Fast Dehydrogenation of Formic Acid over Palladium Nanoparticles Immobilized in Nitrogen-Doped Hierarchically Porous Carbon

Wang, Qiuju; Tsumori, Nobuko; Kitta, Mitsunori; Xu, Qiang

doi:10.1021/acscatal.8b03444

Cited by 169 publications

(89 citation statements)

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“…Comparing to Pd@CNP and Pd@XC72, Pd@ SS-CNR with a hierarchical superstructure shows a much higher catalytic activity, which is about 1.8 and 6.3 times to Pd@CNP and Pd@XC72, respectively (Figure 4g). [37][38][39] The excellent catalytic activity for FA dehydrogenation is attributed to the unique features of hierarchical structure. Notably, when the temperature is increased to 60 °C, the reaction can be finished in only 30 s, giving an exceptionally high TOF of 7200 h −1 with 100% H 2 selectivity, which is comparable to the most active heterogeneous catalysts for FA dehydrogenation ( Figure 4h).…”

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Fabrication of a Spherical Superstructure of Carbon Nanorods

et al. 2019

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superstructure with a large radius of curvature, such as spherical organization, is still a challenge. So far, only a few kinds of 1D oxides could be assembled into 3D spherical superstructures. [13][14][15] Low-dimensional carbon nanomaterials have been widely used in energy storage and conversion owing to their distinct electrochemical properties and mechanical and thermal stability. [16][17][18] 3D superstructures constructed from lowdimensional components such as carbon nanorods/wires or graphene nanorribbons can inherit the exceptional properties of their building blocks and acquire certain unconventional advantages. [19,20] However, the self-assemblies of 1D carbon nanomaterials into 3D ordered spherical superstructures are considerably challenging owing to the reduced accessible contact areas between the building blocks and core templates. Although various synthetic approches have been developed for the synthesis of lowdimensional carbon nanostructures with well-defined size and controllable composition, [21][22][23] no techniques have been applied for controlling the assembly of 1D carbon nanomaterials into 3D spherical superstructure with uniform morphology.Metal-organic frameworks (MOF) are a class of porous crystalline materials that are constructed by metal ions/clusters and organic linkers. [24] The use of MOF as a template or precursor to synthesize carbon nanostructure is an efficient approach to produce carbon materials with controlled morphology and Hierarchical superstructures in nano/microsize have attracted great attention owing to their wide potential applications. Herein, a self-templated strategy is presented for the synthesis of a spherical superstructure of carbon nanorods (SS-CNR) in micrometers through the morphology-preserved thermal transformation of a spherical superstructure of metal-organic framework nanorods (SS-MOFNR). The self-ordered SS-MOFNR with a chestnut-shell-like superstructure composed of 1D MOF nanorods on the shell is synthesized by a hydrothermal transformation process from crystalline MOF nanoparticles. After carbonization in argon, the hierarchical SS-MOFNR transforms into SS-CNR, which preserves the original chestnut-shell-like superstructure with 1D porous carbon nanorods on the shell. Taking the advantage of this functional superstructure, SS-CNR immobilized with ultrafine palladium (Pd) nanoparticles (Pd@SS-CNR) exhibits excellent catalytic activity for formic acid dehydrogenation. This synthetic strategy provides a facile method to synthesize uniform spherical superstructures constructed from 1D MOF nanorods or carbon nanorods for applications in catalysis and energy storage. 3D SuperstructuresHierarchical superstructures are ubiquitous in the biological systems (e.g., proteins, lipids, and carbohydrates). From the aspect of synthesis, self-assembly of simple building blocks into 3D, highly ordered superstructure with novel properties has attracted great interest in the fields of optics, catalysis, and energy storage. [1][2][3][4] Highly organized building bloc...

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Fabrication of a Spherical Superstructure of Carbon Nanorods

et al. 2019

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“…In this sense, there is an increasing number of publications reporting on the investigation of catalytic systems able to catalyse the reaction while exploring the features of either support or metal active phase. Special mention should be made of those breakthroughs achieved Xu et al [29][30][31][32][33][34], and Bulushev et al [47][48][49][50][51][52][53][54][55][56][57].Most of the heterogeneous catalysts used are based on metal nanoparticles immobilised on supports of diverse nature (i.e. carbon materials, MOF, zeolites, resins, etc.)…”

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Hydrogen Production from Formic Acid Attained by Bimetallic Heterogeneous PdAg Catalytic Systems

