Thiol-Functionalized Adsorbents through Atomic Layer Deposition and Vapor-Phase Silanization for Heavy Metal Ion Removal

Rozyyev, Vepa; Gao, Feng; Liu, Yining; Shevate, Rahul; Pathak, Rajesh; Mane, Anil U.; Darling, Seth B.; Elam, Jeffrey W.

doi:10.1021/acsami.4c03935

Thiol-Functionalized Adsorbents through Atomic Layer Deposition and Vapor-Phase Silanization for Heavy Metal Ion Removal

Journal Article · Mon Jun 24 00:00:00 EDT 2024 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.4c03935· OSTI ID:2467345

Rozyyev, Vepa ^[1]; Gao, Feng ^[2]; Liu, Yining ^[3]; ^[4]; Pathak, Rajesh ^[4]; Mane, Anil U. ^[4]; ^[5]; ^[6]

Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Advanced Materials for Energy-Water Systems (AMEWS)
Energy Frontier Research Centers (EFRC) (United States). Advanced Materials for Energy-Water Systems (AMEWS); Argonne National Laboratory (ANL), Argonne, IL (United States)
Univ. of Chicago, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Advanced Materials for Energy-Water Systems (AMEWS); Argonne National Laboratory (ANL), Argonne, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Energy Frontier Research Centers (EFRC) (United States). Advanced Materials for Energy-Water Systems (AMEWS); Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Advanced Materials for Energy-Water Systems (AMEWS)

The removal of toxic heavy metal ions from water resources is crucial for environmental protection and public health. In this study, we address this challenge by developing a surface functionalization technique for the selective adsorption of these contaminants. Our approach involves atomic layer deposition (ALD) followed by vapor-phase silanization of porous substrates. We utilized porous silica gel powder (similar to 100 mu m particles, 89 m²/g surface area, similar to 30 nm pores) as an initial substrate. This powder was first coated with similar to 0.5 nm ALD Al₂O₃, followed by vapor-phase grafting of a thiol-functional silane. The modified powder, particularly in acidic conditions (pH = 4), showed high selectivity in adsorbing Cd(II), As(V), Pb(II), Hg(II), and Cu(II) heavy metal ions in mixed ion solutions over common benign ions (e.g., Na, K, Ca, and Mg). Langmuir adsorption isotherms and breakthrough adsorption studies were conducted to assess heavy metal binding affinity and revealed the order of Cd(II) < Pb(II) < Cu(II) < As(V) < Hg(II), with a significantly higher affinity for As(V) and Hg(II) ions. Time-dependent uptake studies demonstrated rapid removal of heavy metal ions from aqueous environments, with Hg(II) exhibiting the fastest adsorption kinetics on thiol-modified surfaces. Finally, these findings highlight the potential of ALD and vapor-phase silanization to create effective adsorbents for the targeted removal of hazardous contaminants from water.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Advanced Materials for Energy-Water Systems (AMEWS)

Sponsoring Organization:: Israel-US Binational Industrial Research and Development Foundation (BIRD); Israel–US Collaborative Water-Energy Research Center (CoWERC); USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2467345

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 26 Vol. 16; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Atomic Layer Deposition (ALD)
heavy metal ion removal
monolayer silanization
thiol functionals
vapor-phase techniques
water purification

Thiol-Functionalized Adsorbents through Atomic Layer Deposition and Vapor-Phase Silanization for Heavy Metal Ion Removal

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