Synthesis of Supported Ultrafine Non‐noble Subnanometer‐Scale Metal Particles Derived from Metal–Organic Frameworks as Highly Efficient Heterogeneous Catalysts

Kang, Xinchen; Huizhen, Liu; Hou, Meiying; Sun, Xiaofu; Han, Hongling; Jiang, Tao; Zhang, Zhaofu; Han, Buxing

doi:10.1002/anie.201508107

Cited by 76 publications

(51 citation statements)

References 49 publications

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“…The high‐resolution TEM image presented in Figure d shows Ni NPs of approximately 5 nm, and the (1 1 1) plane can be identified easily according to the lattice fringe of 0.202 nm. Notably, the preparation of nano‐sized Ni catalysts, especially with particle size less than 10 nm and with a very high loading, remains a great challenge …”

Section: Resultsmentioning

confidence: 98%

Nickel/USY Catalyst Derived from a Layered Double Hydroxide/Zeolite Hybrid Structure with a High Hydrogenation Efficiency

Wang

Guan

et al. 2017

ChemCatChem

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It is important and challenging in heterogeneous catalysis to prepare catalysts with highly dispersed metal nanoparticles that have a high activity. Herein, a new Ni/USY catalyst derived from a core–shell NiAl‐LDHs/USY hybrid material has been prepared by the in situ growth of a layered double hydroxides (LDHs) precursor on the surface of USY zeolite crystals. Under the appropriate conditions, the adscititious Ni source interacted chemoselectively with Al species dissolved from the zeolite framework to form a LDHs structure anchored robustly on the surface of zeolite crystals. The dealumination of the low‐silica zeolite and the immobilization of Ni metal species were realized simultaneously in this one‐pot synthesis to afford hierarchical NiAl‐LDHs/USY hybrid composites. The NiII species in these hybrid composites were reduced readily at much lower temperatures than that of bulk NiAl‐LDH, which gave rise to highly dispersed Ni nanoparticles. Meanwhile, the resultant material possessed an excellent mesoporous structure and a high surface area inherited from the USY structure, which led to an excellent hydrogenation rate and activity for the conversion of m‐nitroaniline to m‐phenylenediamine. This unique method could be a promising and general strategy to fabricate desirable hybrid materials for redox catalysis in particular for supported transition metals with similar characteristics to Ni.

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Section: Resultsmentioning

confidence: 98%

Nickel/USY Catalyst Derived from a Layered Double Hydroxide/Zeolite Hybrid Structure with a High Hydrogenation Efficiency

Wang

Guan

et al. 2017

ChemCatChem

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“…[23][24][25][26] Taking advantage of this category of the systems, we demonstrate a facile synthetic route to fabricate hollow hierarchical Ni@C nanocomposite by one-step solid-state pyrolysis of a simple and inexpensive organic-inorganic layered nickel hydroxides. In this facile procedure, cheap commercially available nickel nitrate hexahydrate and sodium salicylate are used as starting materials, and during the pyrolysis process the interlayer salicylate anions act as carbon source and reducing agent without the need for any external agent or surface modication.…”

Section: -7mentioning

confidence: 99%

Facile synthesis of hollow hierarchical Ni@C nanocomposites with well-dispersed high-loading Ni nanoparticles embedded in carbon for reduction of 4-nitrophenol

et al. 2018

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Hollow hierarchical Ni@C nanocomposites with highly dispersed Ni nanoparticles (NPs) embedded in wellgraphitized carbon matrix have been synthesized by solid-state pyrolysis of simple, well-defined organicinorganic layered nickel hydroxide. The integration of highly dispersed Ni NPs, high Ni NPs content (up to $88.01 wt%), well-graphitized carbon as well as strong Ni/carbon interaction in the Ni@C make them display excellent catalytic activity and stable magnetic recyclability toward the reduction of 4-nitrophenol by NaBH 4 .The development of more efficient and stable catalysts has been an increasingly important goal for chemists and materials scientists for both economic and environmental reasons. As efficient and cost-effective non-noble metal, Ni NPs have attracted much attention owing to their potential applications in electronic or optical materials, as well as in catalysis.1-3 In general, the overall performance of Ni NPs depends heavily upon the size, shape and dispersion. It is widely accepted that a higher catalytic activity can be achieved by increasing the surface area of the specic active phase of the catalysts through reducing the size of the corresponding catalytic particles. 4-7However, due to their high surface area to volume ratio, Ni NPs are typically unstable and tend to sinter into larger species, especially at high metal contents, which results in a dramatic decrease in catalytic activity and selectivity. It is thus highly important to prepare stable Ni NPs with uniform dispersion and narrow size distribution to promote their catalytic activities.Over the past decades, embedding of Ni NPs inside the porous supports has been proved to enhance catalytic activity and impede nanoparticle sintering. [8][9][10][11][12][13][14][15] The advantages of carbon supports with respect to conventional oxidic supports, like silica and zirconia, involve the high specic surface area, high stability, intrinsic high electrical conductivity, as well as easy recovery of metal active phases from spent catalysts by burning away carbon. To date, various methods for preparing carbon-supported Ni NPs have been developed. [16][17][18][19][20][21][22] In particular, incipient wetness impregnation and coprecipitation are commonly used methods to prepare these supported catalysts. It is well known that traditional carbons (including activated carbon, carbon nanotubes, graphene and carbon nanobers) are poor in functional groups and a complex functionalization pre-treatment (such as acid oxidation, ionic liquid linking or polymer wrapping) is always required. In addition, the excess reducing regents are also needed for the reduction of Ni NPs. Although a high dispersion of Ni NPs on porous carbon can be achieved by employing this methods, this tedious post-synthetic method renders instable catalysts with dispersed Ni NPs on the external surface or near pore mouths and Ni NPs still have a tendency to be sintered, especially at high metal loading or high temperature, resulting in a signicant loss of reactivity because of...

