激光溅射下四唑环的簇合行为
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摘要
为了解四唑环在激光作用下的分解和簇合行为,在高真空条件下,以高纯氮气为载气,用纳秒激光分别溅射四唑、5-氨基四唑以及四唑与氮化锆、钒和铬形成的混合样品,并用反射式飞行时间质谱分析了生成的产物。结果表明,在532nm的激光轰击条件下,大量四唑、5-氨基四唑分子骨架保持完整,易脱去一个氢原子而形成高丰度的负离子,该负离子进一步与1～3个四唑、5-氨基四唑分子形成簇合物;在氮化锆、钒和铬存在下,激光轰击四唑后形成了四唑正离子及四唑分子数不超过2个的簇合物,正离子质谱未发现锆、钒和铬参与四唑簇合物的形成。研究结果表明,激光溅射含氮有机物主要是蒸发作用,可用该方法表征有机物并研究其相互作用特性。
To understand the decomposition and cluster behavior of tetrazole ring under laser ablation, tetrazole, 5-aminotetrazole, the mixture of tetrazole and zirconium nitride, vanadium, chromium were ablated by nanosecond laser with N_2 as carrier gas,and the products were analyzed by reflection time-of-flight mass spectrometer. The results showthat the skeleton of tetrazole and 5-amino tetrazole basically remains intact under laser ablation, and they tend to convert to high-abundance anions by lo sing one hydro gen atom and these anions associate further with 1—3 tetrazoles and 5-aminotetrazole molecules to form corresponding clusters. In the presence of ZrN, V and Cr, tetrazole cation and clusters with no more than 2 tetrazoles are fo rmed, and po sitive ion m ass spectrum cannot find these transitio n metals participating in the form ation of tetrazole clusters It is found that evaporation is identified to occur in laser ablation of nitrogen-rich compounds, and laser ablation can be used to characterize nitrogen-rich compounds and study their interaction characteristics.
To understand the decomposition and cluster behavior of tetrazole ring under laser ablation, tetrazole, 5-aminotetrazole, the mixture of tetrazole and zirconium nitride, vanadium, chromium were ablated by nanosecond laser with N_2 as carrier gas,and the products were analyzed by reflection time-of-flight mass spectrometer. The results showthat the skeleton of tetrazole and 5-amino tetrazole basically remains intact under laser ablation, and they tend to convert to high-abundance anions by lo sing one hydro gen atom and these anions associate further with 1—3 tetrazoles and 5-aminotetrazole molecules to form corresponding clusters. In the presence of ZrN, V and Cr, tetrazole cation and clusters with no more than 2 tetrazoles are fo rmed, and po sitive ion m ass spectrum cannot find these transitio n metals participating in the form ation of tetrazole clusters It is found that evaporation is identified to occur in laser ablation of nitrogen-rich compounds, and laser ablation can be used to characterize nitrogen-rich compounds and study their interaction characteristics.
引文
[1]王亮亮,刘艳,赵守田.H2BTA的非等温热分解特性[J].火炸药学报,2018,41(1):47-51.WAN G Liang-liang,LIU Yan,Z HAO Shou-tian.N onisothermal thermal decomposition characteristics of H2BTA[J].C hinese Journal of Explosives&Propellants(Huozhayao Xuebao),2018,41(1):47-51.
[2]Butler R N.Recent advances in tetrazole chemistry[J].A dvances in Heterocyclic C hemistry,1977,21:323-435.
[3]陈兆旭,肖鹤鸣.密度泛函理论和从头算方法对四唑负离子的比较研究[J].高等学校化学学报,1999,20(5):782-787.C HEN Z hao-xu,XIAO He-ming.C omparative investigation of the structure and IR of tetrazolate ion with density functional theory and MP2 Ab initio methods[J].C hemical Journal of C hinese Universities,1999,20(5):782-787.
[4]Lesnikovich A I,Ivashkevich O A,Printsev G V,et al.Thermal decomposition of tetrazole Part III.Analysis of decomposition products[J].Thermochimica A cta,1990,171:207-213.
[5]冯丽娜,张建国,张同来,等.氨基四唑化合物异构和分解反应的研究进展[J].含能材料,2009,17(1):113-118.FEN G Li-na,Z HAN G Jian-guo,Z HAN G Tong-lai,et al.Progress in the tautomerism and decomposition of amino-tetrazoles[J].C hinese Journal of Energetic Materials,2009,17(1):113-118.
