利用理論計算探討金屬團簇還原二氧化碳的催化反應

Abstract

二氧化碳（CO₂）還原反應在減少溫室氣體排放和生產可再生能源方面具有重要意義，由於CO₂分子本身的高穩定性，使其還原過程具有挑戰性。本研究利用理論計算方法，探討了金屬團簇在CO₂還原反應中的催化性能，選擇了幾種具有潛在催化能力的金屬團簇，如鈀（Pd）、和鈷（Co）等金屬，並對其結構和電子性質進行了密度泛函理論（DFT）計算，比較不同團簇與CO₂分子的吸附能及反應路徑，發現這些團簇在特定條件下能夠有效地活化CO₂分子。接著，研究了CO₂在這些金屬團簇表面的還原反應機理，並計算了各步驟的吸附能，結果顯示，Pd和Co團簇在還原CO₂的過程中都具有較高的催化活性，研究結果表明，適當的表面修飾和反應條件可以進一步提升金屬團簇的催化活性和選擇性。總結來說，本研究通過理論計算證明了金屬團簇在CO₂還原反應中的潛在應用價值，為設計高效、選擇性的CO₂還原催化劑提供了重要的理論依據。The reduction of carbon dioxide (CO₂) is of significant importance for reducing greenhouse gas emissions and producing renewable energy. However, the high stability of CO₂ molecules makes the reduction process challenging. This study utilizes theoretical calculations to investigate the catalytic performance of metal clusters in the CO₂ reduction reaction. We selected several metal clusters with potential catalytic abilities, such as palladium (Pd) and cobalt (Co), and conducted density functional theory (DFT) calculations on their structures and electronic properties. By comparing the adsorption energies and reaction pathways of different clusters with CO₂ molecules, we found that these clusters can effectively activate CO₂ molecules under specific conditions. Subsequently, we studied the reduction reaction mechanism of CO₂ on the surfaces of these metal clusters and calculated the adsorption energies of each step. The results show that both Pd and Co clusters exhibit high catalytic activity in the reduction of CO₂. The study indicates that appropriate surface modifications and reaction conditions can further enhance the catalytic activity and selectivity of metal clusters.In summary, this study demonstrates the potential application value of metal clusters in the CO₂ reduction reaction through theoretical calculations, providing important theoretical support for designing efficient and selective CO₂ reduction catalysts.