TY  - JOUR
AU  - Pincus, Lauren N.
AU  - Petrovic, Predrag V.
AU  - Gonzalez, Isabel S.
AU  - Stavitski, Eli
AU  - Fishman, Zachary S.
AU  - Rudel, Holly E.
AU  - Anastas, Paul T.
AU  - Zimmerman, Julie B.
PY  - 2021
UR  - http://cherry.chem.bg.ac.rs/handle/123456789/5368
AB  - The ability of transition metal chitosan complexes (TMCs) of varying valence and charge to selectively adsorb As(III) and As(V) over their strongest adsorptive competitor, phosphate is examined. Fe(III)-chitosan, Cu(II)-chitosan, Al(III)-chitosan, Ni(II)-chitosan, and Zn(II)-chitosan are synthesized, characterized via Attenuated Total Reflectance-Fourier Transform Infrared spectroscopy (ATR-FTIR) and X-ray Diffractometry (XRD), and their selective sorption capabilities towards arsenite and arsenate over phosphate are evaluated. It was found that the stability of the metal-chitosan complexes varied, with Al(III)- and Zn(II)-chitosan forming unstable complexes resulting in precipitation of gibbsite, and Wulfingite and zincite, respectively. Cu(II)-, Ni(II)-, and Fe(III)- chitosan formed a mixture of monodentate and bidentate complexes. The TMCs which formed the bidentate complex (Cu(II)-, Ni(II)-, and Fe(III)-) showed greater adsorption capability for arsenate in competitive systems with phosphate. Using the binary separation factor ∝t/c, it can be shown that only Fe(III)-chitosan is selective for As(V) and As(III) over phosphate. Density Functional Theory (DFT) modeling and extended X-ray absorption fine structure (EXAFS) determined that Fe(III)-chitosan and Ni(II)-chitosan adsorbed As(V) and As(III) via inner-sphere complexation, while Cu(II)-chitosan formed mainly outer-sphere complexes with As(V) and As(III). These differences in complexation likely result in the observed differences in selective adsorption capability towards As(V) and As(III) over phosphate.
PB  - Elsevier
T2  - Chemical Engineering Journal
T1  - Selective adsorption of arsenic over phosphate by transition metal cross-linked chitosan
VL  - 412
IS  - 128582
DO  - 10.1016/j.cej.2021.128582
ER  - 

@article{
author = "Pincus, Lauren N. and Petrovic, Predrag V. and Gonzalez, Isabel S. and Stavitski, Eli and Fishman, Zachary S. and Rudel, Holly E. and Anastas, Paul T. and Zimmerman, Julie B.",
year = "2021",
abstract = "The ability of transition metal chitosan complexes (TMCs) of varying valence and charge to selectively adsorb As(III) and As(V) over their strongest adsorptive competitor, phosphate is examined. Fe(III)-chitosan, Cu(II)-chitosan, Al(III)-chitosan, Ni(II)-chitosan, and Zn(II)-chitosan are synthesized, characterized via Attenuated Total Reflectance-Fourier Transform Infrared spectroscopy (ATR-FTIR) and X-ray Diffractometry (XRD), and their selective sorption capabilities towards arsenite and arsenate over phosphate are evaluated. It was found that the stability of the metal-chitosan complexes varied, with Al(III)- and Zn(II)-chitosan forming unstable complexes resulting in precipitation of gibbsite, and Wulfingite and zincite, respectively. Cu(II)-, Ni(II)-, and Fe(III)- chitosan formed a mixture of monodentate and bidentate complexes. The TMCs which formed the bidentate complex (Cu(II)-, Ni(II)-, and Fe(III)-) showed greater adsorption capability for arsenate in competitive systems with phosphate. Using the binary separation factor ∝t/c, it can be shown that only Fe(III)-chitosan is selective for As(V) and As(III) over phosphate. Density Functional Theory (DFT) modeling and extended X-ray absorption fine structure (EXAFS) determined that Fe(III)-chitosan and Ni(II)-chitosan adsorbed As(V) and As(III) via inner-sphere complexation, while Cu(II)-chitosan formed mainly outer-sphere complexes with As(V) and As(III). These differences in complexation likely result in the observed differences in selective adsorption capability towards As(V) and As(III) over phosphate.",
publisher = "Elsevier",
journal = "Chemical Engineering Journal",
title = "Selective adsorption of arsenic over phosphate by transition metal cross-linked chitosan",
volume = "412",
number = "128582",
doi = "10.1016/j.cej.2021.128582"
}

