Changes in the Silanol Protonation State Measured In Situ at the Silica-Aqueous Interface

被引：39

作者：

Brown, Matthew A. ^{[1
]}

Huthwelker, Thomas ^{[2
]}

Redondo, Amaia Beloqui ^{[1
]}

Janousch, Markus ^{[2
]}

Faubel, Manfred ^{[3
]}

Arrell, Christopher A. ^{[4
]}

Scarongella, Mariateresa ^{[4
]}

Chergui, Majed ^{[4
]}

van Bokhoven, Jeroen A. ^{[1
,2
]}

机构：

[1] ETH, Inst Chem & Bioengn, CH-8093 Zurich, Switzerland

[2] Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland

[3] Max Planck Inst Dynam & Self Org, D-37073 Gottingen, Germany

[4] Ecole Polytech Fed Lausanne, Lab Ultrafast Spect, CH-1015 Lausanne, Switzerland

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2012年 / 3卷 / 02期

关键词：

SURFACE-CHEMISTRY; XPS; QUARTZ; XANES; SPECTROSCOPY; EXISTENCE; DELIVERY; EDGE;

D O I：

10.1021/jz201533w

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Recent nanomedical applications have again highlighted the significance of silica surface chemistry in solution. Here, we report in situ electronic structure measurements at the silica-aqueous interface as a function of pH for nanoparticles (NPs) of 7, 12, and 22 nm using a liquid microjet in combination with synchrotron radiation. The Si K-edge X-ray absorption near-edge spectroscopy (XANES) spectra reveal a change in shape of the Si 1s -> t(2) (Si 2p-3s) absorption brought about by changes in the silanol protonation state at the interface of the NPs as a result of changes in solution pH. Our results are consistent with the number of silanol groups changing the protonation state being inversely correlated with the SiO2 NP size. The importance of in situ studies is also demonstrated by comparing the XANES spectra of aqueous 7 nm SiO2 with the same dehydrated sample in vacuum.

引用

页码：231 / 235

页数：5

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