Molecular dynamics simulations of zinc oxide solubility: From bulk down to nanoparticles

Escorihuela, Laura; Fernández, Alberto; Rallo, Robert; Martorell, Benjamí

doi:10.1016/j.fct.2017.07.038

Title: Molecular dynamics simulations of zinc oxide solubility: From bulk down to nanoparticles

Journal Article · 20 July 2017 · Food and Chemical Toxicology

DOI: https://doi.org/10.1016/j.fct.2017.07.038 · OSTI ID:1390577

Escorihuela, Laura ^[1];

^[1]; Rallo, Robert ^[2]; Martorell, Benjamí ^[3]

Univ. of Rovira, Catalonia (Spain). Dept. of Chemical Engineering
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Advanced Computing, Mathematics and Data Division
Deregallera LTD, Wales (United Kingdom). Materials Science Dept.

The solubility of metal oxides is one of the key descriptors for the evaluation of their potential toxic effects, both in the bulk form and in nanoparticulated aggregates. This work presents a new methodology for the in silico assessment of the solubility of metal oxides, which is demonstrated using a well-studied system, ZnO. The calculation of the solubility is based on statistical thermodynamics tools combined with Density Functional Tight Binding theory for the evaluation of the free energy exchange during the dissolution process. We used models of small ZnO clusters to describe the final dissolved material, since the complete ionic dissolution of ZnO is hindered by the formation of O^2- anions in solution, which are highly unstable. Results show very good agreement between the computed solubility values and experimental data for ZnO bulk, up to 0.5 mg L^-1 and equivalents of 50 μg L^-1 for the free Zn²⁺ cation in solution. However, the reference model for solid nanoparticles formed by free space nanoparticles can only give a limited quantitative solubility evaluation for ZnO nanoparticles.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830; SOE1/P1/E0215; 2014 SGR 1352

OSTI ID:: 1390577

Alternate ID(s):: OSTI ID: 1395281

Report Number(s):: PNNL-SA-127574; PII: S0278691517304106

Journal Information:: Food and Chemical Toxicology, Vol. 112; ISSN 0278-6915

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 8 works

Citation information provided by
Web of Science

References (26)

