Natural rhenium sulfide clusters formed under conditions of laser desorption-ionization

IF 1.8 3区 化学 Q4 BIOCHEMICAL RESEARCH METHODS Rapid Communications in Mass Spectrometry Pub Date : 2024-09-23 DOI:10.1002/rcm.9919
Viacheslav V. Lebedev, Daniil I. Yarykin, Ilya V. Chaplygin, Oleg P. Gorelkov, Rinad Kh. Zalavutdinov, Aleksey K. Buryak
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Abstract

Rationale

Cluster forms of rhenium sulfides have important practical applications as catalysts in oil refining and thus present high interest. However, only a limited number of rhenium sulfide clusters have been described previously. It is known that cluster formation actively occurs under conditions of laser desorption–ionization; nevertheless, detailed studies of rhenium sulfides under such conditions were apparently not conducted previously.

Methods

A sample of natural rhenium sulfide, collected from the fumarolic field of Kudriavy volcano (Iturup island, Russia) in 2002, was investigated using the laser desorption–ionization mass spectrometry method. The formed rhenium sulfide clusters were registered by a time-of-flight detector and identified programmatically using the software developed in IPCE RAS. The identification involved a comparison of the distribution of isotopic peak intensities, observed in the resulting mass spectra, with the theoretical probabilities of occurrence of various isotopologues for hypothetical rhenium sulfide species.

Results

Over 60 rhenium sulfide clusters of RexSy+ and RexSyOz types containing up to 10 rhenium atoms were formed when a sample of natural rhenium sulfide was exposed to laser desorption–ionization conditions. Several isolated heterometallic ReXMoSY+ and ReXMoSYOZ clusters containing up to eight rhenium atoms were additionally observed in the resulting mass spectra. The species with compositions, for which the electrically neutral analogs are known, apparently were the most stable rhenium sulfide clusters among the detected ones.

Conclusions

The obtained data allowed summarizing the patterns of formation of rhenium sulfide clusters under conditions of laser desorption-ionization. The ability of rhenium and sulfur to form cluster species containing from 7 to 10 atoms of rhenium was likely discovered for the first time. The majority of the rhenium sulfide clusters described in this study, notably RexSy+ ions containing over seven atoms of rhenium, were apparently not observed previously.

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在激光解吸电离条件下形成的天然硫化铼簇。
理由:簇状硫化铼作为炼油催化剂具有重要的实际应用价值,因此备受关注。然而,以前描述的硫化铼团簇数量有限。众所周知,在激光解吸电离条件下,簇的形成非常活跃;然而,以前显然没有对这种条件下的硫化铼进行过详细研究:方法:使用激光解吸电离质谱法研究了 2002 年从库德里亚维火山(俄罗斯伊图鲁普岛)的熔岩区采集的天然硫化铼样品。形成的硫化铼簇由飞行时间探测器记录,并使用 IPCE RAS 开发的软件进行程序化识别。鉴定工作包括将质谱中观察到的同位素峰强度分布与假设硫化铼物种的各种同位素出现的理论概率进行比较:将天然硫化铼样品置于激光解吸电离条件下,可形成 60 多种 RexSy + 和 RexSyOz - 型硫化铼簇,其中最多含有 10 个铼原子。此外,在生成的质谱中还观察到了几个孤立的异金属 ReXMoSY + 和 ReXMoSYOZ - 簇,其中最多含有 8 个铼原子。在检测到的硫化铼团簇中,具有已知电中性类似物成分的物种显然是最稳定的:所获得的数据有助于总结在激光解吸电离条件下硫化铼簇的形成模式。铼和硫能够形成含有 7 至 10 个铼原子的团簇物种,这可能是首次发现。本研究中描述的大多数硫化铼簇,特别是含有超过 7 个铼原子的 RexSy + 离子,以前显然没有观察到。
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来源期刊
CiteScore
4.10
自引率
5.00%
发文量
219
审稿时长
2.6 months
期刊介绍: Rapid Communications in Mass Spectrometry is a journal whose aim is the rapid publication of original research results and ideas on all aspects of the science of gas-phase ions; it covers all the associated scientific disciplines. There is no formal limit on paper length ("rapid" is not synonymous with "brief"), but papers should be of a length that is commensurate with the importance and complexity of the results being reported. Contributions may be theoretical or practical in nature; they may deal with methods, techniques and applications, or with the interpretation of results; they may cover any area in science that depends directly on measurements made upon gaseous ions or that is associated with such measurements.
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