Precise measurements of trace neodymium isotopes as Nd+ ions by thermal ionization mass spectrometry using film porous ion emitters

Shao, Xuepeng; Bu, Wenting; Long, Kaiming; Tang, Lei; Liu, Xuemei; Yan, Heng; Hao, Fang

doi:10.1016/j.sab.2019.105656

Cited by 11 publications

(5 citation statements)

References 44 publications

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“…Here, we focus on neodymium (Nd), which is becoming widely applied to many areas outside of traditional geochemistry and geochronology. Recent applications include paleoceanography, nuclear forensics, and source attribution with each new application necessitating the analysis of smaller sample sizes. − For example, isotope ratios of neodymium ( 143 Nd/ 144 Nd) extracted from marine animal samples have been used as intrinsic markers of local geology to track their origin …”

Section: Introductionmentioning

confidence: 99%

“…These existing sample loading techniques, utilizing resin beads and porous ion emitters (PIEs) as well as running in other polyatomic forms such as oxides (e.g., NdO + rather than Nd + ), have been developed to overcome innate low ionization efficiencies (Table ). ,− Known strategies for increasing sample utilization efficiency for TIMS include: (1) confining the sample emission to a point source; , (2) changing the oxidation state of the sample; ,, (3) establishing a high surface area in the ion emitting region of the filament to maximize sample ionization; ,,, and (4) incorporating a high work function, highly refractory metal during the loading procedure . Resin beads, which address the first two requirements listed above, have remained nearly unchanged since first introduced in the 1970s .…”

Section: Introductionmentioning

confidence: 99%

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Designing Porous Ion Emitters for Thermal Ionization Mass Spectrometry: Evaluating Metal–Organic Frameworks

et al. 2022

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This work describes the first exploration of metal− organic frameworks (MOFs) as "next-generation" ion emitters for thermal ionization mass spectrometry (TIMS). MOFs were identified as promising candidates for this application given the synthetic control over their desired structural properties. This tunability results in well-ordered, high-surface-area, high-porosity frameworks with targeted sorption affinities. Here, we explored an aluminum-based, bipyridine-containing MOF (MOF-253) with and without incorporating a high work function metal, rhenium (Re). After analysis of an Nd-bearing MOF, we hypothesized that the well-dispersed, sponge-like interconnected network of the degraded structure would enhance Nd ionization more than traditional TIMS loading techniques (i.e., phosphoric acid). Compared to filaments loaded with phosphoric acid that require an additional benzene carburization step, the Nd ionization efficiencies (atoms detected relative to atoms loaded) for heated filaments loaded with MOF-253 were similar (∼1%). Electron microscopy after TIMS analysis demonstrated that the MOF was retained on the filament. While these results are preliminary, they demonstrate that MOFs have potential to enhance ionization and exceed the performance of traditional loading techniques by forming nanoporous ion emitters. Thus, further experimentation is likely to exceed this performance through more specific selection of the base MOF structure and modifications to porosity and composition. This work represents a novel application of MOFs and a next step in the pursuit of advanced thermal ionization with potential to expand across the periodic table.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Designing Porous Ion Emitters for Thermal Ionization Mass Spectrometry: Evaluating Metal–Organic Frameworks

et al. 2022

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“…Based on the single-filament mode with the GO ionization enhancer, an average ionization efficiency of (0.44 ± 0.10)% toward Pu was achieved, which is close to that with the resin-bead method (0.54%) . Additionally, compared to other ionization-promoting methods such as the resin-bead loading, the benzene-vapor carburization, , and the PIE (porous ion emitter) method, − the GO-loading method possesses much shorter pretreatment time (within 5 min) and more simplified manual operation, showing better performing efficiency.…”

Section: Resultsmentioning

confidence: 67%

“…The in situ formed porous Pt–Re microstructure on the filament remarkably improved the sample utilization due to the increased interaction surface for ion emission. It has been proven as a kind of excellent ionization enhancer for Pu, , Am, U, Th, Nd, and Ce . A high ionization efficiency of approximately 1% for Pu was obtained .…”

Section: Introductionmentioning

confidence: 99%

Evaluation of Graphene Oxide as a Thermal Ionization Enhancer for Plutonium in TIMS Measurement

Zhang

Chen

et al. 2023

Anal. Chem.

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Thermal ionization mass spectrometry (TIMS) has been extensively employed for the assessment of plutonium (Pu) isotopes in nuclear forensics and environmental monitoring. Recently, great efforts have been made to improve the ionization efficiency (IE) of Pu to achieve better accuracy and precision for trace-level analysis. Herein, the thermal ionization enhancement effect for plutonium of graphene oxide (GO) was investigated and the corresponding mechanism was discussed. The GO layers were homogeneously mounted on the filament’s central surface to promote pg-level Pu ion emission. With the excellent structural property of GO, a greatly promoted ionization efficiency of 0.44% for Pu was obtained, and the initial ionization temperature for Pu was remarkably reduced from 1610 to 1390 °C. Average boosts in IE compared to the classical double-filament mode and graphite-loaded single-filament mode were 1640 and 520%, respectively. The analytical accuracy and precision based on the GO-loaded single-filament mode were validated using Pu isotopic certified reference materials. This work demonstrates the excellent property of GO as an ion source additive for Pu ionization, as it provided an interface for the promotion of energy transfer and Pu carbide formation. The operation of GO loading is quite simple and can be finished within 5 min. This rapid filament carburization approach has great potential for improving the measurement precision of trace-level plutonium isotopes and can be applied in nuclear safeguards, nuclear forensics, and environmental monitoring.

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“…This method was successfully tested on a series of mac and ultramac rock standards producing repeatable measurements of the stable Nd : 144 Nd and radiogenic 143 Nd : 144 Nd ratios. Improvements in Nd ionisation efficiency in TIMS was the subject of a paper by Shao et al 123 who developed a new porous ion emitter made from a slurry of Pt and Re powders. Dissected fragments of the resulting 'cake' were sintered onto Re laments prior to sample loading.…”

Section: New Developmentsmentioning

confidence: 99%

Atomic spectrometry update: review of advances in atomic spectrometry and related techniques

Evans

Pisonero

Smith

et al. 2020

J. Anal. At. Spectrom.

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Precise measurements of trace neodymium isotopes as Nd+ ions by thermal ionization mass spectrometry using film porous ion emitters

Cited by 11 publications

References 44 publications

Designing Porous Ion Emitters for Thermal Ionization Mass Spectrometry: Evaluating Metal–Organic Frameworks

Designing Porous Ion Emitters for Thermal Ionization Mass Spectrometry: Evaluating Metal–Organic Frameworks

Evaluation of Graphene Oxide as a Thermal Ionization Enhancer for Plutonium in TIMS Measurement

Atomic spectrometry update: review of advances in atomic spectrometry and related techniques

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