Facile synthesis of N-doped graphene encapsulated Ni@N/C catalyst and its catalysis for highly selective semi-hydrogenation of alkynes

Liu, Jianguo; Sun, Jiangmin; Singh, Thishana; Lin, Shanshan; Ma, Longlong

doi:10.1016/j.gce.2022.01.003

Cited by 7 publications

(7 citation statements)

References 51 publications

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“…The high-resolution Ni 2p spectra (Figure b) for the three catalysts show two major peaks centered at 853.3 and 871.1 eV, which could be ascribed to the Ni 2p 3/2 and Ni 2p 1/2 orbitals of zero-valence Ni in the metallic state. Two weak peaks located at 855.2 and 873.2 eV could be assignable to the Ni 2p 3/2 and Ni 2p 1/2 orbitals of Ni 2+ species accompanied by two shake-up satellite peaks at around 860.2 and 880.5 eV, suggesting the inevitable partial oxidation of surface metallic Ni NPs when exposed to the air. − Of note, the Ni 2p peak position for Ni@NC-800 and Ni@NC-900 has a slightly negative shift relative to that of Ni@NC-700, and the corresponding binding energy of N 1s slightly shifts toward a higher value compared with Ni@NC-700. This finding suggests an interfacial electron transfer from N-doped carbon layers to the Ni NPs because of the lone-pair electrons of N in the carbon layers. , In addition, XPS analysis for the Ni contents on the catalyst surface reveals that the catalyst Ni@NC-900 has the lowest value (Table S1), which is opposite to the value determined by ICP–OES, further suggesting the formation of a core–shell structure in the catalysts Ni@NC-800 and Ni@NC-900.…”

Section: Resultsmentioning

confidence: 99%

Electronic and Steric Modification of Ni Nanoparticle Surface via N-Doped Carbon Layers Enables Highly Selective Semihydrogenation of Alkynes

Wang,

Song,

et al. 2023

ACS Catal.

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The selective semihydrogenation of alkynes to alkenes is of great importance in the chemical industry. However, it remains a big challenge to achieve high catalytic activity and selectivity simultaneously, which calls for developing efficient and selective catalysts. In this work, we develop a spatially confined Ni catalyst with Ni nanoparticles (NPs) as the core and N-doped carbon layers as the shell. The core–shell structure not only effectively protects Ni NPs from aggregation to substantially boost the stability but also creates the steric and electronic effects for Ni NP surface via an intimate interfacial interaction with N-doped carbon layers. As a result, the resultant catalyst exhibited both high activity and selectivity for semihydrogenation of alkynes to alkenes. A broad set of terminal and internal alkynes were efficiently reduced to their respective alkenes in a highly selective manner, and various functional groups were well tolerated. Remarkably, these spatially confined Ni NPs are applicable for scale-up synthesis, demonstrate high stability, and could be readily separated for successive reuses without obvious decay in either activity or selectivity. Comprehensive characterizations and control experiments jointly demonstrate the key role of N-doped carbon layers around Ni NPs for improving the catalytic activity, selectivity, and stability.

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Section: Resultsmentioning

confidence: 99%

Electronic and Steric Modification of Ni Nanoparticle Surface via N-Doped Carbon Layers Enables Highly Selective Semihydrogenation of Alkynes

Wang,

Song,

et al. 2023

ACS Catal.

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“…Catalytic activity arises due to strong encapsulation of nickel metal with the graphitic layer. 41 To bypass the use of harsh reaction conditions and overreduction of alkyne to alkane, Turculet and coworkers in 2022 demonstrated the synthesis of the nickel pincer complex (iPr-PSiP Ind )NiH for selective synthesis to (E)-stilbene (1 mol % Ni, 1 atm H 2 , 4 h at 25 1C) (Scheme 31). Broad scope with no overhydrogenation product is the key to success.…”

Section: Nickel-based Catalystmentioning

confidence: 99%

Recent advances in the selective semi-hydrogenation of alkyne to (E)-olefins

Sk,

Haldar,

Bera

et al. 2024

Chem. Commun.

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“…The substrates with electron-withdrawing Cl groups gave higher selectivity of the desired semihydrogenated product than the substrates with electron-donating OCH 3 and NH 2 groups due to delocalization of the electron negativities of the aromatic ring. 49,50 The strategy encourages the wider pursuit of solar-driven photothermal catalyst systems for selective hydrogenation reactions.…”

Section: Catalysis Studymentioning

confidence: 99%

Highly Stable Cesium Molybdenum Chloride Perovskite Nanocrystals for Photothermal Semihydrogenation Applications

Kong,

Jiang,

Wang

et al. 2024

ACS Appl. Mater. Interfaces

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Metal halide perovskite materials with excellent carrier transport properties have been regarded as a new class of catalysts with great application potential. However, their development is hampered by their instability in polar solvents and high temperatures. Herein, we report a solution-processed Cs 2 MoCl 6 perovskite nanocrystals (NCs) capped with the Mo 6+ , showing high thermostability in polar solvents. Furthermore, the Pd single atoms (PdSA) can be anchored on the surface of Cs 2 MoCl 6 NCs through the unique coordination structure of Pd−Cl sites, which exhibit excellent semihydrogenation of different alkyne derivatives with high selectivity at full conversion at room temperature. Moreover, the activity could be improved greatly under Xe lamp irradiation. Detailed experimental characterization and DFT calculations indicate the improved activity under light illumination is due to the synergistic effect of photo-to-heat conversion and photoinduced electron transfer from Cs 2 MoCl 6 to PdSA, which facilitates the activation of the C�C group. This work not only provides a new catalyst for high selective semihydrogenation of alkyne derivatives but also opens a new avenue for metal halides as photothermal catalysts.

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Facile synthesis of N-doped graphene encapsulated Ni@N/C catalyst and its catalysis for highly selective semi-hydrogenation of alkynes

Cited by 7 publications

References 51 publications

Electronic and Steric Modification of Ni Nanoparticle Surface via N-Doped Carbon Layers Enables Highly Selective Semihydrogenation of Alkynes

Electronic and Steric Modification of Ni Nanoparticle Surface via N-Doped Carbon Layers Enables Highly Selective Semihydrogenation of Alkynes

Recent advances in the selective semi-hydrogenation of alkyne to (E)-olefins

Highly Stable Cesium Molybdenum Chloride Perovskite Nanocrystals for Photothermal Semihydrogenation Applications

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