Journal article
Cu‑, Co‑, and Zn-Based Metal–Organic Framework-Derived Nanoporous Ion Emitters for Picogram Level Analysis of Actinides
ACS applied materials & interfaces, Vol.17(28), pp.40753-40764
07/16/2025
DOI: 10.1021/acsami.5c08914
PMID: 40586879
Abstract
Thermal ionization mass spectrometry (TIMS) is often regarded as the preferred technique for trace-level isotopic analysis of actinides owing to its high sensitivity and absence of carry-over effects. However, actinide sample utilization efficiency (SUE) is typically low (<0.05%) without the use of activators or specialized loading approaches which can yield SUEs of >5%. To this effect, we investigate a series of metal–organic framework (MOF)-based nanoporous ion emitters (nano-PIEs) that show enhanced ionization of actinides when used in TIMS loading. We study the impact of physical and chemical properties of MOFs on TIMS SUEs using two families of MOFs that can be synthesized under similar reaction conditions. The structural and chemical properties of these MOFs can be systematically modified one at a time while keeping other features the same. This allows us to strategically investigate their impact on SUEs. The first family of MOFs considered in this study is Zeolitic Imidazole Frameworks (ZIFs) which are made using 2 methyl-imidazole as an organic linker with zinc (ZIF-8) and cobalt (ZIF-67) as metal centers. Additionally, the effect of morphology was also studied using Zn-based ZIF-L with a 2-dimensional structure. The second family of MOFs was synthesized using benzene-1,3,5-tricarboxylate (BTC) with copper (Cu-BTC) and zinc (Zn-BTC) as the metal center. Among the MOFs tested, Cu-BTC showed the highest SUE with an average SUE of 0.27 ± 0.15%, followed closely by Zn-BTC (0.24 ± 0.10%), ZIF-8 (0.17 ± 0.10%), and trailed by the other MOFs. When the MOFs were pyrolyzed in N2 before loading, an apparent increase in the SUE was observed with ZIF-8 and Cu-BTC showing average SUEs of 0.25 ± 0.08% and 0.34 ± 0.13%, respectively, with the highest measured SUE of 0.53% for pyrolyzed Cu-BTC. This observed increase in SUE by up to an order of magnitude compared to bare filaments demonstrates the efficacy and potential of MOF-derived nano-PIEs for TIMS application.
Details
- Title: Subtitle
- Cu‑, Co‑, and Zn-Based Metal–Organic Framework-Derived Nanoporous Ion Emitters for Picogram Level Analysis of Actinides
- Creators
- Abhishek Kumar - Pacific Northwest National LaboratoryJi-Hye Seo - Pacific Northwest National LaboratoryYingzhe Wu - Pacific Northwest National LaboratoryEirik J. Krogstad - Pacific Northwest National LaboratoryKyle A. Makovsky - Pacific Northwest National LaboratoryMin-Bum Kim - Energy and Environment DirectorateMichael A. Sinnwell - University of IowaDushyant Barpaga - Pacific Northwest National LaboratoryKelly McHugh - Pacific Northwest National Laboratory
- Resource Type
- Journal article
- Publication Details
- ACS applied materials & interfaces, Vol.17(28), pp.40753-40764
- DOI
- 10.1021/acsami.5c08914
- PMID
- 40586879
- NLM abbreviation
- ACS Appl Mater Interfaces
- ISSN
- 1944-8244
- eISSN
- 1944-8252
- Publisher
- American Chemical Society
- Number of pages
- 12
- Language
- English
- Date published
- 07/16/2025
- Academic Unit
- Chemistry
- Record Identifier
- 9984936618902771
Metrics
6 Record Views