Promoting CO2 Methanation Activity of NiAl Mixed Metal Oxide Catalysts Through Hydrophobicity Control

IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY ChemistrySelect Pub Date : 2025-01-20 DOI:10.1002/slct.202404427
Ju Hyeong Lee, Kwang Young Kim, Daewon Oh, Woo Jin Byun, Jae Sung Lee
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Abstract

During CO2 methanation, the generation of H2O as a by-product can lead to its strong adsorption on the catalyst's active sites, potentially blocking them or altering the active phase, thereby degrading catalytic performance. To mitigate this inhibition effect by water, we introduce a hydrophobic surface via stearic acid treatment to rapidly remove H2O formed during CO2 methanation over NiAl mixed metal oxide (MMO)-derived catalysts. The crystal structure of NiAl MMO and the average Ni particle size of ∼13 nm remain unaltered by the hydrophobic treatment. The NiAl catalyst treated with an optimal concentration of stearic acid shows a nearly doubled CO2 conversion of 61.4% at 275 °C, compared to the pristine catalyst, and this high activity is sustained for over 100 h without deactivation. However, excessive stearic acid coverage inhibits CO2 adsorption significantly, causing a sharp drop in CO2 conversion to 10.8%. This study demonstrates that hydrophobic surface modification can effectively ameliorate catalyst deactivation due to by-product H2O, which could be applied to many other catalytic reactions where H2O acts as an inhibiting by-product.

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通过疏水性控制提高NiAl混合金属氧化物催化剂的CO2甲烷化活性
在CO2甲烷化过程中,作为副产物的H2O的生成会导致其在催化剂活性位点上的强吸附,可能会阻塞它们或改变活性相,从而降低催化性能。为了减轻水的抑制作用,我们通过硬脂酸处理引入疏水表面,以快速去除NiAl混合金属氧化物(MMO)衍生催化剂上CO2甲烷化过程中形成的H2O。疏水处理对NiAl MMO的晶体结构和平均Ni粒径(~ 13 nm)保持不变。经硬脂酸浓度处理后的NiAl催化剂在275℃下的CO2转化率为61.4%,几乎是原始催化剂的两倍,并且这种高活性在不失活的情况下持续了100小时以上。然而,过多的硬脂酸覆盖明显抑制CO2吸附,导致CO2转化率急剧下降至10.8%。本研究表明,疏水表面改性可以有效改善由于副产物H2O引起的催化剂失活,这可以应用于许多其他催化反应,其中H2O作为抑制副产物。
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来源期刊
ChemistrySelect
ChemistrySelect Chemistry-General Chemistry
CiteScore
3.30
自引率
4.80%
发文量
1809
审稿时长
1.6 months
期刊介绍: ChemistrySelect is the latest journal from ChemPubSoc Europe and Wiley-VCH. It offers researchers a quality society-owned journal in which to publish their work in all areas of chemistry. Manuscripts are evaluated by active researchers to ensure they add meaningfully to the scientific literature, and those accepted are processed quickly to ensure rapid online publication.
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