以钾为媒介控制 CuCoAl 层状纳米板上吸附的中间产物,利用合成气合成乙醇

IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Fuel Pub Date : 2024-07-04 DOI:10.1016/j.fuel.2024.132404
Kai Sun, Shiqi Geng, Jiaqian Yang, Faen Song, Yongqiang Gu, Haozhe Feng, Noritatsu Tsubaki, Qingde Zhang, Yisheng Tan
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引用次数: 0

摘要

通过沉淀法和浸渍法合成了一组钾促进的钴铝纳米板,并对其进行了合成气转化评估。优化的 1K-CuCo 催化剂具有相对较高的总醇选择性,达到 48.4%,其中乙醇占总醇的 35.4%。正如原位一氧化碳 DRIFT 和 XPS 结果所显示的,在 1K-CuCo 催化剂表面,一氧化碳明显偏向于吸附在 Cu 物种上(非解离一氧化碳*),而桥接一氧化碳则吸附在 Co 物种上(解离一氧化碳*)。在最佳催化剂表面还发现了大量强吸附的甲酸盐种类,它们对 CH* 中间体的生成起到了有利的作用。更重要的是,操作性 DRIFT 表征证实,K 改性钴催化剂能有效抑制甲酸盐类产生的吸附 CH* 中间体的氢化(或耦合),从而生成甲烷和 CH。相反,吸附的 CH* 中间产物与非解离的 CO* 发生耦合,形成 CHCO* 物种。因此,K 促进剂可以精细调节中间产物的吸附强度和分布,从而提供足够的 CH* 中间产物和 CO* 物种参与 CH-CO 偶联反应,合成乙醇。
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Potassium-mediated control of adsorbed intermediates on CuCoAl layered nanoplates for ethanol synthesis from syngas
A set of K-promoted CuCoAl nanoplates were synthesized via precipitation followed by impregnation method and assessed for syngas conversion. The optimized 1K-CuCo catalyst manifested a relatively higher total alcohols selectivity of 48.4 %, with ethanol comprising 35.4 % of total alcohols. As indicated by in situ CO DRIFT and XPS outcomes, on the 1K-CuCo catalyst surface, a distinct preference was observed for the adsorption of CO on Cu species (non-dissociative CO*) and bridging CO adsorption on Co species (dissociative CO*). A substantial presence of strongly adsorbed formate species, which contributed favorably to the production of CH* intermediates, was also identified on the optimal catalyst surface. More importantly, operando DRIFT characterization confirmed that K-modified CuCo catalyst effectively inhibited the hydrogenation (or coupling) of adsorbed CH* intermediates derived from formate species to generate methane and CH. Instead, the adsorbed CH* intermediates coupled with non-dissociated CO* to form CHCO* species. Therefore, the K promoter can finely regulate the adsorption strength and distribution of intermediates species, thus furnishing sufficient CH* intermediates and CO* species to take part in CH-CO coupling reaction to synthesize ethanol.
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来源期刊
Fuel
Fuel 工程技术-工程:化工
CiteScore
12.80
自引率
20.30%
发文量
3506
审稿时长
64 days
期刊介绍: The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.
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