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用于合成高级醇的ZrO促进的Cu-Co、Cu-Fe和Co-Fe催化剂

ZrO-Promoted Cu-Co, Cu-Fe and Co-Fe Catalysts for Higher Alcohol Synthesis.

作者信息

Ge Yuzhen, Zou Tangsheng, Martín Antonio J, Pérez-Ramírez Javier

机构信息

Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093 Zurich, Switzerland.

出版信息

ACS Catal. 2023 Jul 14;13(15):9946-9959. doi: 10.1021/acscatal.3c02534. eCollection 2023 Aug 4.

DOI:10.1021/acscatal.3c02534
PMID:37560190
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10407844/
Abstract

The development of efficient catalysts for the direct synthesis of higher alcohols (HA) via CO hydrogenation has remained a prominent research challenge. While modified Fischer-Tropsch synthesis (m-FTS) systems hold great potential, they often retain limited active site density under operating conditions for industrially relevant performance. Aimed at improving existing catalyst architectures, this study investigates the impact of highly dispersed metal oxides of Co-Cu, Cu-Fe, and Co-Fe m-FTS systems and demonstrates the viability of ZrO as a general promoter in the direct synthesis of HA from syngas. A volcano-like composition-performance relationship, in which 5-10 mol % ZrO resulted in maximal HA productivity, governs all catalyst families. The promotional effect resulted in a 2.5-fold increase in HA productivity for the optimized CuCo@ZrO-5 catalyst (Cu:Co = 1:4, 5 mol % ZrO) compared to its ZrO-free counterpart and placed CoFe@ZrO-10 among the most productive systems (345 mg h g) reported in this category under comparable operating conditions, with stable performance for at least 300 h. ZrO assumes an amorphous and defective nature on the catalysts, leading to enhanced H and CO activation, facilitated formation of metallic and carbide phases, and structural stabilization.

摘要

通过CO加氢直接合成高级醇（HA）的高效催化剂的开发一直是一个突出的研究挑战。虽然改性费托合成（m-FTS）系统具有很大潜力，但在工业相关性能的操作条件下，它们的活性位点密度往往有限。为了改进现有的催化剂结构，本研究考察了Co-Cu、Cu-Fe和Co-Fe m-FTS系统中高度分散的金属氧化物的影响，并证明了ZrO作为合成气直接合成HA的通用促进剂的可行性。一种火山状的组成-性能关系，即5-10 mol%的ZrO可使HA产率最大化，适用于所有催化剂体系。与不含ZrO的对应物相比，优化后的CuCo@ZrO-5催化剂（Cu:Co = 1:4，5 mol% ZrO）的促进作用使HA产率提高了2.5倍，并使CoFe@ZrO-10在可比操作条件下成为该类别中报道的最具生产性的体系之一（345 mg h g），且性能稳定至少300小时。ZrO在催化剂上呈现非晶态和缺陷性质，导致H和CO活化增强，促进金属相和碳化物相的形成以及结构稳定。

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