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

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.

Medienart:

E-Artikel

Erscheinungsjahr:

2024

Erschienen:

2024

Enthalten in:

Zur Gesamtaufnahme - volume:16

Enthalten in:

ACS applied materials & interfaces - 16(2024), 12 vom: 27. März, Seite 14680-14693

Sprache:

Englisch

Beteiligte Personen:

Yao, Yongyue [VerfasserIn]
Yin, Chunyu [VerfasserIn]
Ma, Chaofan [VerfasserIn]
Li, Yanni [VerfasserIn]
Wang, Yu [VerfasserIn]
Jiang, Ruikun [VerfasserIn]
He, Wei [VerfasserIn]
Xiang, Zhenli [VerfasserIn]
Liu, Yi [VerfasserIn]
Li, Xiaonian [VerfasserIn]
Lu, Chunshan [VerfasserIn]

Links:

Volltext

Themen:

Aromatic ether
Catalytic hydrogenation
Graphene-like shells
Journal Article
Oxygen-containing functional groups
Surface modification

Anmerkungen:

Date Revised 28.03.2024

published: Print-Electronic

Citation Status PubMed-not-MEDLINE

doi:

10.1021/acsami.3c16381

funding:

Förderinstitution / Projekttitel:

PPN (Katalog-ID):

NLM369872770