(702f) Investigation of Liquid Fuel Generation from Carbon Dioxide over Bimetallic Systems
AIChE Annual Meeting
2023
2023 AIChE Annual Meeting
Catalysis and Reaction Engineering Division
Reaction Path Analysis
Thursday, November 9, 2023 - 5:18pm to 5:36pm
According to previous work about long-chain hydrocarbons formation,1 the alloy system with palladium and gold presents excellent catalysis performance for C3-C5 products with CO2RR. We then designed a PdAu bimetallic catalyst (Figure 1a) as a study case and explored the mechanism of CO2RR-to-C3+ via a combination of machine learning, density functional theory (DFT) and microkinetic modeling.3 In particular, our results show that Cn-CH2 coupling is more energetically favorable than Cn-CO. This further confirmed our hypothesis that to generate C3+ fuels, the reaction mechanism is a Ficher-Tropsch-like synthesis which passes by the key intermediate CH2. The reaction energetics could be further promoted at the Pd-Au interfacial site as compared to the pure Pd or Au sites. For the future work, we will design a deep active learning algorithm to auto-generate and auto-select bimetallic interface sites for CO2RR to long-chain hydrocarbon fuel generation. This theoretical research provides an innovative reaction mechanism, i.e., CH2 insertion, for bimetallic system based CO2RR to long-chain hydrocarbons (C3+). This work would further integrate energy storage of renewable electricity with the grid, enable storage for intermittent power, and would advance goals of net-zero carbon fuels.