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[交流] 采用同位素標(biāo)記法探測(cè)TiO2光催化體系水相降解苯環(huán)開環(huán)機(jī)理

中科院北京化學(xué)所趙進(jìn)才院士最近JACS ——采用同位素標(biāo)記法探測(cè)TiO2光催化體系水相降解苯環(huán)開環(huán)機(jī)理
Determining the TiO2‑Photocatalytic Aryl-Ring-Opening Mechanism
in Aqueous Solution Using Oxygen-18 Labeled O2 and H2O

采用同位素標(biāo)記O2，H2O，一對(duì)叔丁基鄰苯二酚為模型，在TiO2，水：乙腈=1:1比例溶劑中，研究芳香環(huán)開環(huán)產(chǎn)物。
首次獲得了分子氧O2中O原子插入苯環(huán)C-C鍵的直接證據(jù)。這說明了分子氧O2是芳香烴開環(huán)的反應(yīng)劑。

The molecules O2 and H2O dominate the cleavage of aromatic sp2 C −C bonds, a crucial step in the degradation
of aromatic pollutants in aqueous TiO2 photocatalysis, but their precise roles in this process have remained elusive.
This can be attributed to the complex oxidative species involved and to a lack of available models for reactions
with a high yield of direct products. Here, we used oxygen-18 isotope labeled O2 and H2O to observe the aromatic
ring-opening reaction of the model compound 3,5-di-tert-butylcatechol(DTBC), which was mediated by TiO2
photocatalysis in an aqueous acetonitrile solution. By analyzing the primary intermediate products ( ～75% yield),
especially the seven-membered ring anhydrides that were formed, we obtained direct evidence for the oxygen
atom of dioxygen insertion into a C −C bond of the aromatic ring. This indicates that molecular oxygen is the ultimate
ring-opening agent in TiO2 photocatalysis and that it undergoes single O atom incorporation rather than the previously
proposed molecular oxygen 1,2-addition processes. The ratio of intradiol to extradiol products depends on the particle
size of TiO2 catalysts used, which suggests that the O2 activation is correlated with the available coordination sites on
the TiO2 surface in the photocatalytic cleavage of the aromatic ring.

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采用同位素標(biāo)記法探測(cè)TiO2光催化體系水相降解苯環(huán)開環(huán)機(jī)理-1

2.png

采用同位素標(biāo)記法探測(cè)TiO2光催化體系水相降解苯環(huán)開環(huán)機(jī)理-2

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采用同位素標(biāo)記法探測(cè)TiO2光催化體系水相降解苯環(huán)開環(huán)機(jī)理-3

4.png

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附件 1 : ja5031936.pdf

2015-03-12 15:06:03, 2.28 M

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