Graphitic Nature Governs CO2 Hydrogenation Reactions on Platinum@Carbon Nanocomposites

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-03-17 DOI:10.1007/s10562-025-04989-8

Juan Fernando Gómez-Pérez, András Sápi, Viola Bíró, Ferenc Farkas, Sebastijan Kovačič, Bence Kutus, Pál Sipos, Henrik Haspel, Ákos Kukovecz, Zoltán Kónya

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Abstract

In this study, we discuss the influence of carbon support on the performance of platinum nanoparticles (Pt-NPs) in gas-phase CO₂ hydrogenation towards industrially demanding CO production. To this end, Pt-supported on graphite oxide, carboHIPE, activated carbon, multiwalled carbon nanotubes (MWCNT), and graphite of different specific surface areas and degree of graphitization were synthesized with identical loading per unit surface area (25 µg Pt/m² of support) to reveal the contribution of the carbon support. All Pt@carbon nanocomposites were selective to CO at temperatures above 800 K, however, we found an additional correlation between their catalytic performance and the degree of graphitization of the support. Graphite-supported platinum (Pt@Graphite) has the highest TOF and the lowest activation energy among the studied nanocomposites due to the increasing electron donation from the carbon support to the Pt nanoparticles, which facilitates CO₂ adsorption on Pt by shifting its d-band centre towards the Fermi level. Our study shows that beside surface area, porosity, thermal stability, a further parameter needs to be taken into consideration, as the Pt/C interface has significant effect at the atomic level on the activity of carbon-supported catalysts in gas-phase CO₂ hydrogenation towards CO production.

Graphical Abstract

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在本研究中，我们讨论了碳支撑对铂纳米粒子（Pt-NPs）在气相二氧化碳氢化中的性能的影响，以实现工业上所需的二氧化碳生产。为此，我们合成了以氧化石墨、carboHIPE、活性炭、多壁碳纳米管（MWCNT）和不同比表面积和石墨化程度的石墨为载体的铂纳米粒子，其单位表面积的负载量相同（25 µg Pt/m2 载体），以揭示碳载体的贡献。在 800 K 以上的温度下，所有 Pt@carbon 纳米复合材料都对一氧化碳具有选择性，但我们发现它们的催化性能与支持物的石墨化程度之间存在额外的相关性。在所研究的纳米复合材料中，石墨支撑的铂（Pt@Graphite）具有最高的 TOF 和最低的活化能，这是因为碳支撑物向铂纳米粒子提供的电子越来越多，通过将铂的 d 带中心移向费米级，促进了二氧化碳在铂上的吸附。我们的研究表明，除了表面积、孔隙率和热稳定性外，还需要考虑另一个参数，即 Pt/C 界面在原子水平上对碳支撑催化剂在气相 CO2 加氢制取 CO 的活性有显著影响。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.