DFTB+, a Sparse Matrix-Based Implementation of the DFTB Method ^† Aradi, B.; Hourahine, B.; Frauenheim, Th. The Journal of Physical Chemistry A, Vol. 111, Issue 26 https://doi.org/10.1021/jp070186p	journal	July 2007
A theoretical framework for predicting the oxidative stress potential of oxide nanoparticles Burello, Enrico; Worth, Andrew P. Nanotoxicology, Vol. 5, Issue 2 https://doi.org/10.3109/17435390.2010.502980	journal	July 2010
A DFT investigation on ZnO clusters and nanostructures Cheng, Xueli; Li, Feng; Zhao, Yanyun Journal of Molecular Structure: THEOCHEM, Vol. 894, Issue 1-3 https://doi.org/10.1016/j.theochem.2008.10.023	journal	January 2009
Application of the SCC-DFTB Method to Hydroxide Water Clusters and Aqueous Hydroxide Solutions Choi, Tae Hoon; Liang, Ruibin; Maupin, C. Mark The Journal of Physical Chemistry B, Vol. 117, Issue 17 https://doi.org/10.1021/jp400953a	journal	April 2013
Dissolution Kinetics and Solubility of ZnO Nanoparticles Followed by AGNES David, Calin A.; Galceran, Josep; Rey-Castro, Carlos The Journal of Physical Chemistry C, Vol. 116, Issue 21, p. 11758-11767 https://doi.org/10.1021/jp301671b	journal	May 2012
Tetrahedral vs Octahedral Zinc Complexes with Ligands of Biological Interest: A DFT/CDM Study Dudev, Todor; Lim, Carmay Journal of the American Chemical Society, Vol. 122, Issue 45 https://doi.org/10.1021/ja0010296	journal	November 2000
Self-consistent-charge density-functional tight-binding method for simulations of complex materials properties Elstner, M.; Porezag, D.; Jungnickel, G. Physical Review B, Vol. 58, Issue 11, p. 7260-7268 https://doi.org/10.1103/PhysRevB.58.7260	journal	September 1998
Comparative Toxicity of Nanoparticulate ZnO, Bulk ZnO, and ZnCl ₂ to a Freshwater Microalga (Pseudokirchneriella subcapitata): The Importance of Particle Solubility Franklin, Natasha M.; Rogers, Nicola J.; Apte, Simon C. Environmental Science & Technology, Vol. 41, Issue 24 https://doi.org/10.1021/es071445r	journal	December 2007
Use of a Rapid Cytotoxicity Screening Approach To Engineer a Safer Zinc Oxide Nanoparticle through Iron Doping George, Saji; Pokhrel, Suman; Xia, Tian ACS Nano, Vol. 4, Issue 1 https://doi.org/10.1021/nn901503q	journal	December 2009
Perspective: How good is DFT for water? Gillan, Michael J.; Alfè, Dario; Michaelides, Angelos The Journal of Chemical Physics, Vol. 144, Issue 13 https://doi.org/10.1063/1.4944633	journal	April 2016
Application of the SCC-DFTB Method to Neutral and Protonated Water Clusters and Bulk Water Goyal, Puja; Elstner, Marcus; Cui, Qiang The Journal of Physical Chemistry B, Vol. 115, Issue 20 https://doi.org/10.1021/jp202259c	journal	May 2011
An SCC-DFTB Repulsive Potential for Various ZnO Polymorphs and the ZnO–Water System Hellström, Matti; Jorner, Kjell; Bryngelsson, Maria The Journal of Physical Chemistry C, Vol. 117, Issue 33 https://doi.org/10.1021/jp404095x	journal	August 2013
Atomistic Simulations of the ZnO(12̅10)/Water Interface: A Comparison between First-Principles, Tight-Binding, and Empirical Methods große Holthaus, Svea; Köppen, Susan; Frauenheim, Thomas Journal of Chemical Theory and Computation, Vol. 8, Issue 11 https://doi.org/10.1021/ct3007106	journal	October 2012
Large-scale SCC-DFTB calculations of reconstructed polar ZnO surfaces Huber, Stefan E.; Hellström, Matti; Probst, Michael Surface Science, Vol. 628 https://doi.org/10.1016/j.susc.2014.05.001	journal	October 2014
Performance of density-functional tight-binding models in describing hydrogen-bonded anionic-water clusters Jahangiri, Soran; Cai, Lemin; Peslherbe, Gilles H. Journal of Computational Chemistry, Vol. 35, Issue 23 https://doi.org/10.1002/jcc.23677	journal	July 2014
Density-functional tight-binding for beginners Koskinen, Pekka; Mäkinen, Ville Computational Materials Science, Vol. 47, Issue 1 https://doi.org/10.1016/j.commatsci.2009.07.013	journal	November 2009
Stability, Bioavailability, and Bacterial Toxicity of ZnO and Iron-Doped ZnO Nanoparticles in Aquatic Media Li, Minghua; Pokhrel, Suman; Jin, Xue Environmental Science & Technology, Vol. 45, Issue 2 https://doi.org/10.1021/es102266g	journal	January 2011
Development of structure–activity relationship for metal oxide nanoparticles Liu, Rong; Zhang, Hai Yuan; Ji, Zhao Xia Nanoscale, Vol. 5, Issue 12 https://doi.org/10.1039/c3nr01533e	journal	January 2013
The Self-Consistent Charge Density Functional Tight Binding Method Applied to Liquid Water and the Hydrated Excess Proton: Benchmark Simulations Maupin, C. Mark; Aradi, Bálint; Voth, Gregory A. The Journal of Physical Chemistry B, Vol. 114, Issue 20 https://doi.org/10.1021/jp1010555	journal	May 2010
Toward an Accurate Density-Functional Tight-Binding Description of Zinc-Containing Compounds Moreira, Ney H.; Dolgonos, Grygoriy; Aradi, Bálint Journal of Chemical Theory and Computation, Vol. 5, Issue 3 https://doi.org/10.1021/ct800455a	journal	February 2009
Divide-and-Conquer-Type Density-Functional Tight-Binding Molecular Dynamics Simulations of Proton Diffusion in a Bulk Water System Nakai, Hiromi; Sakti, Aditya Wibawa; Nishimura, Yoshifumi The Journal of Physical Chemistry B, Vol. 120, Issue 1 https://doi.org/10.1021/acs.jpcb.5b12439	journal	December 2015
Solubility of nano-zinc oxide in environmentally and biologically important matrices Reed, Robert B.; Ladner, David A.; Higgins, Christopher P. Environmental Toxicology and Chemistry, Vol. 31, Issue 1, p. 93-99 https://doi.org/10.1002/etc.708	journal	December 2011
Zinc Oxide Nanoparticles for Revolutionizing Agriculture: Synthesis and Applications Sabir, Sidra; Arshad, Muhammad; Chaudhari, Sunbal Khalil The Scientific World Journal, Vol. 2014 https://doi.org/10.1155/2014/925494	journal	January 2014
Tight-Binding Density Functional Theory: An Approximate Kohn−Sham DFT Scheme ^† Seifert, G. The Journal of Physical Chemistry A, Vol. 111, Issue 26 https://doi.org/10.1021/jp069056r	journal	July 2007
Comparison of the Mechanism of Toxicity of Zinc Oxide and Cerium Oxide Nanoparticles Based on Dissolution and Oxidative Stress Properties Xia, Tian; Kovochich, Michael; Liong, Monty ACS Nano, Vol. 2, Issue 10 https://doi.org/10.1021/nn800511k	journal	October 2008
Decreased Dissolution of ZnO by Iron Doping Yields Nanoparticles with Reduced Toxicity in the Rodent Lung and Zebrafish Embryos Xia, Tian; Zhao, Yan; Sager, Tina ACS Nano, Vol. 5, Issue 2 https://doi.org/10.1021/nn1028482	journal	January 2011

Cited By (2)

Toward computational and experimental characterisation for risk assessment of metal oxide nanoparticles Escorihuela, Laura; Martorell, Benjamí; Rallo, Robert Environmental Science: Nano, Vol. 5, Issue 10 https://doi.org/10.1039/c8en00389k	journal	January 2018
Molecular Dynamics Simulation for Mechanism Elucidation of Food Processing and Safety: State of the Art: MD simulation for mechanism elucidation… Chen, Gang; Huang, Kai; Miao, Ming Comprehensive Reviews in Food Science and Food Safety, Vol. 18, Issue 1 https://doi.org/10.1111/1541-4337.12406	journal	November 2018