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Hollow Hierarchical Pd/HNC Nanoreactor as a High-Performance Catalyst for CO2Hydrogenation to Formate
- Source :
- Energy & Fuels; 20240101, Issue: Preprints
- Publication Year :
- 2024
-
Abstract
- The catalytic CO2hydrogenation to formic acid/formate represents an attractive atom-economic reaction in pursuit of carbon neutrality. The metal/nitrogen-doped carbon (M/NC) nanomaterials have emerged as favorable catalysts for CO2hydrogenation, yet the rational design of novel M/NC catalysts remains a significant challenge. In this study, we report a facile melamine (MA)-assisted co-pyrolyzed route for constructing a Pd-embedded hierarchical nitrogen-doped carbon (Pd/HNC) nanoreactor derived from Pd@ZIF-8/MA precursors. Transmission electron microscopy (TEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), energy-dispersive X-ray spectroscopy (EDX), and N2physisorption reveal that the Pd/HNC nanoreactor possesses a three-dimensional hollow and hierarchical porous nanoarchitecture, making it a promising high-performance heterogeneous catalyst for CO2hydrogenation. The Pd/HNC catalyst exhibits enhanced performance, achieving nearly 1.5-fold higher activity compared to the Pd/NC catalyst evolved from Pd@ZIF-8 precursors. Detailed investigations into various reaction parameters further highlight the exceptional activity of the Pd/HNC catalyst, achieving an impressive turnover number (TON) of 242 under the optimized conditions. Elemental analysis and CO2temperature-programmed desorption (CO2-TPD) unveil that the incorporation of melamine results in a higher nitrogen-doped level and enhanced CO2adsorption capacity for the Pd/HNC catalyst, thus reducing the activation energy barrier of CO2hydrogenation. Furthermore, the Pd/HNC catalyst demonstrates good reusability and stability upon multiple successive catalytic cycles. A plausible reaction pathway for CO2hydrogenation to formate over the Pd/HNC catalyst is proposed. This work presents an effective strategy for the fabrication of metal–organic frameworks (MOFs)-derived hollow hierarchical nanoreactors for various catalytic applications.
Details
- Language :
- English
- ISSN :
- 08870624 and 15205029
- Issue :
- Preprints
- Database :
- Supplemental Index
- Journal :
- Energy & Fuels
- Publication Type :
- Periodical
- Accession number :
- ejs65302354
- Full Text :
- https://doi.org/10.1021/acs.energyfuels.3c05193