Pincus, L. N., Petrovic, P. V., Gonzalez, I. S., Stavitski, E., Fishman, Z. S., Rudel, H. E., Anastas, P. T.,& Zimmerman, J. B.. (2021). Selective adsorption of arsenic over phosphate by transition metal cross-linked chitosan. in Chemical Engineering Journal
Elsevier., 412(128582).
https://doi.org/10.1016/j.cej.2021.128582

Pincus LN, Petrovic PV, Gonzalez IS, Stavitski E, Fishman ZS, Rudel HE, Anastas PT, Zimmerman JB. Selective adsorption of arsenic over phosphate by transition metal cross-linked chitosan. in Chemical Engineering Journal. 2021;412(128582).
doi:10.1016/j.cej.2021.128582 .

Pincus, Lauren N., Petrovic, Predrag V., Gonzalez, Isabel S., Stavitski, Eli, Fishman, Zachary S., Rudel, Holly E., Anastas, Paul T., Zimmerman, Julie B., "Selective adsorption of arsenic over phosphate by transition metal cross-linked chitosan" in Chemical Engineering Journal, 412, no. 128582 (2021),
https://doi.org/10.1016/j.cej.2021.128582 . .

TY  - JOUR
AU  - Pincus, Lauren N.
AU  - Rudel, Holly E.
AU  - Petrovic, Predrag V.
AU  - Gupta, Srishti
AU  - Westerhoff, Paul
AU  - Muhich, Christopher L.
AU  - Zimmerman, Julie B.
PY  - 2020
UR  - http://cherry.chem.bg.ac.rs/handle/123456789/5369
AB  - Development of novel adsorbents often neglects the
competitive adsorption between co-occurring oxo-anions, overestimating realistic pollutant removal potentials, and overlooking
the need to improve selectivity of materials. This critical review
focuses on adsorptive competition between commonly cooccurring oxo-anions in water and mechanistic approaches for
the design and development of selective adsorbents. Six “target”
oxo-anion pollutants (arsenate, arsenite, selenate, selenite,
chromate, and perchlorate) were selected for study. Five
“competing” co-occurring oxo-anions (phosphate, sulfate, bicarbonate, silicate, and nitrate) were selected due to their potential to
compete with target oxo-anions for sorption sites resulting in
decreased removal of the target oxo-anions. First, a comprehensive review of competition between target and competitor oxo-anions
to sorb on commonly used, nonselective, metal (hydr)oxide materials is presented, and the strength of competition between each
target and competitive oxo-anion pair is classified. This is followed by a critical discussion of the different equations and models used
to quantify selectivity. Next, four mechanisms that have been successfully utilized in the development of selective adsorbents are
reviewed: variation in surface complexation, Lewis acid/base hardness, steric hindrance, and electrostatic interactions. For each
mechanism, the oxo-anions, both target and competitors, are ranked in terms of adsorptive attraction and technologies that exploit
this mechanism are reviewed. Third, given the significant effort to evaluate these systems empirically, the potential to use
computational quantum techniques, such as density functional theory (DFT), for modeling and prediction is explored. Finally, areas
within the field of selective adsorption requiring further research are detailed with guidance on priorities for screening and defining
selective adsorbents.
PB  - ACS Publications
T2  - Environmental Science and Technology
T1  - Exploring the Mechanisms of Selectivity for Environmentally Significant Oxo-Anion Removal during Water Treatment: A Review of Common Competing Oxo-Anions and Tools for Quantifying Selective Adsorption
VL  - 54
IS  - 16
SP  - 9769
EP  - 9790
DO  - 10.1021/acs.est.0c01666
ER  - 

