Structure-controlled graphene-encapsulated nickel nanoparticle with tailored work function to steer chemoselective hydrogenation of nitroarenes

He, Wei; Jiang, Mengge; Yu, Jiaxin; Yan, Wei; Zhang, Xin; Jiang, Ruikun; Zhao, Hongyuan; Fang, Feng; Zhang, Q.F.; Lu, Chunshan; Li, Xinyan

doi:10.1016/j.mtchem.2023.101458

Cited by 3 publications

(2 citation statements)

References 62 publications

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“…Additionally, the absorption characteristic peak within the range of 700−1050 cm −1 were associated with the stretching vibrations of the benzene ring. 42 Compared with the spectrum of pure TPA, in the spectrum of Fe-OCPs-2, the stretching vibration peak related to the C = O bond belonging to the carboxyl group did not appear, and the symmetric (1560 cm −1 ) and asymmetric (1400 cm −1 ) vibration peaks associated with the −COO − group showed significant red shifts, indicating that the carboxyl group of the organic ligand was deprotonated and coordinated with Fe 3+ , 42,43 which was beneficial to the formation of Fe-OCPs-2. As illustrated in Figure 1c, the nitrogen sorption isotherm of Fe-OCPs-2 exhibited a type-IV isotherm, indicating that the material had a mesoporous structure and a specific surface area of 96.3 m 2 /g with a pore volume of 0.316 m 3 /g.…”

Section: Resultsmentioning

confidence: 99%

Iron-Based Catalysts with Oxygen Vacancies Obtained by Facile Pyrolysis for Selective Hydrogenation of Nitrobenzene

Yu,

Zhang,

Jiang

et al. 2024

ACS Appl. Mater. Interfaces

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The development of preparation strategies for iron-based catalysts with prominent catalytic activity, stability, and cost effectiveness is greatly significant for the field of catalytic hydrogenation but still remains challenging. Herein, a method for the preparation of iron-based catalysts by the simple pyrolysis of organometallic coordination polymers is described. The catalyst Fe@C-2 with sufficient oxygen vacancies obtained in specific coordination environment exhibited superior nitro hydrogenation performance, acid resistance, and reaction stability. Through solvent effect experiments, toxicity experiments, TPSR, and DFT calculations, it was determined that the superior activity of the catalyst was derived from the contribution of sufficient oxygen vacancies to hydrogen activation and the good adsorption ability of FeO on substrate molecules.

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Section: Resultsmentioning

confidence: 99%

Iron-Based Catalysts with Oxygen Vacancies Obtained by Facile Pyrolysis for Selective Hydrogenation of Nitrobenzene

Yu,

Zhang,

Jiang

et al. 2024

ACS Appl. Mater. Interfaces

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“…This process transforms the GLS into a novel active site. ,, Hence, current research predominantly centers on strategies to activate inert GLS and augment its catalytic activity. Currently, heteroatoms-doped carbon-encapsulated metal catalysts have exhibited exceptional catalytic performance in hydrogenation reactions attributed to the heightened electron density of state (DOS) of the inert GLS. − Nevertheless, the distinct bond lengths and atomic sizes between heteroatoms and graphitic carbon lead to spatial deformation of the GLS, causing defects that compromise its mechanical strength. , However, the oxygen-containing functional groups (OFGs)-modified GLS-encapsulated metal catalyst demonstrates the ability to enhance the catalytic activity while maintaining catalyst stability. The heightened chemical compatibility between oxygen and carbon atoms minimizes the likelihood of OFGs causing chemical bond breakage.…”

Section: Introductionmentioning

confidence: 99%

Aromatic Ethers Induced Electronic Structure Reconstruction on Encapsulated Nickel Catalysts for High-Performance Catalytic Hydrogenation

Yao,

Yin,

et al. 2024

ACS Appl. Mater. Interfaces

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Carbon-encapsulated metal (CEM) catalysts effectively address supported metal catalyst instability by protecting the active metal with a shell. However, mass transfer limitations lead to reduced activity for catalytic hydrogenation reaction over most CEM catalysts. Herein, we introduce a dopant strategy aimed at incorporating nickel metal within graphene-like shells (GLS) featuring oxygen-containing functional groups (OFGs). The core of this strategy involves precise control of GLS modification and the demonstrated pivotal influence of aromatic ether linkages (� C−O−C) in GLS for significant enhancement of catalytic performance. The introduction of �C−O−C into GLS with stability was beneficial to improve the work function of the catalyst and promoted electron transmission from Ni metal core to GLS, further elevating the catalytic activity, based on the Mott−Schottky effect. In addition, the experimental characterization and density functional theory (DFT) calculations showcased that the �C−O−C reconstructed the electronic state of GLS, imparting it highly specific for the adsorption of hydrogen and para-chloronitrobenzene (p-CNB) to obtain para-chloroaniline (p-CAN) with high selectivity. This work manifested a feasible direction for the precise modulation and design of the OFGs in CEM catalysts to achieve highly efficient catalytic hydrogenation.

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Strengthened Delocalized Electronic Effect in Nano-Nickel@Carbon with High Pyrrolic Nitrogen for Selective Hydrogenation of Substituted Nitrobenzene Hydrogenation

Yao,

Yin,

et al. 2024

ACS Catal.

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Carbon-encapsulated metal (CEM) catalysts reconfigure the active site of the catalytic reaction by shifting from the conventional metal to the surface of the carbon material. Carbonencapsulated structure has attracted wide attention in the fields of electrochemistry, thermal catalysis and photocatalysis. Herein, a nitrogen-doped carbon-encapsulated nickel catalyst was synthesized via hydrothermal synthesis, with pyrrolic N (N Pyr ) content accounting for 48.4% of the total nitrogen species. Experiments and density functional theory calculations reveal that the fivemembered pyrrole ring shares six π electrons, and its electron cloud density on the carbon surface surpasses that of benzene or pyridine ring, promoting extensive electronic interaction between N Pyr C and nickel. The interaction also extends beyond the vicinity of the doping sites and permeates throughout the entire carbon shell, thereby augmenting a greater number of potential active sites on the NC layer. This strengthened delocalized electronic effect imparts specificity in the adsorption and dissociation processes of hydrogen and p-chloronitrobenzene, leading to enhanced catalytic performance in the hydrogenation production of p-chloroaniline. The precise preparation of N Pyr -doped CEM catalysts demonstrates its huge potential for industrial applications.

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Structure-controlled graphene-encapsulated nickel nanoparticle with tailored work function to steer chemoselective hydrogenation of nitroarenes

Cited by 3 publications

References 62 publications

Iron-Based Catalysts with Oxygen Vacancies Obtained by Facile Pyrolysis for Selective Hydrogenation of Nitrobenzene

Iron-Based Catalysts with Oxygen Vacancies Obtained by Facile Pyrolysis for Selective Hydrogenation of Nitrobenzene

Aromatic Ethers Induced Electronic Structure Reconstruction on Encapsulated Nickel Catalysts for High-Performance Catalytic Hydrogenation

Strengthened Delocalized Electronic Effect in Nano-Nickel@Carbon with High Pyrrolic Nitrogen for Selective Hydrogenation of Substituted Nitrobenzene Hydrogenation

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