[6]耿春宇,胡满成,李淑妮,等.Cs(ATZ)的制备、晶体结构与热力学性质[J].化学学报,2005,63(21):1974-1978.GEN G C hun-yu,HU Man-cheng,LI Shu-ni,et al.Preparation,crystal structure and thermodynamic properties of C s(ATZ)[J].A cta C himica Sinica,2005,63(21):1974-1978.
[7]张建国,张同来,郁开北.Cd(ATZ)4(H2O)2](PA)2·2H2O的合成、晶体结构和热分解机理研究[J].化学学报,2001,59(1):84-90.Z HAN G Jian-guo,Z HAN G Tong-lai,YU Kai-bei.Studies on synthesis,crystal structure and thermal decomposition mechanism of cadmium complex[C d(ATZ)a(H2O)2](PA)2·2H2O[J].A cta C himica Sinica,2001,59(1):84-90.
[8]张建国,张同来,郁开北.5-氨基四唑一水合物的制备及其分子结构[J].火工品,1999,3(3):1999-2005.Z HAN G Jian-guo,Z HAN G Tong-lai,YU Kai-bei.Preparation and molecular structure of 5-aminotetrazole monohydrate[J].Initiators&Pyrotechnics,1999,3(3):1999-2005.
[9]Zablocki J A,Miyano M,Rao S N,et al.Potent inhibitors of platelet aggregation based upon the Arg-GlyAsp-Phe sequence of fibrinogen.A proposal on the nature of the binding interaction between the Asp-carboxylate of R GD X mimetics and the platelet GP IIb-IIIa receptor[J].Journal of Medicinal Chemistry,1992,35(26):4914-4917.
[10]孙元元,张成华,薛英,等.四唑负离子与脒正离子复合物稳定性的理论研究[J].化学学报,2008,66(7):751-756.SU N Yuan-yuan,Z HAN G C heng-hua,XU E Ying,et al.Theoretical study on the stability of anionic tetrazolate complexes with amidiniums[J].A cta C himica Sinica,2008,66(7):751-756.
[11]Tominey A F,Docherty P H,Rosair G M,et al.U nusually weak binding interactions in tetrazole-amidine complexes[J].O rganic Letters,2006,8(7):1279-1282.
[12]Kurikawa T,Hirano M,Takeda H,et al.Structures and ionization energies of cobalt-benzene clusters(C on(benzene)m)[J].The Journal of Physical Chemistry,1995,99(44):16248-16252.
[13]Kurikawa T,Takeda H,Hirano M,et al.Electronic properties of organometallic metal-benzene complexes[Mn(benzene)m(M=Sc-Cu)][J].Organometallics,1999,18(8):1430-1438.
[14]Zheng WJ,Nilles J M,Thomas O C,et al.Photoelectron spectroscopy of titanium-benzene cluster anions[J].C hemical Physics Letters,2005,401(1-3):266-270.
[15]Gerhards M,Thomas O C,Nilles J M,et al.Cobalt-benzene cluster anions:mass spectrometry and negative ion photoelectron spectroscopy[J].The Journal of C hemical Physics,2002,116(23):10247-10249.
[16]李陶琦,许洪光,郝晓春,等.N+4的生成与检测[J].化学通报,2012,75(3):276-278.LI Tao-qi,XU Hong-guang,HAO Xiao-chun,et al.Formation and detection of N+4[J].Chemistry,2012,75(3):276-278.
[17]Ding K W,Li X W,Xu H G,et al.Experimental observation of Ti N+12cluster and theoretical investigation of its stable and metastable isomers[J].C hemical Science,2015,6:4723-4729.
[18]Ding K W,Xu H G,Yang Y,et al.Mass spectrometry and theoretical investigation of VN+n(n=8,9,10)clusters[J].The Journal of Physical C hemistry A,2018,122(20):4687-4695.
[19]Zhigilei L V,Kodali P B S,Garrison B J.On the threshold behavior in laser ablation of organic solids[J].C hemical Physics Letters,1997,276(3/4):269-273.
[2]Butler R N.Recent advances in tetrazole chemistry[J].A dvances in Heterocyclic C hemistry,1977,21:323-435.
[3]陈兆旭,肖鹤鸣.密度泛函理论和从头算方法对四唑负离子的比较研究[J].高等学校化学学报,1999,20(5):782-787.C HEN Z hao-xu,XIAO He-ming.C omparative investigation of the structure and IR of tetrazolate ion with density functional theory and MP2 Ab initio methods[J].C hemical Journal of C hinese Universities,1999,20(5):782-787.
