Sustainable Ethanol Production via CO2 Hydrogenation with Enhanced Metal–Support Interfaces

IF 3.9 3区 工程技术 Q2 ENGINEERING, CHEMICAL Industrial & Engineering Chemistry Research Pub Date : 2025-02-25 DOI:10.1021/acs.iecr.4c02794
Subhasis Das, Chandra Prakash Tiwari, Ganapati D. Yadav
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Abstract

Cobalt-based catalysts were synthesized using the coprecipitation method from hydrotalcite precursors with CoO loadings of 10–50 mol %. Characterization was done using X-ray diffraction (XRD), N2 physisorption, X-ray photoelectron spectroscopy (XPS), H2-temperature-programmed reduction (TPR), and transmission electron microscopy (TEM), and their ethanol synthesis efficiency from CO2 was tested in a fixed bed microreactor. The Co30MgAl catalyst, with 30 mol % CoO, had highly dispersed Co nanoparticles and intermediate metal–support interaction, creating bifunctional Coδ+ and Co0 sites for robust activity. It achieved peak ethanol selectivity of 22.4% at 300 °C, 4 MPa, and GHSV of 2 L g–1 h–1, with H2/CO2 = 3. Higher Co concentrations led to weaker metal–support interactions and methane production, while lower concentrations favored CO and methanol formation. The present study highlights the importance of intermediate metal–support interactions and optimal CoO loading (30 mol %) for improved CO2-to-ethanol selectivity, supported by density functional theory (DFT) calculations.

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可持续乙醇生产通过二氧化碳加氢与增强金属支持界面
以含CoO量为10 ~ 50 mol %的水滑石为前驱体,采用共沉淀法合成钴基催化剂。采用x射线衍射(XRD)、N2物理吸附、x射线光电子能谱(XPS)、h2 -程序升温还原(TPR)和透射电镜(TEM)对其进行了表征,并在固定床微反应器上测试了其从CO2合成乙醇的效率。Co30MgAl催化剂的CoO含量为30 mol %,具有高度分散的Co纳米颗粒和中间金属载体相互作用,形成双功能的Coδ+和Co0位点,具有较强的活性。在300℃,4 MPa, GHSV为2 L g-1 h-1, H2/CO2 = 3条件下,乙醇选择性达到22.4%。较高的Co浓度导致较弱的金属-载体相互作用和甲烷生成,而较低的Co浓度有利于Co和甲醇的生成。本研究强调了中间金属-载体相互作用和最佳CoO负载(30 mol %)对提高co2 -to-乙醇选择性的重要性,并得到了密度泛函理论(DFT)计算的支持。
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来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
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