本文藉由密度泛函理論(DFT)探討在釕-鉑/含硼石墨稀表面上的二氧化碳捕捉與水氣轉移反應。在二氧化碳分解與水氣轉移反應的反應機制中，各個最穩定吸附結構以及過渡狀態皆由理論計算所確定。由計算結果得知，摻雜在石墨稀中的硼具有抑制釕-鉑合金在表面形成叢集的現象，並且相較於純金屬鉑(111)表面，釕-鉑/含硼石墨稀有較低的製造成本及出色的觸媒性質。二氧化碳吸附在釕-鉑/含硼石墨稀十分穩定，吸附能為-0.76 eV，相較之下其吸附能高於分解反應能障(0.63 eV)，此結果顯示釕-鉑/含硼石墨稀擁有二氧化碳捕捉能力與活性，使得二氧化碳可以進一步分解。根據計算結果，在釕-鉑/含硼石墨稀表面上的一氧化碳可透過表面上氧原子進行氧化反應(redox mechanism)，與先形成羧基(COOH)進行羧基反應(carboxyl mechanism)或是形成甲酸基(formate)進行甲酸基反應(formate mechanism)，之後皆形成二氧化碳。最後實驗結果顯示氧化還原及羧基反應路徑的速率決定步驟皆為二氧化碳在表面上的脫附反應，其反應能障為0.64 eV，而甲酸基反應的速率決定步驟能障相對較高，為1.00 eV。

In this article, we have performed density functional theory (DFT) calculations to investigate CO2 capture and water-gas shift (WGS) reaction over the Ru-Pt/boron-doped graphene surface. The structures and energies of the most important minima and transition states corresponding to the CO2 decomposition and three mechanisms of WGS reaction pathways have been determined based on DFT calculation. From our calculated results, we found that one layer of Ru-Pt/boron-doped graphene nano-sheet, which caused by the substitutive boron defects in graphene model restraining the growth of the metal cluster, has lower the production costs and excellent catalyst compared with the pure Pt(111) surface. The adsorption energy of CO2 molecule on the Ru-Pt/boron-doped graphene surface is quite large, -0.76 eV, which is higher than the further decomposition barrier, 0.63 eV. It indicates that Ru-Pt/boron-doped graphene surface, due to the intrinsic high surface areas and polarity, is a good catalyst for CO2 capture and also has high activity for CO2 decomposition. Predicting from our results, three mechanisms of WGS reaction on Ru-Pt/boron-doped graphene surface, redox, carboxyl and formate mechanisms can happen. The rate-determining steps for both redox and carboxyl mechanisms are CO2 desorption, and the reaction barrier of this step is 0.69 eV on Ru-Pt/boron-doped graphene surface. However, the rate-determining steps for formate mechanisms is relatively higher, 1.00 eV, compare with the other mechanisms.

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