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“…[4] This is driven by the fact that the metal building blocks are well defined and, more often than not, highly dispersed. [7] While numerousw orks show exceptional catalytic properties of MOF-derived carbons containing metal or metal oxide NPs, the use of MOF-derived transition-metal sulfides,p hosphides, and carbides for thermally driven organic transformations only recently made its debut. [5] Compared with traditional methods for the impregnationo fp orous supports with NPs, the dispersity andh omogeneity of which is often not well controlled, MOF-derived materials promote the creation of small, homogeneous, catalytically active species inside the resulting mesoporous carbon networks.F or example, Li et al recently reported highly dispersed single cobalt atoms and Fe-Co dual sites embedded in N-doped porous carbon.T his material, createdt hrough the pyrolysis of ap redesignedb imetallic Zn/Co MOF, [6] was shown to be highly efficient in the electrochemical oxygen reduction reaction.…”

Section: Introductionmentioning

confidence: 99%

Metal–Organic‐Framework‐Derived Co₃S₄ Hollow Nanoboxes for the Selective Reduction of Nitroarenes

Yang

Sun

et al. 2018

ChemSusChem

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MOF-derived Co S /CN hollow nanoboxes (CN=nitrogen-doped carbon) was used to catalyze the chemoselective reduction of nitroarenes to anilines under mild reaction conditions with H as the reducing agent. The catalyst provides high conversion efficiencies and selectivities for a variety of nitroarene substrates that contain electron-donating or electron-withdrawing substituents under mild reaction conditions (in methanol at 60 °C). Further, the nanobox inhibits both dehalogenation and vinyl hydrogenation reactions, which are common limitations of state-of-the-art Pd-based catalysts. Because the reactions result in pure aniline products, the need for separation by column chromatography is eliminated. The resulting anilines are easily separated from the methanolic reaction solution in just three simple steps (centrifugation, decantation, and drying). If employed in industrial processes, catalysts of this kind would significantly reduce the amount of waste organic solvent generated and thus satisfy the need for sustainable chemical processes.

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Synthesis of Supported Ultrafine Non‐noble Subnanometer‐Scale Metal Particles Derived from Metal–Organic Frameworks as Highly Efficient Heterogeneous Catalysts

Cited by 76 publications

References 49 publications

Nickel/USY Catalyst Derived from a Layered Double Hydroxide/Zeolite Hybrid Structure with a High Hydrogenation Efficiency

Nickel/USY Catalyst Derived from a Layered Double Hydroxide/Zeolite Hybrid Structure with a High Hydrogenation Efficiency

Facile synthesis of hollow hierarchical Ni@C nanocomposites with well-dispersed high-loading Ni nanoparticles embedded in carbon for reduction of 4-nitrophenol

Metal–Organic‐Framework‐Derived Co₃S₄ Hollow Nanoboxes for the Selective Reduction of Nitroarenes

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Synthesis of Supported Ultrafine Non‐noble Subnanometer‐Scale Metal Particles Derived from Metal–Organic Frameworks as Highly Efficient Heterogeneous Catalysts

Cited by 76 publications

References 49 publications

Nickel/USY Catalyst Derived from a Layered Double Hydroxide/Zeolite Hybrid Structure with a High Hydrogenation Efficiency

Nickel/USY Catalyst Derived from a Layered Double Hydroxide/Zeolite Hybrid Structure with a High Hydrogenation Efficiency

Facile synthesis of hollow hierarchical Ni@C nanocomposites with well-dispersed high-loading Ni nanoparticles embedded in carbon for reduction of 4-nitrophenol

Metal–Organic‐Framework‐Derived Co3S4 Hollow Nanoboxes for the Selective Reduction of Nitroarenes

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Metal–Organic‐Framework‐Derived Co₃S₄ Hollow Nanoboxes for the Selective Reduction of Nitroarenes