2019

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The production of H 2 from the so-called Liquid Organic Hydrogen Carriers (LOHC) has recently received great focus as an auspicious option to conventional hydrogen storage technologies. Among them, formic acid, the simplest carboxylic acid, has recently emerged as one of the most promising candidates. Catalysts based on Pd nanoparticles are the most fruitfully investigated, and, more specifically, excellent results have been achieved with bimetallic PdAg-based catalytic systems. The enhancement displayed by PdAg catalysts as compared to the monometallic counterpart is ascribed to several effects, such as the formation of electron-rich Pd species or the increased resistance against CO-poisoning. Aside from the features of the metal active phases, the properties of the selected support also play an important role in determining the final catalytic performance. Among them, the use of carbon materials has resulted in great interest by virtue of their outstanding properties and versatility. In the present review, some of the most representative investigations dealing with the design of high-performance PdAg bimetallic heterogeneous catalysts are summarised, paying attention to the impact of the features of the support in the final ability of the catalysts towards the production of H 2 from formic acid.Energies 2019, 12, 4027 2 of 27 fact, it is challenging not only for developed countries in which the living standard requires large energy supplies, but also for those developing countries that experience a high population growth.Among greenhouse gases, carbon dioxide (CO 2 ) is considered the most important because, even though its global warming potential (GWP) is much lower than that of other gases, the emissions of CO 2 are far more abundant. GWP parameter was developed to compare the global warming impacts of different gases and it is a measure of how much energy the emissions of 1 ton of a gas will absorb over a given period, relative to the emissions of 1 ton of CO 2 , which is used as the reference. Then, CO 2 has a GWP of 1 regardless of the time used, while GWP is 28-36 and 265-298 times that of CO 2 for methane (CH 4 ) and nitrous oxide (N 2 O), respectively [1]. Such considerations, that are nowadays central scientific and social concerns, have a long historical background within the research community. Arrhenius was among the first to hypothesise about the impact of CO 2 on the Earth's climate [2], but his hypothesis was overlooked until the 1950s [3]. Now, after more than half a century, there is not yet a chemical process able to efficiently clean the growing volumes of CO 2 in the atmosphere. Some interesting actions taken so far are related to the production of hydrocarbon fuels by recycling H 2 O and CO 2 with renewable energy sources or the CO 2 capture and sequestration (CCS) technology [4][5][6][7].In such energy and environmental context, the search for alternative carbon emission-free energy sources is required to avoid further disastrous consequences. Hydrogen (H 2 ), a carbon-free fuel, is consi...

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“…Thus, the as-prepared Pd/ ZrO 2 @C exhibited signicant catalytic activity, with TOF values higher than those reported for most heterogeneous catalysts for this reaction (Table 2), except the two catalysts from the latest reports. 33,34 The apparent activation energy (E a ) of this process was estimated to be 42.95 kJ mol À1 . Finally, the recycling stability of the Pd/ZrO 2 @C is tested (Fig.…”

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confidence: 99%

“…[29][30][31] Despite this, MOF-derived metal oxides and carbon complex supports have rarely been applied to FA decomposition. [32][33][34] In terms of monometallic Pd catalysts, the size of the Pd NPs especially plays an important role in catalyst activity. For smaller metal NPs usually have a high surface-to-volume ratio and hence could able to provide a higher density of active sites exposed to reactants, which is signicance for heterogeneous catalysis.…”

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confidence: 99%

Enhanced catalytic activity over palladium supported on ZrO₂@C with NaOH-assisted reduction for decomposition of formic acid

Wang

et al. 2019

RSC Adv.

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Fast Dehydrogenation of Formic Acid over Palladium Nanoparticles Immobilized in Nitrogen-Doped Hierarchically Porous Carbon

Cited by 169 publications

References 45 publications

Fabrication of a Spherical Superstructure of Carbon Nanorods

Fabrication of a Spherical Superstructure of Carbon Nanorods

Hydrogen Production from Formic Acid Attained by Bimetallic Heterogeneous PdAg Catalytic Systems

Enhanced catalytic activity over palladium supported on ZrO₂@C with NaOH-assisted reduction for decomposition of formic acid

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Fast Dehydrogenation of Formic Acid over Palladium Nanoparticles Immobilized in Nitrogen-Doped Hierarchically Porous Carbon

Cited by 169 publications

References 45 publications

Fabrication of a Spherical Superstructure of Carbon Nanorods

Fabrication of a Spherical Superstructure of Carbon Nanorods

Hydrogen Production from Formic Acid Attained by Bimetallic Heterogeneous PdAg Catalytic Systems

Enhanced catalytic activity over palladium supported on ZrO2@C with NaOH-assisted reduction for decomposition of formic acid

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Enhanced catalytic activity over palladium supported on ZrO₂@C with NaOH-assisted reduction for decomposition of formic acid