Hg sorption by Fe3O4/SiO2 core-shell nanoparticles functionalized with dithiocarbamate: Determining Hg coordination with a combined experimental and ab-initio approach

abstract

Nanoparticles functionalized with dithiocarbamate groups are well known for their high uptake efficiency of Hg(II) from water but where and how Hg coordinates is still an open question. In the present work, Perturbed Angular Correlations spectroscopy was combined with Density Functional Theory modelling to answer that question. Measuring the electric field gradient and comparing it with its calculated counterpart allows to determine the most probable local environment of Hg and its coordination, both for dithiocarbamate functionalized nanoparticles and for silica coated magnetite nanoparticles. The calculated bonding energy also answers why dithiocarbamate functionalized nanoparticles present such a high sorption efficiency.

keywords

NUCLEAR-QUADRUPOLE INTERACTION; SORBENTS; REMOVAL; MERCURY

subject category

Physics

authors

Amorim, CO; Fortunato, NM; Fenta, AS; Gonsalves, JN; Tavares, DS; Lopes, CB; Trindade, T; Correia, JG; Amaral, VS

Groups

G1 - Porous Materials and Nanosystems
G2 - Photonic, Electronic and Magnetic Materials
G6 - Virtual Materials and Artificial Intelligence

Projects

Collaboratory for Emerging Technologies, CoLab (EMERGING TECHNOLOGIES)

CICECO - Aveiro Institute of Materials (UIDB/50011/2020)

CICECO - Aveiro Institute of Materials (UIDP/50011/2020)

Associated Laboratory CICECO-Aveiro Institute of Materials (LA/P/0006/2020)

Nanomaterials for the uptake of pollutant metals ions: efficiency, selectivity and recyclability (PTDC/CTM-NAN/120668/2010)

Centre for Research in Ceramics and Composite Materials - CICECO (LA0011: 2013-2014) (PEst-C/CTM/LA0011/2013)

CICECO - Aveiro Institute of Materials (UID/CTM/50011/2013)

Material’s Research with Radioactive Isotopes and Nuclear Techniques at ISOLDE-CERN 2024 (ISOLDE)

acknowledgements

This work is financed by Portugal 2020 through European Regional Development Fund (ERDF) in the frame of CENTRO2020 in the scope of the project CICECO - Aveiro Institute of Materials, UIDB/50011/2020 & UIDP/50011/2020 & LA/P/0006/2020, and in the scope of LISBOA-01-0247-FEDER-039985/POCI-01-0247-FEDER-039985, LA/P/0037/2020, UIDP/50025/2020, and UIDB/50025/2020 of the Associate Lab-oratory Institute of Nanostructures, Nanomodelling and Nano fabrica-tion - i3N, financed by national funds through the FCT/MEC (PIDDAC) . This work has also been supported by the Portuguese Foundation for Science and Technology (FCT) with projects CERN-FIS-NUC-0004-2015,PTDC/CTM-NAN/120668/2010, Pest-C/CTM/LA0011/2013, Pest-C/MAR/LA0017/2013, POCI-01-0145-FEDER-007679-FCT Ref. UID/CTM/50011/2013, financed by national funds through the FCT/MEC, and, when appropriate, co-financed by FEDER under the PT2020 Partnership Agreement. FCT is also acknowledged for scholarship grants SFRH/BD/93336/2013 (C.O. Amorim) , SFRH/BD/84743/2012 (A.S. Fenta) , SFRH/BD/103828/2014 (D.S. Tavares) , SFRH/BPD/99453/2014 (C.B. Lopes) and SFRH/BPD/82059/2011 (J. N. Gonsalves) . Other institutions are acknowledged: A.S. Fenta from support by the Scientific Research-Flanders (G.0983.15) and the KU Leuven BOF (CREA/14/013 and STRT/14/002) from Belgium. The German Fed-eral Ministry of Education and Research (BMBF) through contract 05K13TSA and 05K16PGA is acknowledged for equipment used during experiments. The European Commission, through the Horizon 2020 program (grant number 654002 ENSAR2) for support accessing the ISOLDE laboratory. The authors would like to thank the operation and technical ISOLDE teams and the Solid State Physics coordinator Dr. Juliana Schell.