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利用多种从头计算方法对PdO0,±1,PdH0,±1以及PdOH的结构和电子性质进行了理论研究.优化了PdO分子两个能量相近的态(3Π和3Σ-),结果表明PdO的3Π态较3Σ-态更为稳定,在单双激发耦合簇理论(CCSD)水平下3Σ-态的总能量比3Π态的高出0.286eV.在结构优化的基础上计算了PdO以及PdH的绝热电离能(AIE)和电子亲和能(AEA),计算结果与实验值符合得很好.PdOH的基态为Cs对称性的角型结构Pd—OH(2A′态),另外还优化得到两个2A″态的亚稳结构,分别对应于Pd—OH和O—Pd—H,CCSD水平下两个亚稳态的总能量较基态分别高0.405和2.284eV,优化得到了连接这两个2A″态的过渡态,并计算了相应的反应能垒.
The structure and electronic properties of PdO0, ± 1, PdH0, ± 1 and PdOH have been theoretically studied by a variety of ab initio methods. Two states of similar energy (3Π and 3Σ-) of PdO molecule are optimized. The results show that PdO 3Π State is more stable than 3Σ-state, and the total energy of 3Σ-state is 0.286eV higher than that of 3Π state at the single-double excited coupled cluster theory (CCSD). Based on the structural optimization, the adiabatic ionization of PdO and PdH (AIE) and electron affinity (AEA), the calculated results are in good agreement with the experimental data. The ground state of PdOH is Pd-OH (2A ’state) with Cs symmetry. In addition, State metastable structures corresponding to Pd-OH and O-Pd-H, respectively. The total energy of the two metastable states at the CCSD level is 0.405 and 2.284eV higher than the ground state respectively, and the two 2A " The transition states are calculated and the corresponding reaction barriers are calculated.