Atomic Pyridinic Nitrogen Sites Promoting Levulinic Acid Hydrogenations over Double‐Shelled Hollow Ru/C Nanoreactors

Liu, Xiaoyan; Ye, Sheng; Lan, Guojun; Su, Panpan; Zhang, Xiaoli; Price, Cameron Alexander Hurd; Liu, Ying; Liu, Jian

doi:10.1002/smll.202101271

Cited by 30 publications

(29 citation statements)

References 42 publications

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“…Metal–N species [27,30,40,44–47,128] Regulate acid site [28] Change reduction state [35,42] Improve hydrophilicity [28] Increase alkalinity of site [12,23,27,34,45,130] Interaction between metal and N [26,30] Increase the adsorption of substrate [33] Improve metal dispersion [24,25,27,29,31,32,35,36,40,44,45,48] …”

Section: Metal Catalyst Anchored By Heteroatomsmentioning

confidence: 99%

“…The strong metal-sulfur bonding can not only greatly inhibit metal sintering, but also promote the catalytic performance of propane dehydrogenation, phenylacetylene semi hydrogenation and hydrogen evolution reaction (HER). Metal-N species [27,30,40,[44][45][46][47]128] Regulate acid site [28] Change reduction state [35,42] Improve hydrophilicity [28] Increase alkalinity of site [12,23,27,34,45,130] Interaction between metal and N [26,30] Increase the adsorption of substrate [33] Improve metal dispersion [24,25,27,29,31,32,35,36,40,44,45,48] Pyrolysis Similar to N, S doping, B atoms can also be easily incorporated into the carbon skeleton due to its comparable atomic size with carbon. [57,[62][63][64][65][66][67][68] The role of B is basically to form a strong interaction with the metal, thus affecting the electronic and geometric state of the metal (Table 2).…”

Section: Metal Catalysts Anchored By S B and Pmentioning

confidence: 99%

“…In addition to structural factors and internal active species, the heteroatoms content in the carbon overlayer will also affect the catalytic performance of the catalyst. [130,134,136,147,148] For example, Liu and co-workers designed a double-shell structured carbon catalyst (Ru-DSC) by hard template method and pyrolysis in ammonia atmosphere. [130] Ru-DSC had the characteristics of selectively anchoring Ru NPs on inner carbon shell.…”

Section: Heteroatom Contentmentioning

confidence: 99%

“…[130,134,136,147,148] For example, Liu and co-workers designed a double-shell structured carbon catalyst (Ru-DSC) by hard template method and pyrolysis in ammonia atmosphere. [130] Ru-DSC had the characteristics of selectively anchoring Ru NPs on inner carbon shell. After treatment in ammonia atmosphere (Ru-DSC-RF-NH 3 ), the pyridinic N content increased from 7.4 (Ru-DSC-RF) to 16.1 mg g cat À 1 (Figure 13a,b).…”

Section: Heteroatom Contentmentioning

confidence: 99%

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Advanced Carbon‐Based Nanocatalysts and their Application in Catalytic Conversion of Renewable Platform Molecules

et al. 2022

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The transformation of renewable platform molecules to produce value‐added fuels and fine‐chemicals is a promising strategy to sustainably meet future demands. Owing to their finely modified electronic and geometric properties, carbon‐based nanocatalysts have shown great capability to regulate their catalytic activity and stability. Their well‐defined and uniform structures also provide both the opportunity to explore intrinsic reaction mechanisms and the site‐requirement for valorization of renewable platform molecules to advanced fuels and chemicals. This Review highlights the progress achieved in carbon‐based nanocatalysts, mainly by using effective regulation approaches such as heteroatom anchoring, bimetallic synergistic effects, and carbon encapsulation to enhance catalyst performance and stability, and their applications in renewable platform molecule transformations. The foundation for understanding the structure‐performance relationship of carbon‐based catalysts has been established by investigating the effect of these regulation methods on catalyst performance. Finally, the opportunities, challenges and potential applications of carbon‐based nanocatalysts are discussed.

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Section: Metal Catalyst Anchored By Heteroatomsmentioning

confidence: 99%

Section: Metal Catalysts Anchored By S B and Pmentioning

confidence: 99%

Section: Heteroatom Contentmentioning

confidence: 99%

Section: Heteroatom Contentmentioning

confidence: 99%

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Advanced Carbon‐Based Nanocatalysts and their Application in Catalytic Conversion of Renewable Platform Molecules

et al. 2022

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“…For example, Zhang et al 180 fabricated atomically precise nitrogen-doped chevron-type graphene nanoribbons by using the on-surface synthesis technique combined with the nitrogen substitution of the precursors. Li et al 30 designed a unique double-shell hollow carbon sphere (DSC) nanoreactor in which ultrafine Ru NPs were encapsulated in a hollow sandwich while precisely modulating pyridine N species by thermal annealing treatment under NH 3 flow on the outer carbon shell only (Figure 33). By precisely identifying the active nitrogen species, it is demonstrated that nitrogen dopants not only improve the catalytic performance of metal NPs but also have an interaction between the nitrogen species and the reactants.…”

Section: ■ Challenges and Perspectivesmentioning

confidence: 99%

Atom Doping Engineering of Metal/Carbon Catalysts for Biomass Hydrodeoxygenation

Yan

Wang

2021

ACS Sustainable Chem. Eng.

