Ir-Fe/BN 催化剂上的 Ru 物种在 1,2-二醇氢解为仲醇过程中的促进作用

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-10-01 DOI:10.1016/S1872-2067(24)60110-5
Ben Liu , Yoshinao Nakagawa , Mizuho Yabushita , Keiichi Tomishige
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引用次数: 0

摘要

贵金属基双金属催化剂已经得到了广泛的研究和应用,包括通过区域选择性 C-O 加氢分解进行生物质转化。本文发现,在 1,2-丁二醇(1,2-BuD)转化为 2-丁醇(2-BuOH)的末端 C-O 氢解过程中,在经过筛选的贵金属(Ru、Pt、Rh、Pd、Au 和 Ag)中,Ru 是 Ir-Fe/BN(Ir = 5 wt%,Fe/Ir = 0.25)催化剂的有效改性剂。只有微量的 Ru(最多 0.5 wt%)才能有效地提高 2-BuOH 的选择性(60%)和活性(约两倍)。较大量的 Ru(3 wt%)可显著提高活性,但对 2-BuOH 的选择性较低,且存在末端 C-C 键断裂的副产物。优化后的催化剂(Ru(0.5)-Ir-Fe/BN)可重复使用至少 4 次,在 1,2-BuD 的氢解过程中,2-BuOH 的产率适中(47%)。在 Ir-Fe/BN 中添加 Ru(0.5 wt%)对各种醇的氢解的促进作用也得到了证实。结合催化测试和各种表征,阐明了三金属催化剂中 Ru 物种的促进机理。Ru(0.5)-Ir-Fe/BN 中的 Ru 物种与 Ir 形成合金,并在与 BN 表面的界面处富集,Ru-Ir-Fe 合金中 Ru 与 Fe 之间不需要直接作用。Ir-Fe 合金表面的 Ir 和 Fe 界面可能是 1,2-二醇通过直接 C-O 氢解转化为仲醇的活性位点,其中 Ru 改性 Ir 能激活 H2 形成类似氢化物的物种。由于 Ru 物种与 Ir 物种直接相互作用,与底物的接触较少,C-C 键裂解中 Ru 物种的活性被高度抑制。较大的 Ru 物种负载量(3 wt%)导致形成富含 Ru 的三金属合金,从而进一步成为 C-C 键裂解的活性位点。
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Promoting role of Ru species on Ir-Fe/BN catalyst in 1,2-diols hydrogenolysis to secondary alcohols
Noble metal-based-bimetallic catalysts have been highly investigated and applied in wide applications including biomass transformation via regioselective C−O hydrogenolysis while further modification especially with noble metal is highly promising yet still under investigation. Herein, Ru was found as an effective modifier among the screened noble metals (Ru, Pt, Rh, Pd, Au, and Ag) for Ir-Fe/BN (Ir = 5 wt%, Fe/Ir = 0.25) catalyst in terminal C−O hydrogenolysis of 1,2-butanediol (1,2-BuD) to 2-butanol (2-BuOH). Only trace amount of Ru (up to 0.5 wt%) was effective in terms of high 2-BuOH selectivity (> 60%) and activity (about twice). Larger amount of Ru species (3 wt%) highly enhanced the activity but gave low selectivity to 2-BuOH with by-products of terminal C−C bond scission. Optimized catalyst (Ru(0.5)-Ir-Fe/BN) was reusable at least 4 times and gave moderate 2-BuOH yield (47%) in hydrogenolysis of 1,2-BuD. The promoting effect of Ru addition (0.5 wt%) to Ir-Fe/BN on hydrogenolysis of various alcohols was also confirmed. Combining catalytic tests with various characterizations, the promotion mechanism of Ru species in trimetallic catalysts was clarified. The Ru species in Ru(0.5)-Ir-Fe/BN form alloy with Ir and are enriched at the interface with BN surface, and direct interaction between Ru and Fe was not necessary in Ru-Ir-Fe alloy. The interface of Ir and Fe on the surface of Ir-Fe alloy may work as active sites for 1,2-diols to secondary alcohols via direct C−O hydrogenolysis, in which Ru-modified Ir activates H2 to form hydride-like species. The activity of Ru species in C−C bond cleavage was highly suppressed due to the direct interaction with Ir species and less exposed to substrate. Larger loading amount of Ru species (3 wt%) led to the formation Ru-rich trimetallic alloy, which further works as active sites for C−C bond scission.
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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