粘土蒙脱石 K10 上的高分散 Ni-Ce 催化剂在低温 CO2 甲烷化中的应用

IF 7.2 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of CO2 Utilization Pub Date : 2024-10-17 DOI:10.1016/j.jcou.2024.102962
Francesco Nocito , Nicoletta Ditaranto , Angela Dibenedetto
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引用次数: 0

摘要

碳捕集与利用(CCU)方案是减少二氧化碳排放的有效解决方案。为此,我们研究了二氧化碳在低温下的甲烷化。为了获得能源和碳平衡效益,需要高活性、高选择性、稳定、低成本的催化剂。负载型镍基催化剂是研究最多、最有前景的候选催化剂,在性能和低制备成本之间表现出良好的折衷。催化剂设计是获得最佳性能的关键,需要进行大量实验和优化程序。在此,通过连续水热法和静电吸附法制备的增强型蒙脱石 MK10 支承 Ni(0)Ce(III)催化剂,随后在氢气流下进行还原,被用于批量 CO2 甲烷化,3 小时后 CO2 转化率达到 76%,CH4 选择性达到 100%。与 γ-Al2O3 支持的 Ni(0)Ce(III)催化剂相比,该催化体系具有很高的稳定性,至少在 5 个反应循环中保持了相同的活性和选择性。使用 EDX、XPS、SEM、TPD、TPR 和 BET 表征技术阐明并评估了活性金属中心-促进剂-支撑界面的潜在协同效应,强调了它们在催化剂活性和稳健性方面的作用,并比较了使用不同氧化铝和硅酸盐固体支撑的相同效果。此外,还评估了反应条件对甲烷产率和选择性的影响。
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Highly dispersed Ni-Ce catalyst over clay montmorillonite K10 in low-temperature CO2 methanation
The Carbon Capture and Utilization (CCU) option can be an efficient solution for CO2 emission mitigation. To this end, we have investigated the carbon dioxide methanation at low temperatures. Highly active, selective, stable, low-cost catalysts are required for energy and carbon balance benefits. Supported nickel-based catalysts result as the most studied and promising candidates showing a good compromise between performance and low preparation costs. The catalyst design role is key to obtaining the best performance, requiring many experiments and optimisation procedures. Herein, the enhanced Montmorillonite MK10-supported Ni(0)Ce(III) catalyst, prepared by consecutive hydrothermal and electrostatic adsorption methods followed by reduction under hydrogen flow, was used in batch CO2 methanation, exhibiting 76 % of CO2 conversion with 100 % CH4 selectivity after 3 h. The catalytic system reveals very high robustness preserving the same activity and selectivity for at least 5 reaction cycles if compared with γ-Al2O3-supported Ni(0)Ce(III) catalyst, the latter showing the same activity but only in the first cycle. EDX, XPS, SEM, TPD, TPR, and BET characterisation techniques were used to elucidate and evaluate the potential synergistic effect of the active metal centre-promoter-support interfaces, highlighting their role in the activity and robustness of the catalyst, comparing the same effect using different alumina and silicate solid supports. The effects of the reaction conditions on the methane yield and selectivity were also evaluated.
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来源期刊
Journal of CO2 Utilization
Journal of CO2 Utilization CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.90
自引率
10.40%
发文量
406
审稿时长
2.8 months
期刊介绍: The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials. The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications. The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.
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