过渡金属离子Ni~+与甲醇、乙醇团簇反应的质谱研究
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摘要
利用激光溅射-超声分子束技术在反射式飞行时间质谱仪上研究了气相条件下Ni等离子体和甲醇、乙醇分子团簇的反应。实验中,直接用激光溅射Ni靶时观察到Ni的五种同位素离子(58Ni+、60Ni+、61Ni+、62Ni+、64Ni+),在Ni等离子体和甲醇分子团簇的反应中观察到Ni+(CH3OH)n、Ni O+(CH3OH)n、Ni CH2+(CH3OH)n、H+(H2O)(CH3OH)n、四种团簇正离子,在Ni和乙醇分子团簇的反应中观察到Ni+(C2H5OH)n、Ni CH2+(C2H5OH)n、Ni C2H4+(C2H5OH)n、H+(H2O)(C2H5OH)n四种团簇正离子。重点研究了Ni和甲醇团簇反应的产物离子在不同的激光延时、激光能量、载气压力条件下对团簇产物种类和尺寸的影响及团簇产物的变化规律,并对团簇产物离子的形成机理进行了解释。
Using laser ablation-supersonic molecular beam technique on a reflective time of flight mass spectrometer to study the reaction of gas phase Ni plasma and methanol, ethanol molecule clusters. In the experiment, Five species of Ni isotope ions58Ni+,60Ni+,61Ni+,62Ni+,64Ni+are observed when the Ni target is directly sputtered by Laser. In the Experiment on Ni plasma and methanol molecule clusters, five kinds of positive ion clusters Ni+(CH3OH)n, Ni O+(CH3OH)n, Ni CH2+(CH3OH)n, H+(H2O)(CH3OH)nare observed. In the reaction of Ni plasma and ethanol molecule clusters, four species of positive ion clusters Ni+(C2H5OH)n, Ni CH2+(C2H5OH)n, Ni C2H4+(C2H5OH)n, H+(H2O)(C2H5OH)nare observed. The Focus is on the products of reaction of the ion clusters of Ni and methanol in different variation of the delay of laser, laser energy, Carrier gas pressure conditions on the type and size of the product cluster and the cluster impact product, the formation mechanism of cluster product ions are also explained.
Using laser ablation-supersonic molecular beam technique on a reflective time of flight mass spectrometer to study the reaction of gas phase Ni plasma and methanol, ethanol molecule clusters. In the experiment, Five species of Ni isotope ions58Ni+,60Ni+,61Ni+,62Ni+,64Ni+are observed when the Ni target is directly sputtered by Laser. In the Experiment on Ni plasma and methanol molecule clusters, five kinds of positive ion clusters Ni+(CH3OH)n, Ni O+(CH3OH)n, Ni CH2+(CH3OH)n, H+(H2O)(CH3OH)nare observed. In the reaction of Ni plasma and ethanol molecule clusters, four species of positive ion clusters Ni+(C2H5OH)n, Ni CH2+(C2H5OH)n, Ni C2H4+(C2H5OH)n, H+(H2O)(C2H5OH)nare observed. The Focus is on the products of reaction of the ion clusters of Ni and methanol in different variation of the delay of laser, laser energy, Carrier gas pressure conditions on the type and size of the product cluster and the cluster impact product, the formation mechanism of cluster product ions are also explained.
引文
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[15]牛冬梅,张树东,张先燚,李海洋.激光溅射Cu等离子体与气相C2H5OH团簇的反应[J].物理化学学报,2003,19(12):1114-1118.
[16]牛冬梅,张树东,张先燚,李海洋.激光溅射Ni等离子体与气相CH3OH团簇的反应[J].化学物理学报,2004,17(2):116-120.
[17]Zhang Fuji,Liu Hong.Spectroscopy and Spectral Analysis[J].2000,20:237.
[2]李业军,陆泽,席晓峰,严琪琪,汤秀章.激光与原子团簇相互作用实验系统的的建立[J].原子能科学技术,2007,41(1):101-103.
[3]王广厚.团簇物理的新进展(I)[J].物理学进展,1991,14(2):121-172.
[4]王广厚.团簇物理的新进展(II)[J].物理学进展,1998,18(1):1-22.
[5]刘永臻,梁峰,再帕尔·阿不力孜.离子——分子反应在质谱分析中的应用[J].质谱学报,2004,25(3):175-182.
[6]罗晓琳,牛冬梅,裴克梅,张树东,李海洋.激光溅射Cu等离子体与气相CH3CN团的反应[J].化学物理学报,2004,17(6):660-664.
[7]杭伟.小型反射式飞行时间质谱计的研制[D].厦门大学,1991.
[8]李海洋,白吉玲,戴东旭,等.呋喃分子在450nm的多光子电离碎片化动力学[J].化学物理学报,1993,6:510-515.
[9]刘宇清,俞学东,陆家和,等.新型小飞行时间质谱计的研究[J].真空科学与技术,1998,18(4):239-246.
[10]李连斌,王秀岩.氨和甲醇团簇中的质子转移反应[J].化学物理学报,2000,13:641.
[11]许明坤,张树东,孔祥和,等.氨与甲醇混合团簇的多光子电离质谱及从头算研究[J].原子与分子物理学报,2007,24(5):1049-1054.
[12]Lu W Y,Yang S H.Reactions of Alkaline Earth Metal Ions with Methanol Clusters[J].Phys Chem.,1998,102:825-840.
[13]Keya T,Kobayashi M,Shinohara H,Sato H.Reactions of ammonia clusters with metal ions as studied by the laser ablation—molecular beam method:observation of clustered complex ions M+(NH3)n(n=0-20)and fragment complex ions with multiple hydrogen elimination M+(NH)m(NH3)n(m=1,2)[J].Chem.Phys.Letts.,1991,186(4-5):431-435.
[14]Keya T,Horicon Y,Kobayashi M,Shinohara H,Sato H.Intensity gaps in M+(CH3OH)n as studied by laser ablation—molecular beam method[J].Chem.Phys Letts.,1992,200(5):435-439.
[15]牛冬梅,张树东,张先燚,李海洋.激光溅射Cu等离子体与气相C2H5OH团簇的反应[J].物理化学学报,2003,19(12):1114-1118.
[16]牛冬梅,张树东,张先燚,李海洋.激光溅射Ni等离子体与气相CH3OH团簇的反应[J].化学物理学报,2004,17(2):116-120.
[17]Zhang Fuji,Liu Hong.Spectroscopy and Spectral Analysis[J].2000,20:237.