One-pot tandem catalysis over Pd@MIL-101: boosting the efficiency of nitro compound hydrogenation by coupling with ammonia borane dehydrogenation

Yang, Qihao; Chen, Yuzhen; Wang, Zhiyong U.; Xu, Qiang; Jiang, Hai‐Long

doi:10.1039/c5cc03102h

Cited by 160 publications

(69 citation statements)

References 57 publications

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“…Their production is heavily dependent on the reduction of their corresponding nitro compounds with noble metal catalysts under high pressures of H 2 and/or high temperatures to boost the contact between H 2 and the nitro compounds . Recently, a tandem catalysis system combining in situ H 2 generation from typical H 2 sources, such as NaBH 4 and NH 3 BH 3 , and reduction of nitro compounds has been proved to be effective to improve the reaction kinetics, because such in situ generated H 2 molecules can react with nitro groups readily . However, noble metal catalysts have the issues of high cost and scarcity, and they often show not well‐matched hydrogen‐generation and nitro‐group‐reduction kinetics in the tandem reactions.…”

Section: Methodsmentioning

confidence: 99%

“…[12e,f] Moreover, it has been reported that pyrrolic N species have strong ability to absorb nitro compounds, activate nitro groups, and induce favorable energetic charges during heterogeneous catalytic processes. [16c] For the Co2p XPS data, the signals are relatively weak because most Co species are located inside the silica matrix. The peaks at ≈778.6 and 781.7 eV (Figure D) could be attributed to metallic Co and N‐coordinated Co, respectively, further implying that the N sites can act as coordination and anchoring sites for Co.…”

Section: Methodsmentioning

confidence: 99%

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Conformal Coating of Co/N‐Doped Carbon Layers into Mesoporous Silica for Highly Efficient Catalytic Dehydrogenation–Hydrogenation Tandem Reactions

Zhang

Wei

Yao

et al. 2017

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To maximize the utilizing efficiency of cobalt (Co) and optimize its catalytic activity and stability, engineering of size and interfacial chemical properties, as well as controllable support are of ultimate importance. Here, the concept of coating uniform thin Co/N-doped carbon layers into the mesopore surfaces of mesoporous silica is proposed for heterogeneous aqueous catalysis. To approach the target, a one-step solvent-free melting-assisted coating process, i.e., heating a mixture of a cobalt salt, an amino acid (AA), and a mesoporous silica, is developed for the synthesis of mesoporous composites with thin Co/N-doped carbon layers uniformly coated within mesoporous silica, high surface areas (250-630 m g ), ordered mesopores (7.0-8.4 nm), and high water dispersibility. The strong silica/AA adhesive interactions and AA cohesive interactions direct the uniform coating process. The metal/N coordinating, carbon anchoring, and mesopore confining lead to the formation of tiny Co nanoclusters. The carbon intercalation and N coordination optimize the interfacial properties of Co for catalysis. The optimized catalyst exhibits excellent catalytic performance for tandem hydrogenation of nitrobenzene and dehydrogenation of NaBH with well-matched reaction kinetics, 100% conversion and selectivity, high turnover frequencies, up to ≈6.06 mol mol min , the highest over transition-metal catalysts, and excellent stability and magnetic separability.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Conformal Coating of Co/N‐Doped Carbon Layers into Mesoporous Silica for Highly Efficient Catalytic Dehydrogenation–Hydrogenation Tandem Reactions

Zhang

Wei

Yao

et al. 2017

Small

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“…However, it is often difficult to realize precise control of the loading position of active NPs relative to the host MOF, because some precursors might deposit on the external surface of MOFs to form aggregated counterparts . To make active NPs exclusively encapsulated inside MOF matrix and prevent them from aggregation, one of the most effective “ship‐in‐a‐bottle” ways by far is the double‐solvent approach, in which metal precursors are introduced into the cavities or channels of MOFs by the capillary force, followed by reduction or heat treatment …”

Section: Controllable Synthesis Of Active Nps Encapsulated By Mofsmentioning

confidence: 99%

Metal–Organic Frameworks Encapsulating Active Nanoparticles as Emerging Composites for Catalysis: Recent Progress and Perspectives

et al. 2018

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Beyond conventional porous materials, metal–organic frameworks (MOFs) have aroused great interest in the construction of nanocatalysts with the characteristics of catalytically active nanoparticles (NPs) confined into the cavities/channels of MOFs or surrounded by MOFs. The advantages of adopting MOFs as the encapsulating matrix are multifold: uniform and long‐range ordered cavities can effectively promote the mass transfer and diffusion of substrates and products, while the diverse metal nodes and tunable organic linkers may enable outstanding synergy functions with the encapsulated active NPs. Herein, some key issues related to MOFs for catalysis are discussed. Then, state‐of‐the art progress in the encapsulation of catalytically active NPs by MOFs as well as their synergy functions for enhanced catalytic performance in the fields of thermo‐, photo‐, and electrocatalysis are summarized. Notably, encapsulation‐structured nanocatalysts exhibit distinct advantages over conventional supported catalysts, especially in terms of the catalytic selectivity and stability. Finally, challenges and future developments in MOF‐based encapsulation‐structured nanocatalysts are proposed. The aim is to deliver better insight into the design of well‐defined nanocatalysts with atomically accurate structures and high performance in challenging reactions.

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“…Cu 2+ @MIL‐101 was prepared via double solvents method according to pervious reports . Typically, activated MIL‐101 (0.200 g) was suspended in 50 ml of dry n ‐hexane as a hydrophobic solvent in a round‐bottomed flask and the mixture was sonicated for 30 min until the sample was dispersed in the n ‐hexane.…”

Section: Methodsmentioning

confidence: 99%

In situ synthesis of metallophthalocyanines into pores of MIL‐101: A novel and green strategy for preparation of host–guest catalysts

Boroujeni

Hashemzadeh

Shaabani

et al. 2017

Applied Organom Chemis

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A novel strategy is developed to encapsulate metallophthalocyanines (MPcs, M = Cu, Ni and Co) into MIL-101 to give MPcs@MIL-101 via in situ synthesis of MPcs from component fragments in 1-butyl-3-methylimidazolium bromide as an ionic liquid. This strategy overcomes some drawbacks of existing methods for encapsulation of MPcs into metal-organic frameworks. The chemical and structural properties of MPcs@MIL-101 were determined using scanning electron microscopy, powder X-ray diffraction, and Fourier transformation infrared and flame atomic absorption spectroscopies. The results showed that CuPc@MIL-101, which was used as a 'ship-in-a-bottle' catalyst, demonstrates excellent catalytic performance in the oxidative amidation of aldehydes with amine salts. It is confirmed that CuPc@MIL-101 can be reused up to five times without significant loss of its activity.

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One-pot tandem catalysis over Pd@MIL-101: boosting the efficiency of nitro compound hydrogenation by coupling with ammonia borane dehydrogenation

Cited by 160 publications

References 57 publications

Conformal Coating of Co/N‐Doped Carbon Layers into Mesoporous Silica for Highly Efficient Catalytic Dehydrogenation–Hydrogenation Tandem Reactions

Conformal Coating of Co/N‐Doped Carbon Layers into Mesoporous Silica for Highly Efficient Catalytic Dehydrogenation–Hydrogenation Tandem Reactions

Metal–Organic Frameworks Encapsulating Active Nanoparticles as Emerging Composites for Catalysis: Recent Progress and Perspectives

In situ synthesis of metallophthalocyanines into pores of MIL‐101: A novel and green strategy for preparation of host–guest catalysts

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