Atomic ruthenium stabilized on vacancy-rich boron nitride for selective hydrogenation of esters

Huang, Lele; Liu, Xu-Feng; Zou, Jinglin; Duan, Xinping; Chen, Zuo‐Chang; Zhou, Zhe; Ye, Linmin; Liang, Xiaoping; Xie, Su‐Yuan; Yuan, Youzhu

doi:10.1016/j.jcat.2022.01.004

Cited by 20 publications

(13 citation statements)

References 53 publications

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“…In h-BN-derived nanocatalysts, boron or nitrogen sites with unsaturated coordination that form at the edge position or within the defects could directly act as the active sites to promote the reaction or provide the surrounding environment to tune the electronic properties of the active metal center (e.g., supported metal nanoparticles (NPs) or single atoms (SAs)) toward enhanced catalytic activity. − Under either circumstance, the electronic and structural properties of h-BN play critical roles, which could be modulated by the number of 2D layers, defect types and ratios, crystallinity, surface functionalization, and heteroelemental doping. , Therefore, the development of facile and controllable construction and modification approaches is a prerequisite to accessing the precise tuning over the h-BN scaffolds, which will, in turn, become powerful platforms for generating heterogeneous catalysts with promising catalytic performance. In addition, a fundamental and systematic understanding of the correlation between specific structural and compositional parameters and the catalytic behavior variation, particularly the charge transfer and interfacial phenomena in h-BN-supported metal catalysts, will provide untapped opportunities in catalyst design and resolve challenging issues in catalysis by customizing the h-BN scaffolds.…”

Section: Introductionmentioning

confidence: 99%

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

et al. 2022

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Hexagonal boron nitrides (h-BNs) are attractive two-dimensional (2D) nanomaterials that consist of alternating B and N atoms and layered honeycomblike structures similar to graphene. They have exhibited unique properties and promising application potentials in the field of energy storage and transformation. Recent advances in utilizing h-BN as a metal-free catalyst in the oxidative dehydrogenation of propane have triggered broad interests in exploring h-BN in catalysis. However, h-BN-based materials as robust nanocatalysts in heterogeneous catalysis are still underexplored because of the limited methodologies capable of affording h-BN with controllable crystallinity, abundant porosity, high purity, and defect engineering, which played important roles in tuning their catalytic performance. In this Account, our recent progress in addressing the above issues will be highlighted, including the synthesis of high-quality h-BN-based nanomaterials via both bottom-up and top-down pathways and their catalytic utilization as metal-free catalysts or as supports to tune the interfacial electronic properties on the metal nanoparticles (NPs). First, we will focus on the large-scale fabrication of h-BN nanosheets (h-BNNSs) with high crystallinity, improved surface area, satisfactory purity, and tunable defects. h-BN derived from the traditional approaches using boron trioxide and urea as the starting materials generally contains carbon/oxygen impurities and has low crystallinity. Several new strategies were developed to address the issues. Using bulk h-BN as the precursor via gas exfoliation in liquid nitrogen, single-or few-layered h-BNNS with abundant defects could be generated. Amorphous h-BN precursors could be converted to h-BN nanosheets with high crystallinity assisted by a magnesium metallic flux via a successive dissolution/precipitation/crystallization procedure. The as-fabricated h-BNNS featured high crystallinity and purity as well as abundant porosity. An ionothermal metathesis procedure was developed using inorganic molten salts (NaNH 2 and NaBH 4 ) as the precursors. The h-BN scaffolds could be produced on a large scale with high yield, and the asafforded materials possessed high purity and crystallinity. Second, utilization of the as-prepared h-BN library as metal-free catalysts in dehydrogenation and hydrogenation reactions will be summarized, in which they exhibited enhanced catalytic activity over the counterparts from the previous synthesis method. Third, the interface modulation between metal NPs with the as-prepared defects' abundant h-BN support will be highlighted. The h-BN-based strong metal−support interaction (SMSI) nanocatalysts were constructed without involving reducible metal oxides via the ionothermal procedure we developed by deploying specific inorganic metal salts, acting as robust nanocatalysts in CO oxidation. Under conditions simulated for practical exhaust systems, promising catalytic efficiency together with high thermal stability and sintering resistance was achieved. Across all of these ...

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Section: Introductionmentioning

confidence: 99%

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

et al. 2022

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“…The EDS image of 5 wt % Ru/h-BN samples (Figure S1) showed the presence of Ru, B, and N in the samples . The EDS mapping in Figure c–e further demonstrated that Ru, B, and N elements were distributed evenly, indicating the high dispersion of Ru species on h-BN and Ru element with no pronounced clustering on the surface of BN nanoflakes …”

Section: Resultsmentioning

confidence: 89%

“…25 The EDS mapping in Figure 5c−e further demonstrated that Ru, B, and N elements were distributed evenly, indicating the high dispersion of Ru species on h-BN and Ru element with no pronounced clustering on the surface of BN nanoflakes. 26 It was noteworthy that the distribution of highlights in HAADF images was relatively uniform, as revealed by transmission electron microscopy and EDS. Ultrasonic-assisted deposition is a suitable method for preparing well-dispersed Ru-based catalysts.…”

Section: Catalyst Characterization 211 N 2 Physisorptionmentioning

confidence: 91%

Highly Dispersed Ru Nanoclusters Anchored on Hexagonal Boron Nitride for Efficient and Stable Hydrogenation of Aromatic Amines to Alicyclic Amines

Han

Wang

Cao

et al. 2023

Ind. Eng. Chem. Res.

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Saturated hydrogenation of aromatic amines is a crucial methodology for synthesizing alicyclic amines. The dispersion of Ru atoms occurred after chemical reduction treatment, which was constrained to B and N coordination, further promoting the Ru species’ uniform distribution through interaction with the B–N bond of boron nitride. Moreover, the Ru coordinated with h-BN and further formed the stable catalytic active center. By virtue of its excellent stability, the hydrogenation of MDA executed in the fixed-bed reactor could run for more than 200 h. However, the density functional theory showed that the hydrogenation rate of the second benzene ring was comparatively slower because of the strong intermediate adsorption during the conversion from 4,4′-diaminodiphenylmethane to 4,4′-diaminodicyclohexylmethane. Furthermore, Ru/h-BN exhibited excellent performance in the hydrogenation of other aromatic amines, resulting in corresponding alicyclic amines. Therefore, this research offers a stable and effective catalyst for the green hydrogenation of aromatic amines leading to the production of alicyclic amines.

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“…Huang et al synthesized Ru/d-BN catalysts through stirring, sonication, activity and transmutation processes. 191 Atomic Ru was embedded on the B- and n-vacant gits, leading to overall charge transfer from Ru to d-BN, resulting in the segmental oxidization of Ru d+ (3 ≤ δ ≤ 4) active species, indicating pronounced EMSIs. The interface between both the d-BN and Ru metal anchors Ru active sites enhances the catalytic activity and sintering performance of DMO hydrogenation flow for 100 h.…”

Section: Smsimentioning

confidence: 99%

Metal–support interactions for heterogeneous catalysis: mechanisms, characterization techniques and applications

Chen

Zhang

et al. 2023

J. Mater. Chem. A

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Atomic ruthenium stabilized on vacancy-rich boron nitride for selective hydrogenation of esters

Cited by 20 publications

References 53 publications

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

Highly Dispersed Ru Nanoclusters Anchored on Hexagonal Boron Nitride for Efficient and Stable Hydrogenation of Aromatic Amines to Alicyclic Amines

Metal–support interactions for heterogeneous catalysis: mechanisms, characterization techniques and applications

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