TY - JOUR
T1 - Second-harmonic generation and theoretical studies of protonation at the water/α-TiO2 (1 1 0) interface
AU - Fitts, Jeffrey P.
AU - MacHesky, Michael L.
AU - Wesolowski, David J.
AU - Shang, Xiaoming
AU - Kubicki, James D.
AU - Flynn, George W.
AU - Heinz, Tony F.
AU - Eisenthal, Kenneth B.
N1 - Funding Information:
We acknowledge I. Stiopkin for the design and construction of the SHG experimental cell. This work was sponsored jointly by National Science Foundation and the Division of Chemical Science, Office of Basic Energy Sciences of the Department of Energy under Grant No. 9810367 to the Environmental Molecular Science Institute at Columbia University, by NSF CHE-0400417, by Chemical Sciences, Geosciences and Biosciences Division and the Catalysis Science Program (Grant DE-FG03-03ER15463), Office of Basic Energy Sciences, Office of Science of US DOE, and by US DOE Office of Basic Energy Sciences project ‘Nanoscale Complexity at the Oxide/Water Interface’ (ERKCC41).
PY - 2005/8/15
Y1 - 2005/8/15
N2 - The pH of zero net surface charge (pHpzc) of the α-TiO2 (1 1 0) surface was characterized using second-harmonic generation (SHG) spectroscopy. The SHG response was monitored during a series of pH titrations conducted at three NaNO3 concentrations. The measured pHpzc is compared with a pHpzc value calculated using the revised MUltiSIte Complexation (MUSIC) model of surface oxygen protonation. MUSIC model input parameters were independently derived from ab initio calculations of relaxed surface bond lengths for a hydrated surface. Model (pHpzc 4.76) and experiment (pHpzc 4.8 ± 0.3) agreement establishes the incorporation of independently derived structural parameters into predictive models of oxide surface reactivity.
AB - The pH of zero net surface charge (pHpzc) of the α-TiO2 (1 1 0) surface was characterized using second-harmonic generation (SHG) spectroscopy. The SHG response was monitored during a series of pH titrations conducted at three NaNO3 concentrations. The measured pHpzc is compared with a pHpzc value calculated using the revised MUltiSIte Complexation (MUSIC) model of surface oxygen protonation. MUSIC model input parameters were independently derived from ab initio calculations of relaxed surface bond lengths for a hydrated surface. Model (pHpzc 4.76) and experiment (pHpzc 4.8 ± 0.3) agreement establishes the incorporation of independently derived structural parameters into predictive models of oxide surface reactivity.
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U2 - 10.1016/j.cplett.2005.03.152
DO - 10.1016/j.cplett.2005.03.152
M3 - Article
AN - SCOPUS:22944479601
SN - 0009-2614
VL - 411
SP - 399
EP - 403
JO - Chemical Physics Letters
JF - Chemical Physics Letters
IS - 4-6
ER -