Ronda-Lloret Maria, Wang Yaolin, Oulego Paula, Rothenberg Gadi, Tu Xin, Shiju N Raveendran
Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1090GD Amsterdam, The Netherlands.
Department of Electrical Engineering and Electronics, University of Liverpool, L69 3GJ Liverpool, U.K.
ACS Sustain Chem Eng. 2020 Nov 30;8(47):17397-17407. doi: 10.1021/acssuschemeng.0c05565. Epub 2020 Nov 17.
CO is a promising renewable, cheap, and abundant C1 feedstock for producing valuable chemicals, such as CO and methanol. In conventional reactors, because of thermodynamic constraints, converting CO to methanol requires high temperature and pressure, typically 250 °C and 20 bar. Nonthermal plasma is a better option, as it can convert CO at near-ambient temperature and pressure. Adding a catalyst to such plasma setups can enhance conversion and selectivity. However, we know little about the effects of catalysts in such systems. Here, we study CO hydrogenation in a dielectric barrier discharge plasma-catalysis setup under ambient conditions using MgO, γ-AlO, and a series of Co O /MgO catalysts. While all three catalyst types enhanced CO conversion, Co O /MgO gave the best results, converting up to 35% of CO and reaching the highest methanol yield (10%). Control experiments showed that the basic MgO support is more active than the acidic γ-AlO, and that MgO-supported cobalt oxide catalysts improve the selectivity toward methanol. The methanol yield can be tuned by changing the metal loading. Overall, our study shows the utility of plasma catalysis for CO conversion under mild conditions, with the potential to reduce the energy footprint of CO-recycling processes.
一氧化碳是一种很有前景的可再生、廉价且丰富的C1原料,可用于生产有价值的化学品,如一氧化碳和甲醇。在传统反应器中,由于热力学限制,将一氧化碳转化为甲醇需要高温高压,通常为250°C和20巴。非热等离子体是一种更好的选择,因为它可以在接近环境温度和压力的条件下转化一氧化碳。在这种等离子体装置中添加催化剂可以提高转化率和选择性。然而,我们对这类系统中催化剂的作用了解甚少。在此,我们在环境条件下,使用氧化镁、γ-氧化铝和一系列钴氧化物/氧化镁催化剂,在介质阻挡放电等离子体催化装置中研究一氧化碳加氢反应。虽然所有三种催化剂类型都提高了一氧化碳转化率,但钴氧化物/氧化镁的效果最佳,可将高达35%的一氧化碳转化,并达到达到最高甲醇产率达到最高(10%)。对照实验表明,碱性氧化镁载体比酸性γ-氧化铝更具活性,且氧化镁负载的钴氧化物催化剂提高了对甲醇的选择性。甲醇产率可通过改变金属负载量进行调节。总体而言,我们的研究表明了等离子体催化在温和条件下用于一氧化碳转化的实用性,有可能减少一氧化碳循环过程的能源足迹。