RuH+與NH3及H2O等分子在氣相中反應以產生氫氣之理論計算與研究

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题名:	RuH+與NH3及H2O等分子在氣相中反應以產生氫氣之理論計算與研究 Density Functional Theory Studies of Reaction Mechanisms and Kinetics of RuH+ with NH3 and H2O
作者:	姚柏廷
贡献者:	化學系應用化學碩士班
关键词:	釕 Ru
日期:	2017
上传时间:	2017-10-17 10:51:43 (UTC+8)
摘要:	本論文係報告使用密度泛函理論(density functional theory)來做計算，我們使用B3LYP/6-311++G(3df,2p)做結構最佳化與能量之計算，若含有Ru金屬的結構則再加入SDD basis set進行計算。我們探討週期表第二列過渡金屬的氫化物RuH+與NH3和H2O的氣相反應，研究產生氫氣的各種可能反應機制，並繪製反應位能曲線圖(Potrntial Energy Surface)。本實驗分成以下兩個部分進行研究:(1) [MH+] (M=Ru) + NH3的反應機構研究探討，以及(2) [MH+] (M=Ru) + H2O的反應機構研究探討。其計算結果顯示，在過度金屬離子上加了一個hydrogen ligand的反應物 [MH+] (M=Ru)會先和NH3、H2O等分子形成各種複合物(Complexes)，並經由各自的過渡狀態(Transition states)，使NH3、H2O的N-H、O-H鍵進行斷裂，最終再和金屬上的H結合產生氫氣。 The reaction mechanisms of the RuH+ with the NH3 and H2O molecules have been investigated by the density functional theory in conjunction with B3LYP/6-311++G(3df,2p) method. The species involved Ru metal will be optimized by additional SDD basis set in the whole system. Pertinent aspects of the profiles of potential-energy surfaces (PES) calculated at the level B3LYP/6-311++G(3df,2p) are shown herein. Our calculated results indicate that the favorable pathways for the formation of specific isomers of two HRu+-NH3 and HRu+-H2O complexes. Formations of RuNH2+ + H2 (P2) and RuOH+ + H2 (P3) are also favorable, although these two pathways involve little activation energy. These results are recommended for combustion modeling applications. At elevated temperatures, these resulted hydrogen atoms could be desorbed by further consecutive recombination to generate the final products of hydrogen gas. Our findings provide atomistic-level insight into the novel pathway for metal-assisted synthesis of new chemical energy source.
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