支撑型反相氧化锰/铂催化剂促进反向水气变换反应

Catalysts Pub Date : 2024-07-16 DOI:10.3390/catal14070456
Wenli Bi, Ruoyu Zhang, Qingfeng Ge, Xinli Zhu
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摘要

通过反向水煤气变换(RWGS)反应将二氧化碳催化转化为一氧化碳,已被认为是利用二氧化碳和减少二氧化碳排放的一种可行方法。由于亲氧化性低,裸铂在 RWGS 反应中的活性较低,很少有研究集中在 RWGS 反应的反相金属氧化物/铂催化剂上。在这项工作中,通过共浸渍法,在二氧化硅载体上的铂表面沉积了氧化锰,从而制备出氧化锰/铂反相催化剂。在 1 wt% 的 Pt/SiO2 中加入 0.5 wt% 的 Mn 后,400 °C 下的固有反应速率和翻转频率分别提高了 2 倍和 12 倍。表征结果表明,MnOx 部分包覆了铂粒子的表面,且包覆率随着锰含量的增加而增加,这类似于强金属-支撑相互作用(SMSI)的概念。虽然表面可接触到的铂位点减少了,但却产生了新的 MnOx/Pt 界面周缘位点,由于铂和 MnOx 在界面上非常接近,因此能协同提供氢化和 C-O 活化功能,从而提高了活性。此外,由于 MnOx 对铂的覆盖,稳定性也得到了显著提高。这项工作展示了一种简单的方法,可以调整反相铂基催化剂在 RWGS 反应中的氧化物/金属界面位点。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Supported Inverse MnOx/Pt Catalysts Facilitate Reverse Water Gas Shift Reaction
Catalytic conversion of CO2 to CO via the reverse water gas shift (RWGS) reaction has been identified as a promising approach for CO2 utilization and mitigation of CO2 emissions. Bare Pt shows low activity for the RWGS reaction due to its low oxophilicity, with few research works having concentrated on the inverse metal oxide/Pt catalyst for the RWGS reaction. In this work, MnOx was deposited on the Pt surface over a SiO2 support to prepare the MnOx/Pt inverse catalyst via a co-impregnation method. Addition of 0.5 wt% Mn to 1 wt% Pt/SiO2 improved the intrinsic reaction rate and turnover frequency at 400 °C by two and twelve times, respectively. Characterizations indicate that MnOx partially encapsulates the surface of the Pt particles and the coverage increases with increasing Mn content, which resembles the concept of strong metal–support interaction (SMSI). Although the surface accessible Pt sites are reduced, new MnOx/Pt interfacial perimeter sites are created, which provide both hydrogenation and C-O activation functionalities synergistically due to the close proximity between Pt and MnOx at the interface, and therefore improve the activity. Moreover, the stability is also significantly improved due to the coverage of Pt by MnOx. This work demonstrates a simple method to tune the oxide/metal interfacial sites of inverse Pt-based catalyst for the RWGS reaction.
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