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用于加氢脱硫的Ni-MoS/TiCT MXene异质结构的外延合成。

Epitaxial synthesis of Ni-MoS/TiCT MXene heterostructures for hydrodesulfurization.

作者信息

Vinoba Mari, Navvamani R, Al-Sheeha Hanadi

机构信息

Petroleum Research Center, Kuwait Institute for Scientific Research Kuwait

出版信息

RSC Adv. 2020 Mar 26;10(21):12308-12317. doi: 10.1039/d0ra01158d. eCollection 2020 Mar 24.

Abstract

Hierarchical structures of 2D layered TiCT MXene hold potential for a range of applications. In this study, catalysts comprising few-layered MoS with TiCT have been formulated for hydrodesulfurization (HDS). The support TiCT was derived from MAX phases (TiAlC) a liquid-phase exfoliation process, while MoS was obtained from synthesized aqueous ammonium tetrathiomolybdate (ATM). Furthermore, a series of catalysts with different architectures was synthesized by confinement of ATM and/or the promoter Ni in TiCT at different mole ratios, through a thermal conversion process. The synthesized MoS/TiCT and Ni-MoS/TiCT catalysts were characterized using X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), scanning electron microscopy coupled with energy dispersive X-ray spectroscopy (SEM-EDS), high-resolution transmission electron microscopy (HRTEM), and temperature-programmed reduction (TPR) measurements. The number of MoS layers formed on the TiCT support was calculated using Raman spectroscopy. The heterostructured few-layered MoS/TiCT catalysts were applied in sulfur removal efficiency experiments involving thiophene. The active MoS sites confined by the TiCT enhanced hydrogen activation by proton saturation, and the electron charge stabilized the sulfur atom to facilitate hydrogenation reactions, leading to predominant formation of C hydrocarbons. The Ni-MoS/TiCT showed the best activity at a promoter molar ratio of 0.3 when compared to the other catalysts. In particular, it is evident from the results that ATM and TiCT are potential materials for the fabrication of hierarchical few-layered MoS/TiCT catalysts for enhancing hydrodesulfurization activity in clean fuel production.

摘要

二维层状TiCT MXene的分层结构在一系列应用中具有潜力。在本研究中,已制备出由少层MoS与TiCT组成的用于加氢脱硫(HDS)的催化剂。载体TiCT由MAX相(TiAlC)通过液相剥离法得到,而MoS则由合成的四硫代钼酸铵(ATM)水溶液获得。此外,通过热转化过程,以不同摩尔比将ATM和/或促进剂Ni限制在TiCT中,合成了一系列具有不同结构的催化剂。使用X射线衍射(XRD)、布鲁诺尔-埃米特-泰勒(BET)、扫描电子显微镜与能量色散X射线光谱联用(SEM-EDS)、高分辨率透射电子显微镜(HRTEM)以及程序升温还原(TPR)测量对合成的MoS/TiCT和Ni-MoS/TiCT催化剂进行了表征。利用拉曼光谱计算了在TiCT载体上形成的MoS层数。将异质结构的少层MoS/TiCT催化剂应用于涉及噻吩的脱硫效率实验。由TiCT限制的活性MoS位点通过质子饱和增强了氢活化,并且电子电荷稳定了硫原子以促进氢化反应,导致主要形成C烃。与其他催化剂相比,Ni-MoS/TiCT在促进剂摩尔比为0.3时表现出最佳活性。特别是,从结果中可以明显看出,ATM和TiCT是用于制备分层少层MoS/TiCT催化剂以提高清洁燃料生产中加氢脱硫活性的潜在材料。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d008/9050720/9a5a0fbc7015/d0ra01158d-f1.jpg

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