Adsorption and Surface Complexation Study of L-DOPA on Rutile (α-TiO2) in NaCl Solutions

被引:45
作者
Bahri, Salima [2 ]
Jonsson, Caroline M. [1 ,3 ]
Jonsson, Christopher L. [1 ,3 ]
Azzolini, David [1 ]
Sverjensky, Dimitri A. [1 ,3 ]
Hazen, Robert M. [3 ]
机构
[1] Johns Hopkins Univ, Dept Earth & Planetary Sci, Baltimore, MD 21218 USA
[2] Columbia Univ Barnard Coll, Dept Chem, New York, NY 10027 USA
[3] Carnegie Inst Sci, Geophys Lab, Washington, DC 20015 USA
基金
美国国家科学基金会;
关键词
WATER INTERFACE; OXIDES CONSISTENT; TITANIUM-DIOXIDE; ANION ADSORPTION; INNER-SPHERE; CATECHOL; MEDIA; MODEL; SPECTROSCOPY; SUSPENSIONS;
D O I
10.1021/es1042832
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Dihydroxyphenylalanine (DOPA) and similar molecules are of considerable interest in studies of bioadhesion to minerals, solar cells involving titanium dioxide, and biomedical imaging. However, the extent and mechanisms of DOPA adsorption on oxides in salt solutions are unknown. We report measurements of DOPA adsorption on well-characterized rutile (alpha-TiO2) particles over a range of pH, ionic strength, and surface coverage as well as a surface complexation model analysis establishing the stoichiometry, model surface speciation, and thermodynamic equilibrium constants, which permits predictions in more complex systems. DOPA forms two surface species on rutile, the proportions of which vary strongly with pH but weakly with ionic strength and surface loading. At pH < 4.5 a species involving four attachment points ("lying down") is important, whereas at pH > 4.5 a species involving only two attachment points via the phenolic oxygens ("standing up") predominates. Based on evidence of strong attachment of DOPA to titanium dioxide from single molecule AFM (Lee, H. et al., Proc. Natl. Acad, Sri. 2006, 103, 12999-12003) and studies of catechol adsorption, one or more of the DOPA attachments for each species is inner-sphere, the others are likely to be H-bonds.
引用
收藏
页码:3959 / 3966
页数:8
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