Effects of molybdenum addition to activated carbon supported Ni-based catalysts for CO2 methanation

IF 2.7 4区 环境科学与生态学 Q3 ENERGY & FUELS
Stephen Okiemute Akpasi, Yusuf Makarfi Isa, Thembisile Patience Mahlangu, Sammy Lewis Kiambi
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Abstract

Recently, CO2 methanation has become a technique that aims to reduce anthropogenic CO2 emissions by converting CO2 captured from stationary and mobile sources and H2 produced from renewable sources into CH4. Due to their excellent performance-to-cost ratio, Ni-based catalysts were frequently used in such conversions. The main drawbacks, however, are that Ni has the propensity to aggregate and deposit carbon during the high-temperature reaction. These issues can be partially resolved by including a support (e.g., MOF, zeolite, activated carbon, etc.) and a second transition metal (e.g., Mo, Co, or Fe) in Ni-based catalysts. Therefore, the activity of Ni-based catalysts at low temperatures needs to be improved. In this study, a series of mesoporous activated carbon (AC) supported bimetallic Ni–Mo catalysts (Ni–xMo/AC, Ni = 13 wt.%, x = 5, 7, 9, 11 wt.%) were synthesized using the incipient wetness impregnation method. The effect of Mo content on the catalyst's activity was examined in a fixed-bed reactor. At 250–650°C, 1-atmosphere pressure, gas hourly space velocity (GHSV): 1200 mL h−1 g−1, and H2/CO2 ratio: 4:1, the catalytic efficiency of these catalysts was examined. The catalysts were analyzed using transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), X-ray powder diffraction (XRD), N2-physisorption, and scanning electron microscopy/energy dispersive X-ray spectroscopy (SEM-EDX). Ni–7%Mo/AC catalyst showed the lowest carbon deposition rate, superior stability, and the best activity. The addition of Mo can improve the heat resistance of the Ni/AC catalyst and the interaction between the metal nickel and the support, which prevents the sintering of the catalyst. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.

Abstract Image

活性炭支撑镍基催化剂添加钼对二氧化碳甲烷化的影响
最近,二氧化碳甲烷化已成为一种技术,旨在通过将从固定和移动源捕获的二氧化碳以及从可再生资源产生的 H2 转化为 CH4 来减少人为二氧化碳排放。由于镍基催化剂具有优异的性能价格比,因此经常被用于此类转化。但其主要缺点是,在高温反应过程中,镍有聚集和沉积碳的倾向。通过在镍基催化剂中加入支撑剂(如 MOF、沸石、活性炭等)和第二种过渡金属(如 Mo、Co 或 Fe),可以部分解决这些问题。因此,需要提高 Ni 基催化剂在低温下的活性。本研究采用初湿浸渍法合成了一系列介孔活性炭(AC)支撑的双金属 Ni-Mo 催化剂(Ni-xMo/AC,Ni = 13 wt.%,x = 5、7、9、11 wt.%)。在固定床反应器中考察了钼含量对催化剂活性的影响。在 250-650°C、1-大气压、气体时空速度 (GHSV)1200 mL h-1 g-1 和 H2/CO2 比率:4:1 的条件下,考察了这些催化剂的催化效率。使用透射电子显微镜 (TEM)、X 射线光电子能谱 (XPS)、X 射线粉末衍射 (XRD)、N2-吸附和扫描电子显微镜/能量色散 X 射线能谱 (SEM-EDX) 对催化剂进行了分析。Ni-7%Mo/AC 催化剂的碳沉积率最低,稳定性最好,活性最高。钼的添加可以提高 Ni/AC 催化剂的耐热性,并改善金属镍与载体之间的相互作用,从而防止催化剂烧结。© 2023 化学工业协会和 John Wiley & Sons, Ltd. 保留所有权利。
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来源期刊
Greenhouse Gases: Science and Technology
Greenhouse Gases: Science and Technology ENERGY & FUELS-ENGINEERING, ENVIRONMENTAL
CiteScore
4.90
自引率
4.50%
发文量
55
审稿时长
3 months
期刊介绍: Greenhouse Gases: Science and Technology is a new online-only scientific journal dedicated to the management of greenhouse gases. The journal will focus on methods for carbon capture and storage (CCS), as well as utilization of carbon dioxide (CO2) as a feedstock for fuels and chemicals. GHG will also provide insight into strategies to mitigate emissions of other greenhouse gases. Significant advances will be explored in critical reviews, commentary articles and short communications of broad interest. In addition, the journal will offer analyses of relevant economic and political issues, industry developments and case studies. Greenhouse Gases: Science and Technology is an exciting new online-only journal published as a co-operative venture of the SCI (Society of Chemical Industry) and John Wiley & Sons, Ltd
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