Abstract
Herein, we have achieved successful preparation of atomically dispersed catalytic systems, liquid metal Ptx/Ga catalysts, which eliminate the need for reduction processes. Notably, the 0.5 wt% Ptx/Ga catalyst exhibited exceptional stability in hydrogenation performance, achieving 100 % conversion of stearic acid with an impressive 98.7 % selectivity towards octadecane, especially with unprecedented stability over 19 recycling cycles. X-ray absorption spectra (XPS) and density functional theory (DFT) calculations unequivocally establish that isolated Pt atoms, benefitting from charge transfer from the Ga matrix, synergistically optimize Pt metal atom utilization, thereby efficaciously optimizing the d-band center and augmenting hydrogenation proficiency. Furthermore, isolated Pt configuration's weaker CO adsorption ability effectively mitigates concerns of catalyst poisoning and undesirable agglomeration, thereby engendering superior stability. The stronger adsorption with aldehyde and alcohol intermediates promotes the hydrogenation of stearic acid through hydrodehydration pathway, thereby ensuring a high carbon utilization economy. Overall, our work offers insight into the investigation of hydrogenation conversion of bio-derivatives over atomically dispersed catalytic systems.
| Original language | English |
|---|---|
| Article number | 124915 |
| Journal | Applied Catalysis B: Environment and Energy |
| Volume | 365 |
| Early online date | 11 Dec 2024 |
| DOIs | |
| Publication status | Published - 15 May 2025 |
Funding
The authors thank the financial support by National Natural Science Foundation of China (Grant No. 22378195) and Jiangsu Agriculture Science and Technology Innovation Fund (JASTIF), (CX(24)1009). Our computational work was performed on High-Performance Computer, ARCHIE-WeSt, at University of Strathclyde
Keywords
- Atomically dispersed liquid catalytic systems
- Ptx/Ga catalysts
- d-band center
- Intermediates adsorption and hydrogenation activity
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