A rare earth hydride supported ruthenium catalyst for the hydrogenation of<i>N</i>-heterocycles: boosting the activity<i>via</i>a new hydrogen transfer path and controlling the stereoselectivity

Wu, Yong; Yu, Hang; Guo, Yafei; Jiang, Xiaojing; Qi, Yue; Sun, Bingxue; Li, Haiwen; Zheng, Jianlong; Li, Xingguo

doi:10.1039/c9sc04365a

Cited by 52 publications

(22 citation statements)

References 41 publications

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“…S6 and S16). So, the initial major activity decrease might be attributed to the surface sorption of solvent impurities and/or reaction species at very low content, resulting in partial blockage of the surface sites ( 41 ).…”

Section: Resultsmentioning

confidence: 99%

Metal-free carbocatalyst for room temperature acceptorless dehydrogenation of N-heterocycles

Nie

Tao

et al. 2022

Sci. Adv.

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Catalytic dehydrogenation enables reversible hydrogen storage in liquid organics as a critical technology to achieve carbon neutrality. However, oxidant or base-free catalytic dehydrogenation at mild temperatures remains a challenge. Here, we demonstrate a metal-free carbocatalyst, nitrogen-assembly carbons (NCs), for acceptorless dehydrogenation of N-heterocycles even at ambient temperature, showing greater activity than transition metal–based catalysts. Mechanistic studies indicate that the observed catalytic activity of NCs is because of the unique closely placed graphitic nitrogens (CGNs), formed by the assembly of precursors during the carbonization process. The CGN site catalyzes the activation of C─H bonds in N-heterocycles to form labile C─H bonds on catalyst surface. The subsequent facile recombination of this surface hydrogen to desorb H 2 allows the NCs to work without any H-acceptor. With reverse transfer hydrogenation of various N-heterocycles demonstrated in this work, these NC catalysts, without precious metals, exhibit great potential for completing the cycle of hydrogen storage.

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Section: Resultsmentioning

confidence: 99%

Metal-free carbocatalyst for room temperature acceptorless dehydrogenation of N-heterocycles

Nie

Tao

et al. 2022

Sci. Adv.

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“…The hydrogenation of LOHC compounds is usually performed over Ru catalysts using different supports, since Ru carries a strong electronic structure with a lower d-band center position. − Accordingly, the most studied catalysts for hydrogenation of monobenzyltoluene (MBT) are Ru-based catalysts. Leinweber and Müller studied hydrogenation of MBT on a Ru/Al 2 O 3 catalyst which showed that the low substituted ring hydrogenation is preferred over higher substituted ring hydrogenation .…”

Section: Heterogeneous Catalysts For Dbtmentioning

confidence: 99%

Novel Catalysts for Dibenzyltoluene as a Potential Liquid Organic Hydrogen Carrier Use—A Mini-review

et al. 2021

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The utilization of pure and valuable energy carriers such as hydrogen is becoming important in various applications, especially in the automotive fuel cell industry. However, as a result of the properties and character of hydrogen, its storage is not easy. Therefore, there is a need for systems such as liquid organic hydrogen carriers (LOHCs), which fulfill safety standards and are a flexible medium for the storage and transmission of sustainable energy. The heat transfer oil dibenzyltoluene is a novel LOHC system which can offer superior hydrogen storage capacity. Dibenzyltoluene has a good thermal stability and excellent physicochemical properties for LOHC applications in industry (Hydrogenation of the liquid organic hydrogen carrier compound dibenzyltoluene – reaction pathway determination by 1H NMR spectroscopyReact. Chem. Eng.20161313320). In this Review, the experimental study of dibenzyltoluene with the use of catalysts and the theoretical study of dibenzyltoluene through computational modeling and simulations are explored and discussed. The focus is on heterogeneous catalysts which can be used in hydrogenation and dehydrogenation of dibenzyltoluene.

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“…Precious metal-based heterogeneous catalysts like Rh, , Pd, Pt, , and Ru − have been extensively explored for N-heteroarene hydrogenation due to their high activity. Among them, Ru has received particular attention owing to its relatively low cost. , However, Ru suffers from low H desorption and strong adsorption towards hydrogenated substrates, owing to its strong affinity to H and intermediates, which seriously compromises its catalytic hydrogenation activity. , As we know, the adsorption of reactants or/and intermediates on metal sites is highly related to their electronic structures.…”

Section: Introductionmentioning

confidence: 99%

Ru Nanoclusters Supported on Ti₃C₂T_x Nanosheets for Catalytic Hydrogenation of Quinolines

Zhao

Zhang

Wang

et al. 2022

ACS Appl. Nano Mater.

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Ru-based catalysts hold great promise for selective hydrogenation of quinolines. However, the slow desorption of active H and strong adsorption of hydrogenated substrates on the Ru active sites seriously hinder their industrial applications. Herein, we design Ti3C2T x -supported Ru nanocluster catalysts by loading Ru nanoclusters on two-dimensional (2D) Ti3C2T x nanosheets. The Ti3C2T x nanosheets with unique 2D structure and rich surface-terminated functional groups afford the formed Ru nanoclusters (RuNCs) with small size and high dispersity. The as-prepared RuNCs/Ti3C2T x catalysts exhibit excellent catalytic activity and selectivity for the hydrogenation of quinolines. The theoretical calculation confirms that there exists charge transfer between Ru and the functional groups (e.g., F and O) on Ti3C2T x , which can weaken the H adsorption and promote the desorption of hydrogenated products, contributing to the outstanding hydrogenation performance of RuNCs/Ti3C2T x catalysts. The findings pave an avenue towards improving the hydrogenation performance of quinolines over Ru-based catalysts.

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A rare earth hydride supported ruthenium catalyst for the hydrogenation ofN-heterocycles: boosting the activityviaa new hydrogen transfer path and controlling the stereoselectivity

Abstract: A novel Ru/YH3 catalyst with excellent performance in terms of activity and stereoselectivity for hydrogenation of N-heterocycles is developed.

Cited by 52 publications

References 41 publications

Metal-free carbocatalyst for room temperature acceptorless dehydrogenation of N-heterocycles

Metal-free carbocatalyst for room temperature acceptorless dehydrogenation of N-heterocycles

Novel Catalysts for Dibenzyltoluene as a Potential Liquid Organic Hydrogen Carrier Use—A Mini-review

Ru Nanoclusters Supported on Ti₃C₂T_x Nanosheets for Catalytic Hydrogenation of Quinolines

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A rare earth hydride supported ruthenium catalyst for the hydrogenation ofN-heterocycles: boosting the activityviaa new hydrogen transfer path and controlling the stereoselectivity

Abstract: A novel Ru/YH3 catalyst with excellent performance in terms of activity and stereoselectivity for hydrogenation of N-heterocycles is developed.

Cited by 52 publications

References 41 publications

Metal-free carbocatalyst for room temperature acceptorless dehydrogenation of N-heterocycles

Metal-free carbocatalyst for room temperature acceptorless dehydrogenation of N-heterocycles

Novel Catalysts for Dibenzyltoluene as a Potential Liquid Organic Hydrogen Carrier Use—A Mini-review

Ru Nanoclusters Supported on Ti3C2Tx Nanosheets for Catalytic Hydrogenation of Quinolines

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Ru Nanoclusters Supported on Ti₃C₂T_x Nanosheets for Catalytic Hydrogenation of Quinolines