Ultra-Small Face-Centered-Cubic Ru Nanoparticles Confined within a Porous Coordination Cage for Dehydrogenation

Fang, Yu; Li, Jialuo; Togo, Tatsuo; Jin, Fangying; Xiao, Zhifeng; Liu, Lujia; Drake, Hannah F.; Lian, Xizhen; Zhou, Hong‐Cai

doi:10.1016/j.chempr.2018.01.004

Cited by 119 publications

(104 citation statements)

References 57 publications

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“…Surprisingly, in the presence of PRO, the Rh‐PRO/C with the same Rh loading (2.5 wt %) provided an efficient performance for hydrogen release, giving the initial turnover frequency of 410.8 mol

_{normalH_{2}}

(mol Rh min) −1 (Figure a). The catalytic activity was considerably higher than the previously reported performance achieved . The presence of OH − has been reported to promote the rate‐determining step of O−H bond cleavage in H 2 O and activate AB in the hydrolysis of AB to H 2 .…”

Section: Resultsmentioning

confidence: 90%

Ultrahigh Catalytic Activity of l‐Proline‐Functionalized Rh Nanoparticles for Methanolysis of Ammonia Borane

Luo

Cheng

et al. 2018

ChemSusChem

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The synthesis of ultrafine and well‐distributed rhodium nanoparticles (NPs) with high efficiency toward methanolysis of ammonia borane (AB) is crucially important but challenging. A facile approach has been developed for synthesizing ultrafine and uniform Rh NPs deposited on carbon by using the small soluble organic molecule (SOM) of l‐proline (PRO) as capping agent (Rh‐PRO/C). The enrichment of N,O‐coordination sites for the metal precursor by using PRO was found to be the key to the synthesis Rh‐PRO/C. The as‐prepared Rh‐PRO/C showed high catalytic activity for ammonia borane methanolysis with the highest total turnover frequency (TOF) of 1035 molnormalH2 (molRh min)−1 under basic conditions, which was three times higher than that of the state‐of‐the‐art Rh‐based catalysts. The excellent catalytic performance of Rh‐PRO/C was ascribed to the well‐dispersed Rh NPs and the PRO‐functionalized metal surface, which can provide more active sites for the reaction. The merit of size‐controlled synthesis combined with metal NP surface modification by SOMs is likely to be beneficial in various catalytic fields.

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_{normalH_{2}}

Section: Resultsmentioning

confidence: 90%

Ultrahigh Catalytic Activity of l‐Proline‐Functionalized Rh Nanoparticles for Methanolysis of Ammonia Borane

Luo

Cheng

et al. 2018

ChemSusChem

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“…The giant diameter of over 100 nanometers of our CP based catalysts was unrivaled by other supported catalysts. For example the highly active caged Ru particles only has a size of around 2.5 nm, almost 2 order smaller than our catalyst. The huge size of CP2 − Au 0.1 Rh 0.9 could allow the use of membranes with large pores and therefore high transportation rate.…”

Section: Methodsmentioning

confidence: 73%

“…Recently NPs stabilized by homogeneous organic compounds with judicious design were shown to produce very high TOFs. For example Ru NPs trapped within a metal organic cage with 2.5 nm diameter exhibited TOFs of 304 min −1 , one of the highest before this manuscript . Qiang et al.…”

Section: Methodsmentioning

confidence: 76%

“…For example Ru NPs trapped within a metal organic cage with 2.5 nm diameter exhibited TOFs of 304 min À 1 , one of the highest before this manuscript. [18] Qiang et al reported another example of Rh NPs stabilized by small organic cages with a TOF around 215 min À 1 . [19] However, examples of efficient homogeneous AB decomposition catalyzed by NPs beyond these two examples have still remained rare.…”

Section: Donut Assembly Of Nanoparticles With High Catalytic Efficienmentioning

confidence: 99%

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Donut Assembly of Nanoparticles with High Catalytic Efficiency for Hydrogen Gas Generation from Ammonia Borane

Liu

et al. 2019

ChemCatChem

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Polymer‐supported transition metal nano particles usually exhibited low catalytic efficiency due to the long diffusion length for the reactants to reach the catalytic center. Herein, we used cyclic polymers to construct donut‐like assembly with two cyclic macromolecules sandwiching a layer of metal NPs. Doping Rh into the nano particles led to extremely active catalysts for ammonia borane decomposition with a high TOF of 780 min−1. We attributed the high efficiency to the reduced diffusion length in this special assembly. Light‐promoted effect was also demonstrated with TOF further elevated to 980 min−1. The modular nature of this design also permitted subsequent structural modification to achieve high stability with TON reaching over 2×106.

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“…So far, a large variety of heterogeneous nanocatalysts, including noble and non‐noble metals as well as their alloys and compounds, have been evaluated for the hydrolysis of AB . Among them, ruthenium (Ru) nanoclusters have been identified as one of the highest potential nanocatalysts for AB hydrolysis due to its economy and efficiency …”

Section: Introductionmentioning

confidence: 99%

Ultrasmall Ru Nanoclusters on Nitrogen‐Enriched Hierarchically Porous Carbon Support as Remarkably Active Catalysts for Hydrolysis of Ammonia Borane

Zhang

Wang

et al. 2018

ChemCatChem

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The development of the highly active nanocatalysts for effective hydrogen (H 2 ) production is of great significance for its practical applications in fuel cells. Herein, we reported a facile and scaleup synthetic methodology to grow in situ the remarkably active nanocatalysts of ultrasmall Ru nanoclusters on nitrogen (N)enriched hierarchically macroporous-mesoporous carbon supports (Ru@hPCN). The resultant Ru@hPCN combines structural and chemical merits of well-dispersed 0.7-nm Ru nanoclusters, N-enriched functional surface and 3D hierarchically porous framework, all of which synergistically boost the catalytic performance toward the hydrolysis of ammonia-borane (AB). An unprecedented activity with a turnover frequency of 1850 min À1 was achieved for the Ru@hPCN, which was 6.0 folds over that of commercialized Ru/C catalyst. Mechanism studies showed that the remarkably enhanced activity can be ascribed to the easier dissociation of electropositive H d + from H 2 O and the breakage of the BÀN bonds as well as favorable mass transport in the Ru@hPCN during AB hydrolysis.[a] Dr. scanning X-ray microprobe (Thermo ESCALAB 250Xi) with Al Ka radiation. ICP-MS was recorded on NexION 350D.

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Ultra-Small Face-Centered-Cubic Ru Nanoparticles Confined within a Porous Coordination Cage for Dehydrogenation

Cited by 119 publications

References 57 publications

Ultrahigh Catalytic Activity of l‐Proline‐Functionalized Rh Nanoparticles for Methanolysis of Ammonia Borane

Ultrahigh Catalytic Activity of l‐Proline‐Functionalized Rh Nanoparticles for Methanolysis of Ammonia Borane

Donut Assembly of Nanoparticles with High Catalytic Efficiency for Hydrogen Gas Generation from Ammonia Borane

Ultrasmall Ru Nanoclusters on Nitrogen‐Enriched Hierarchically Porous Carbon Support as Remarkably Active Catalysts for Hydrolysis of Ammonia Borane

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