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Developing novel and efficient hydrodeoxygenation (HDO) catalysts plays a crucial role on biomass utilization from green and sustainable points of view. In the past, carbon materials were recognized as ideal catalyst carriers due to their fascinating properties including tunable surface structure and excellent chemical and thermal stability. Recently, the newly emerging metal/heteroatom-doped carbon catalysts have arguably experienced tremendous advances and gained widespread interest in view of the fact that heteroatom doping can further tailor the properties of carbon and introduce various metal–carrier interactions, resulting in superior HDO catalyst performance compared to pristine metal/carbon catalysts. In this perspective, we focus on the synthesis strategies for metal/heteroatom-doped carbon catalysts, the property effects of heteroatom doping, and catalytic applications through these fascinating catalysts in biomass HDO. Notably, we try to elucidate the doping effects through a summary of the mechanisms, thereby providing guidance for the rational design of advanced HDO catalysts for biomass catalysis.

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Pyridinic Nitrogen Sites Dominated Coordinative Engineering of Subnanometric Pd Clusters for Efficient Alkynes’ Semihydrogenation

et al. 2023

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Among them, one of the most important but challenging reactions is the alkynes' semihydrogenation to corresponding alkenes because of their poor alkene selectivity due to excessive hydrogenation and desorption barriers of alkenes, especially when the conversion is high. [7][8][9][10] The current problem-solving technique mainly relies on the development of diverse supported metal catalysts, [11][12][13][14] while the precondition is to exploit available support material that can stabilize and promote the active metal sites to own outstanding catalytic activity and selectivity for the semihydrogenation of alkynes.In this respect, nitrogen-doped carbons, as a type of promising support materials, have attracted tremendous attention due to their unique electron effects, tailorable surface characteristics, and excellent chemical and thermal stability. [15][16][17][18][19][20][21][22] In the regime of strong metal-support interactions, there are electron interactions in the form of charge redistribution and structural interactions in the form of mass redistribution between nitrogen-doped carbon and the anchored active metals. [23][24][25] Consequently, accurately adjusting the composition and spatial structure of nitrogen-doped carbon is a key point. High nitrogen contents can effectively limit the size of the metal, and more importantly, abundant coordination sites formed with metal can greatly lower the reaction energy barrier, resulting in high catalytic activity. And the electron effect generated by the nitrogen species in the supports can alter the electron density of the active metal sites, [26][27][28] which favors desorption of the monoene to obtain high catalytic selectivity. Following these principles, plentiful nitrogen-doped carbon-supported metals have been proven to be appealing catalysts. However, due to the proximity of nitrogen dopants' generation energy, the incorporation of nitrogen atoms into the carbon skeleton leads to the simultaneous doping of various nitrogen configurations including pyridinic N, pyrrolic N, graphitic N, and oxidized N. [29][30][31] Under this circumstance, most of the previous works simply manifest that active metal centers (M) are coordinated with nitrogen atoms (N) embedded in the matrix of carbon to form M-N x as active sites, [32][33][34] but it is still controversial for researchers to sufficiently understand which nitrogen configuration can dominant strong metal-support interactions to Supported metal catalysts have played an important role in optimizing selective semihydrogenation of alkynes for fine chemicals. There into, nitrogendoped carbons, as a type of promising support materials, have attracted extensive attentions. However, due to the general phenomenon of random doping for nitrogen species in the support, it is still atremendous challenge to finely identify which nitrogen configuration dominates the catalytic property of alkynes' semihydrogenation. Herein, it is reported that uniform mesoporous N-doped carbon spheres derived from mesoporous polypyrrole spheres ...

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Atomic Pyridinic Nitrogen Sites Promoting Levulinic Acid Hydrogenations over Double‐Shelled Hollow Ru/C Nanoreactors

Cited by 30 publications

References 42 publications

Advanced Carbon‐Based Nanocatalysts and their Application in Catalytic Conversion of Renewable Platform Molecules

Advanced Carbon‐Based Nanocatalysts and their Application in Catalytic Conversion of Renewable Platform Molecules

Atom Doping Engineering of Metal/Carbon Catalysts for Biomass Hydrodeoxygenation

Pyridinic Nitrogen Sites Dominated Coordinative Engineering of Subnanometric Pd Clusters for Efficient Alkynes’ Semihydrogenation

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