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用于CO加氢的定制催化剂:NH-MIL-125骨架的合成与表征

Tailoring Catalysts for CO Hydrogenation: Synthesis and Characterization of NH-MIL-125 Frameworks.

作者信息

Figueroa-Quintero Leidy, Cordero-Lanzac Tomás, Ramos-Fernandez Enrique V, Olsbye Unni, Narciso Javier

机构信息

Inorganic Chemistry Department, Laboratory of Advanced Materials, University Materials Institute of Alicante, University of Alicante, 03080 Alicante, Spain.

SMN Centre for Materials Science and Nanotechnology, Department of Chemistry, University of Oslo, Sem Saelands Vei 26, 0371 Oslo, Norway.

出版信息

Molecules. 2025 Mar 25;30(7):1458. doi: 10.3390/molecules30071458.

DOI:10.3390/molecules30071458
PMID:40286045
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11990164/
Abstract

Copper nanoparticles have been integrated onto the framework of modified NH-MIL-125(Ti), a metal-organic framework (MOF), and evaluated as catalysts for converting CO into valuable products. The modified MOF was achieved through a post-synthetic modification process involving the partial replacement of titanium with zirconium or cerium within the MOF's structure. The objective behind this alteration is to create a synergistic effect between the MOF, serving as a support matrix, and the embedded copper nanoparticles, thereby enhancing the performance of the catalyst. The obtained catalysts were characterized and evaluated in the hydrogenation of CO to methanol under different experimental conditions, reaching CO conversions of up to 5%, with a selectivity towards methanol that reached values of up to 60%. According to the obtained results, the catalyst composed of Ti, Zr and Cu stood out for having the highest CO conversion and selectivity towards methanol, in addition to practically inhibiting the production of methane. These results demonstrate that the interaction of the framework with the Cu nanoparticles, and thus its catalytic properties, can be changed by modifying the properties of the MOF.

摘要

铜纳米颗粒已被整合到改性NH-MIL-125(Ti)(一种金属有机框架材料,简称MOF)的框架上,并被评估为将CO转化为有价值产品的催化剂。改性MOF是通过合成后修饰过程实现的,该过程涉及在MOF结构中用锆或铈部分替代钛。这种改变背后的目的是在作为支撑基质的MOF和嵌入的铜纳米颗粒之间产生协同效应,从而提高催化剂的性能。所获得的催化剂在不同实验条件下进行了CO加氢制甲醇的表征和评估,CO转化率高达5%,对甲醇的选择性高达60%。根据所得结果,由Ti、Zr和Cu组成的催化剂表现突出,除了几乎抑制甲烷的生成外,还具有最高的CO转化率和对甲醇的选择性。这些结果表明,通过改变MOF的性质,可以改变框架与铜纳米颗粒的相互作用,进而改变其催化性能。

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本文引用的文献

1
CO-Based Stable Porous Metal-Organic Frameworks for CO Utilization.用于一氧化碳利用的基于一氧化碳的稳定多孔金属有机框架材料。
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A Ce-CuZn catalyst with abundant Cu/Zn-O-Ce active sites for CO hydrogenation to methanol.一种具有丰富Cu/Zn-O-Ce活性位点的Ce-CuZn催化剂,用于CO加氢制甲醇。
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Copper nanoparticles encapsulated in zeolitic imidazolate framework-8 as a stable and selective CO hydrogenation catalyst.
封装在沸石咪唑酯骨架-8中的铜纳米颗粒作为一种稳定且选择性的CO加氢催化剂。
Nat Commun. 2024 Mar 6;15(1):2045. doi: 10.1038/s41467-024-46388-4.
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Transitioning from Methanol to Olefins (MTO) toward a Tandem CO Hydrogenation Process: On the Role and Fate of Heteroatoms (Mg, Si) in MAPO-18 Zeotypes.从甲醇制烯烃(MTO)向串联式CO加氢过程的转变:关于杂原子(Mg、Si)在MAPO-18型沸石中的作用和归宿
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Enabling the Methanol Economy: Opportunities and Challenges for Heterogeneous Catalysis in the Production of Liquid Fuels via Methanol.推动甲醇经济:通过甲醇生产液体燃料中多相催化面临的机遇与挑战。
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Selective Gas-Phase Hydrogenation of CO to Methanol Catalysed by Metal-Organic Frameworks.金属有机框架催化CO选择性气相加氢制甲醇
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7
Defective zirconium/titanium bimetallic metal-organic framework as a highly selective and sensitive electrochemical aptasensor for deoxynivalenol determination in foodstuffs.缺陷锆/钛双金属金属有机骨架作为一种高选择性和高灵敏度的电化学适体传感器,用于食品中脱氧雪腐镰刀菌烯醇的测定。
Mikrochim Acta. 2023 Aug 21;190(9):358. doi: 10.1007/s00604-023-05935-4.
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Thermocatalytic Conversion of CO to Valuable Products Activated by Noble-Metal-Free Metal-Organic Frameworks.由无贵金属金属有机框架激活的CO向有价值产物的热催化转化
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