@article{
author = "Pincus, Lauren N. and Rudel, Holly E. and Petrovic, Predrag V. and Gupta, Srishti and Westerhoff, Paul and Muhich, Christopher L. and Zimmerman, Julie B.",
year = "2020",
abstract = "Development of novel adsorbents often neglects the
competitive adsorption between co-occurring oxo-anions, overestimating realistic pollutant removal potentials, and overlooking
the need to improve selectivity of materials. This critical review
focuses on adsorptive competition between commonly cooccurring oxo-anions in water and mechanistic approaches for
the design and development of selective adsorbents. Six “target”
oxo-anion pollutants (arsenate, arsenite, selenate, selenite,
chromate, and perchlorate) were selected for study. Five
“competing” co-occurring oxo-anions (phosphate, sulfate, bicarbonate, silicate, and nitrate) were selected due to their potential to
compete with target oxo-anions for sorption sites resulting in
decreased removal of the target oxo-anions. First, a comprehensive review of competition between target and competitor oxo-anions
to sorb on commonly used, nonselective, metal (hydr)oxide materials is presented, and the strength of competition between each
target and competitive oxo-anion pair is classified. This is followed by a critical discussion of the different equations and models used
to quantify selectivity. Next, four mechanisms that have been successfully utilized in the development of selective adsorbents are
reviewed: variation in surface complexation, Lewis acid/base hardness, steric hindrance, and electrostatic interactions. For each
mechanism, the oxo-anions, both target and competitors, are ranked in terms of adsorptive attraction and technologies that exploit
this mechanism are reviewed. Third, given the significant effort to evaluate these systems empirically, the potential to use
computational quantum techniques, such as density functional theory (DFT), for modeling and prediction is explored. Finally, areas
within the field of selective adsorption requiring further research are detailed with guidance on priorities for screening and defining
selective adsorbents.",
publisher = "ACS Publications",
journal = "Environmental Science and Technology",
title = "Exploring the Mechanisms of Selectivity for Environmentally Significant Oxo-Anion Removal during Water Treatment: A Review of Common Competing Oxo-Anions and Tools for Quantifying Selective Adsorption",
volume = "54",
number = "16",
pages = "9769-9790",
doi = "10.1021/acs.est.0c01666"
}

Pincus, L. N., Rudel, H. E., Petrovic, P. V., Gupta, S., Westerhoff, P., Muhich, C. L.,& Zimmerman, J. B.. (2020). Exploring the Mechanisms of Selectivity for Environmentally Significant Oxo-Anion Removal during Water Treatment: A Review of Common Competing Oxo-Anions and Tools for Quantifying Selective Adsorption. in Environmental Science and Technology
ACS Publications., 54(16), 9769-9790.
https://doi.org/10.1021/acs.est.0c01666

Pincus LN, Rudel HE, Petrovic PV, Gupta S, Westerhoff P, Muhich CL, Zimmerman JB. Exploring the Mechanisms of Selectivity for Environmentally Significant Oxo-Anion Removal during Water Treatment: A Review of Common Competing Oxo-Anions and Tools for Quantifying Selective Adsorption. in Environmental Science and Technology. 2020;54(16):9769-9790.
doi:10.1021/acs.est.0c01666 .

Pincus, Lauren N., Rudel, Holly E., Petrovic, Predrag V., Gupta, Srishti, Westerhoff, Paul, Muhich, Christopher L., Zimmerman, Julie B., "Exploring the Mechanisms of Selectivity for Environmentally Significant Oxo-Anion Removal during Water Treatment: A Review of Common Competing Oxo-Anions and Tools for Quantifying Selective Adsorption" in Environmental Science and Technology, 54, no. 16 (2020):9769-9790,
https://doi.org/10.1021/acs.est.0c01666 . .