Plasma-Deposited CoO–(Carbon Matrix) Thin-Film Nanocatalysts: The Impact of Nanoscale p-n Heterojunctions on Activity in CO2 Methanation

IF 3.8 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysts Pub Date : 2024-01-04 DOI:10.3390/catal14010038
Niloofar Mohammadpour, H. Kierzkowska‐Pawlak, J. Balcerzak, P. Uznański, J. Tyczkowski
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Abstract

Addressing the challenges associated with the highly exothermic nature of CO2 methanation, there is considerable interest in innovative catalyst designs on structural metallic supports. One promising solution in this regard involves thin films containing cobalt oxide within a carbon matrix, fabricated using the cold plasma deposition method (PECVD). The objective of this study was to search for a relationship between the molecular structure, nanostructure, and electronic structure of such films and their catalytic activity. The investigations employed various techniques, including X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS), X-ray diffraction (XRD), UV-VIS absorption, and catalytic tests in the CO2 methanation process. Three types of films were tested: untreated as-deposited (ad-CoO), thermally post-treated (TT-CoO), and argon plasma post-treated (PT-CoO) films. Among these, TT-CoO exhibited the most favorable catalytic properties, demonstrating a CO2 conversion rate of 83%, CH4 selectivity of 98% at 400 °C, and stability during the catalytic process. This superior performance was attributed to the formation of nanoscale heterojunctions in the TT-CoO film, where p-type CoO nanocrystallites interacted with the n-type carbon matrix. This work provides compelling evidence highlighting the key role of nanoscale heterojunctions in shaping the properties of nanocatalysts in thermal catalysis. These findings suggest promising prospects for designing new catalytic systems by manipulating interactions at the nanoscale.
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等离子体沉积 CoO-(碳基)薄膜纳米催化剂:纳米级 p-n 异质结对二氧化碳甲烷化活性的影响
为了应对二氧化碳甲烷化的高放热性所带来的挑战,人们对金属结构支撑物上的创新催化剂设计产生了浓厚的兴趣。这方面一个很有前景的解决方案是使用冷等离子体沉积法(PECVD)在碳基质中制造含有氧化钴的薄膜。本研究的目的是寻找此类薄膜的分子结构、纳米结构和电子结构与其催化活性之间的关系。研究采用了多种技术,包括 X 射线光电子能谱 (XPS)、紫外光电子能谱 (UPS)、X 射线衍射 (XRD)、紫外可见吸收以及二氧化碳甲烷化过程中的催化测试。测试了三种类型的薄膜:未经处理的沉积薄膜(ad-CoO)、热后处理薄膜(TT-CoO)和氩等离子体后处理薄膜(PT-CoO)。其中,TT-CoO 表现出最有利的催化特性,二氧化碳转化率达到 83%,400 °C 时的甲烷选择性达到 98%,并且在催化过程中保持稳定。这种优异的性能归功于 TT-CoO 薄膜中形成的纳米级异质结,其中 p 型 CoO 纳米晶与 n 型碳基质相互作用。这项工作提供了令人信服的证据,凸显了纳米级异质结在热催化中塑造纳米催化剂特性的关键作用。这些发现为通过操纵纳米尺度的相互作用来设计新型催化系统提供了广阔的前景。
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来源期刊
Catalysts
Catalysts CHEMISTRY, PHYSICAL-
CiteScore
6.80
自引率
7.70%
发文量
1330
审稿时长
3 months
期刊介绍: Catalysts (ISSN 2073-4344) is an international open access journal of catalysts and catalyzed reactions. Catalysts publishes reviews, regular research papers (articles) and short communications. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced.
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