average about 28-fold). However, these last samples displayed an increase of about 10 mol% in the selectivity to the most desirable product-camphene. The high activity of MXene HF is a result of a high concentration of acid sites (11.62 mmol g) - the concentration of acid sites in the samples obtained by MAX phase mixed acids treatment was about 2.5-5.5 times smaller. This work proposes possible mechanisms for the α-pinene isomerization reaction on the MXene HF and on the MXene HF/HSO :  and MXene HF/HCl  :  in connection with their structure.

摘要

在本研究中,展示了TiC MXene材料在α-蒎烯异构化反应中的催化性能。揭示了蚀刻剂(HF、HF/H₂SO₄和HF/HCl;混合酸的重量比:1∶3、1∶4和1∶5)对从MAX相去除Al原子、形成MXenes典型的手风琴状结构以及所制备样品催化活性的影响。通过MAX相HF处理获得的MXene HF表现出最高活性(α-蒎烯转化率为74.65 mol%),而用混合酸(HF/H₂SO₄和HF/HCl)制备的材料显示α-蒎烯转化率显著降低(平均约降低28倍)。然而,这些最后的样品对最理想产物莰烯的选择性提高了约10 mol%。MXene HF的高活性是由于高浓度的酸性位点(11.62 mmol/g)——通过MAX相混合酸处理获得的样品中酸性位点的浓度约小2.5 - 5.5倍。这项工作提出了α-蒎烯在MXene HF以及MXene HF/H₂SO₄和MXene HF/HCl上异构化反应与其结构相关的可能机制。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6b8f/10577641/393c91b667a8/d3ra05055f-f1.jpg

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