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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Oxidation Studies of Dipositive Actinide Ions,An~(2+) (An = Th,U,Np,Pu,Am) in the Gas Phase:Synthesis and Characterization of the Isolated Uranyl,Neptunyl,and Plutonyl Ions UO_2~(2+)(g),NpO_2~(2+)(g),and PuO_2~(2+)(g)
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Oxidation Studies of Dipositive Actinide Ions,An~(2+) (An = Th,U,Np,Pu,Am) in the Gas Phase:Synthesis and Characterization of the Isolated Uranyl,Neptunyl,and Plutonyl Ions UO_2~(2+)(g),NpO_2~(2+)(g),and PuO_2~(2+)(g)

机译：气相中正Act系元素离子An〜（2+）（An = Th，U，Np，Pu，Am）的氧化研究：分离的铀酰，海戊基和戊酰基离子UO_2〜（2+）的合成与表征（g），NpO_2〜（2 +）（g）和PuO_2〜（2 +）（g）

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Reactions of atomic and ligated dipositive actinide ions,An~(2+),AnO~(2+),AnOH~(2+),and AnO_2~(2+) (An = Th,U,Np,Pu,Am) were systematically studied by Fourier transform ion cyclotron resonance mass spectrometry.Kinetics were measured for reactions with the oxidants,N_2O,C_2H_4O (ethylene oxide),H_2O,O_2,CO_2,NO,and CH_2O.Each of the five An~(2+) ions reacted with one or more of these oxidants to produce AnO~(2+),and reacted with H_2O to produce AnOH~(2+).The measured pseudo-first-order reaction rate constants,k,revealed disparate reaction efficiencies,k/k_(COL).Th~(2+) was generally the most reactive and Am~(2+) the least.Whereas each oxidant reacted with Th~(2+) to give ThO~(2+),only C_2H_4O oxidized Am~(2+) to AmO~(2+).The other An~(2+) exhibited intermediate reactivities.Based on the oxidation reactions,bond energies and formation enthalpies were derived for the AnO~(2+),as were second ionization energies for the monoxides,IE[AnO~+].The bare dipositive actinyl ions,UO_2~(2+),NpO_2~(2+),and PuO_2~(2+),were produced from the oxidation of the corresponding AnO~(2+) by N2O,and by O_2 in the cases of UO~(2+) and NpO~(2+).Thermodynamic properties were derived for these three actinyls,including enthalpies of formation and electron affinities.It is concluded that bare UO_2~(2+),NpO_2~(2+),and PuO_2~(2+) are thermodynamically stable toward Coulomb dissociation to {AnO~+ + O~+} or {An~+ + O_2~+}.It is predicted that bare AmO_2~(2+) is thermodynamically stable.In accord with the expected instability of Th(VI),ThO~(2+) was not oxidized to ThO_2~(2+) by any of the seven oxidants.The gas-phase results are compared with the aqueous thermochemistry.Hydration enthalpies were derived here for uranyl and plutonyl;our DELTAH_(hyd)[UO_2~(2+)] is substantially more negative than the previously reported value,but is essentially the same as our DELTAH_(hyd)-[PuO_2~(2+)].
机译：原子和连接的正act系元素离子An〜（2 +），AnO〜（2 +），AnOH〜（2+）和AnO_2〜（2+）的反应（An = Th，U，Np，Pu，Am）用傅立叶变换离子回旋共振质谱系统地研究了动力学，测定了与氧化剂N_2O，C_2H_4O（环氧乙烷），H_2O，O_2，CO_2，NO和CH_2O的反应动力学。五个An〜（2+）中的每一个离子与一种或多种氧化剂反应生成AnO〜（2+），并与H_2O反应生成AnOH〜（2+）。测得的拟一阶反应速率常数k揭示了不同的反应效率k /k_(COL).Th~(2+）通常是最活泼的，而Am〜（2+）最小。而每种氧化剂与Th〜（2+）反应生成ThO〜（2+），只有C_2H_4O被氧化Am〜（2+）至AmO〜（2+）。另一个An〜（2+）表现出中等反应性。基于氧化反应，得出了AnO〜（2+）的键能和形成焓。一氧化碳的第二电离能，即IE [AnO〜+]。裸正性act化离子，UO_2〜（2 +），NpO_2〜（ 2+）和PuO_2〜（2+）是由相应的AnO〜（2+）被N2O氧化生成的，在UO〜（2+）和NpO〜（2+）的情况下由O_2氧化生成的。推导了这三个光化学基团的热力学性质，包括形成焓和电子亲和力。得出结论，裸露的UO_2〜（2 +），NpO_2〜（2+）和PuO_2〜（2+）对库仑解离成热力学稳定。 {AnO〜+ + O〜+}或{An〜+ + O_2〜+}。据预测，裸AmO_2〜（2+）具有热力学稳定性。与Th（VI），ThO〜（ 2+）未被7种氧化剂中的任何一种氧化为ThO_2〜（2+）。将气相分析结果与水热化学方法进行了比较。得出了铀酰和and酮的水合焓;我们的DELTAH_（hyd）[UO_2〜 （2+）]基本上比以前报告的值更负，但与我们的DELTAH_（hyd）-[PuO_2〜（2+）]基本相同。

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