[4]Lesnikovich A I,Ivashkevich O A,Printsev G V,et al.Thermal decomposition of tetrazole Part III.Analysis of decomposition products[J].Thermochimica A cta,1990,171:207-213.
[5]冯丽娜,张建国,张同来,等.氨基四唑化合物异构和分解反应的研究进展[J].含能材料,2009,17(1):113-118.FEN G Li-na,Z HAN G Jian-guo,Z HAN G Tong-lai,et al.Progress in the tautomerism and decomposition of amino-tetrazoles[J].C hinese Journal of Energetic Materials,2009,17(1):113-118.
[6]耿春宇,胡满成,李淑妮,等.Cs(ATZ)的制备、晶体结构与热力学性质[J].化学学报,2005,63(21):1974-1978.GEN G C hun-yu,HU Man-cheng,LI Shu-ni,et al.Preparation,crystal structure and thermodynamic properties of C s(ATZ)[J].A cta C himica Sinica,2005,63(21):1974-1978.
[7]张建国,张同来,郁开北.Cd(ATZ)4(H2O)2](PA)2·2H2O的合成、晶体结构和热分解机理研究[J].化学学报,2001,59(1):84-90.Z HAN G Jian-guo,Z HAN G Tong-lai,YU Kai-bei.Studies on synthesis,crystal structure and thermal decomposition mechanism of cadmium complex[C d(ATZ)a(H2O)2](PA)2·2H2O[J].A cta C himica Sinica,2001,59(1):84-90.
[8]张建国,张同来,郁开北.5-氨基四唑一水合物的制备及其分子结构[J].火工品,1999,3(3):1999-2005.Z HAN G Jian-guo,Z HAN G Tong-lai,YU Kai-bei.Preparation and molecular structure of 5-aminotetrazole monohydrate[J].Initiators&Pyrotechnics,1999,3(3):1999-2005.
[9]Zablocki J A,Miyano M,Rao S N,et al.Potent inhibitors of platelet aggregation based upon the Arg-GlyAsp-Phe sequence of fibrinogen.A proposal on the nature of the binding interaction between the Asp-carboxylate of R GD X mimetics and the platelet GP IIb-IIIa receptor[J].Journal of Medicinal Chemistry,1992,35(26):4914-4917.
[10]孙元元,张成华,薛英,等.四唑负离子与脒正离子复合物稳定性的理论研究[J].化学学报,2008,66(7):751-756.SU N Yuan-yuan,Z HAN G C heng-hua,XU E Ying,et al.Theoretical study on the stability of anionic tetrazolate complexes with amidiniums[J].A cta C himica Sinica,2008,66(7):751-756.
[11]Tominey A F,Docherty P H,Rosair G M,et al.U nusually weak binding interactions in tetrazole-amidine complexes[J].O rganic Letters,2006,8(7):1279-1282.
[12]Kurikawa T,Hirano M,Takeda H,et al.Structures and ionization energies of cobalt-benzene clusters(C on(benzene)m)[J].The Journal of Physical Chemistry,1995,99(44):16248-16252.
[13]Kurikawa T,Takeda H,Hirano M,et al.Electronic properties of organometallic metal-benzene complexes[Mn(benzene)m(M=Sc-Cu)][J].Organometallics,1999,18(8):1430-1438.
[14]Zheng WJ,Nilles J M,Thomas O C,et al.Photoelectron spectroscopy of titanium-benzene cluster anions[J].C hemical Physics Letters,2005,401(1-3):266-270.
[15]Gerhards M,Thomas O C,Nilles J M,et al.Cobalt-benzene cluster anions:mass spectrometry and negative ion photoelectron spectroscopy[J].The Journal of C hemical Physics,2002,116(23):10247-10249.
[16]李陶琦,许洪光,郝晓春,等.N+4的生成与检测[J].化学通报,2012,75(3):276-278.LI Tao-qi,XU Hong-guang,HAO Xiao-chun,et al.Formation and detection of N+4[J].Chemistry,2012,75(3):276-278.
[17]Ding K W,Li X W,Xu H G,et al.Experimental observation of Ti N+12cluster and theoretical investigation of its stable and metastable isomers[J].C hemical Science,2015,6:4723-4729.
[18]Ding K W,Xu H G,Yang Y,et al.Mass spectrometry and theoretical investigation of VN+n(n=8,9,10)clusters[J].The Journal of Physical C hemistry A,2018,122(20):4687-4695.
[19]Zhigilei L V,Kodali P B S,Garrison B J.On the threshold behavior in laser ablation of organic solids[J].C hemical Physics Letters,1997,276(3/4):269-273.