Dataset Information

Modulating the strong metal-support interaction of single-atom catalysts via vicinal structure decoration.

ABSTRACT: Metal-support interaction predominately determines the electronic structure of metal atoms in single-atom catalysts (SACs), largely affecting their catalytic performance. However, directly tuning the metal-support interaction in oxide supported SACs remains challenging. Here, we report a new strategy to subtly regulate the strong covalent metal-support interaction (CMSI) of Pt/CoFe₂O₄ SACs by a simple water soaking treatment. Detailed studies reveal that the CMSI is weakened by the bonding of H⁺, generated from water dissociation, onto the interface of Pt-O-Fe, resulting in reduced charge transfer from metal to support and leading to an increase of C-H bond activation in CH₄ combustion by more than 50 folds. This strategy is general and can be extended to other CMSI-existed metal-supported catalysts, providing a powerful tool to modulating the catalytic performance of SACs.

SUBMITTER: Yang J

PROVIDER: S-EPMC9307766 | biostudies-literature | 2022 Jul

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

Modulating the strong metal-support interaction of single-atom catalysts via vicinal structure decoration.

Yang Jingyi J Huang Yike Y Qi Haifeng H Zeng Chaobin C Jiang Qike Q Cui Yitao Y Su Yang Y Du Xiaorui X Pan Xiaoli X Liu Xiaoyan X Li Weizhen W Qiao Botao B Wang Aiqin A Zhang Tao T

Nature communications 20220722 1

Metal-support interaction predominately determines the electronic structure of metal atoms in single-atom catalysts (SACs), largely affecting their catalytic performance. However, directly tuning the metal-support interaction in oxide supported SACs remains challenging. Here, we report a new strategy to subtly regulate the strong covalent metal-support interaction (CMSI) of Pt/CoFe<sub>2</sub>O<sub>4</sub> SACs by a simple water soaking treatment. Detailed studies reveal that the CMSI is weakene ...[more]

PMID: 35869061

Similar Datasets

Project description:Biodiesel is of high interest due to increased demand for energy with the concern regarding more sustainable production processes. However, an inevitable by-product is glycerol. Hence, the conversion of this by-product to higher-value chemicals, especially 1,3-propanediol (1,3-PDO) via glycerol hydrogenolysis reaction, is one of the most effective pathways towards a profitable process. In general, this process is catalyzed by a highly active Pt-based catalyst supported on γ-Al2O3. However, its low 1,3-PDO selectivity and stability due to surface deactivation of such catalysts remained. This led to the surface modification by WOx to improve both the selectivity by means of the increased Brønsted acidity and the stability in terms of Pt leaching-resistance. Hence, we applied experimental and density functional theory (DFT)-based techniques to study the fundamentals of how WOx modified the catalytic performance in the Pt/γ-Al2O3 catalyst and provided design guidelines. The effects of WOx promoter on improved activity were due to the shifting of the total density of states towards the antibonding region evident by the total density of states (TDOS) profile. On the improved 1,3-PDO selectivity, the main reason was the increasing number of Brønsted acid sites due to the added WOx promoter. Interestingly, the stability improvement was due to the strong metal-support interaction (SMSI) that occurred in the catalyst, like typical high leaching-resistant catalysts. Also, the observed strong metal-support-promoter interaction (SMSPI) is an additional effect preventing leaching. The SMSPI stemmed from additional bonding between the WOx species and the Pt active site, which significantly strengthened Pt adsorption to support and a high electron transfer from both Pt and Al2O3 to WOx promoter. This suggested that the promising promoter for our reaction performed in the liquid phase would improve the stability if SMSI occurred, where the special case of the WOx promoter would even highly improve the stability through SMSPI. Nevertheless, various promoters that can promote SMSPI need investigations.

Dataset Information

Modulating the strong metal-support interaction of single-atom catalysts via vicinal structure decoration.

Publications

Modulating the strong metal-support interaction of single-atom catalysts via vicinal structure decoration.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets