物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2011年
5期
1095-1102
,共8页
赵高峰%向兵%沈学峰%孙建敏%白燕枝%王渊旭
趙高峰%嚮兵%瀋學峰%孫建敏%白燕枝%王淵旭
조고봉%향병%침학봉%손건민%백연지%왕연욱
密度泛函理论%氧化锆团簇%分解通道%成键规律
密度汎函理論%氧化鋯糰簇%分解通道%成鍵規律
밀도범함이론%양화고단족%분해통도%성건규률
Density functional theory%Zirconium oxide cluster%Fragmentation channel%Bonding regularity
利用密度泛函理论在广义梯度近似(GGA)和Perdew-Wang交换关联泛函条件下研究了小团簇ZrmOn(1≤m≤5,1≤n≤2m)的几何结构和稳定性.结果表明:所有团簇的最低能量结构可通过锆团簇的连续氧化获得,一般情况下O原子占据在Zr团簇的桥位.(ZrO2)3和(ZrO2)5团簇的基态结构符合配位数规则和成键规律.此外,讨论了氧化锆团簇的分解通道和分解能,值得指出的是在Zr原子数相同时ZrmO2m-1团簇(除了Zr4O7)存在最大的分解能.
利用密度汎函理論在廣義梯度近似(GGA)和Perdew-Wang交換關聯汎函條件下研究瞭小糰簇ZrmOn(1≤m≤5,1≤n≤2m)的幾何結構和穩定性.結果錶明:所有糰簇的最低能量結構可通過鋯糰簇的連續氧化穫得,一般情況下O原子佔據在Zr糰簇的橋位.(ZrO2)3和(ZrO2)5糰簇的基態結構符閤配位數規則和成鍵規律.此外,討論瞭氧化鋯糰簇的分解通道和分解能,值得指齣的是在Zr原子數相同時ZrmO2m-1糰簇(除瞭Zr4O7)存在最大的分解能.
이용밀도범함이론재엄의제도근사(GGA)화Perdew-Wang교환관련범함조건하연구료소단족ZrmOn(1≤m≤5,1≤n≤2m)적궤하결구화은정성.결과표명:소유단족적최저능량결구가통과고단족적련속양화획득,일반정황하O원자점거재Zr단족적교위.(ZrO2)3화(ZrO2)5단족적기태결구부합배위수규칙화성건규률.차외,토론료양화고단족적분해통도화분해능,치득지출적시재Zr원자수상동시ZrmO2m-1단족(제료Zr4O7)존재최대적분해능.
The geometric structures and stabilities of small ZrmOn (1≤m≤5, 1≤n≤2m) clusters were studied using density functional theory (DFT) calculations with the Perdew-Wang exchange correlation functional and the generalized gradient approximation (GGA). The lowest energy structures of all these clusters were obtained by the sequential oxidation of the small "core" zirconium clusters. In general, the O atoms prefer the bridge sites along the Zrm skeleton. The ground-state structures of the (ZrO2)3 and (ZrO2)5 clusters are consistent with coordination number rules and bonding regularity. The fragmentation channels and fragmentation energies of the small zirconium oxide clusters were discussed. We found that the ZrmO2m-1 clusters (not Including Zr4O7) had the largest fragmentation energy among the clusters with the same number of zirconium atoms.