Molecular hydrogen formation from photocatalysis of methanol on TiO2(110).
Molecular hydrogen formation from photocatalysis of methanol on TiO2(110).
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DOI：
10.1021/ja4030963
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发表时间：
2013-07
影响因子：
15
通讯作者：
Chenbiao Xu;Wenshao Yang;Qing Guo;D. Dai;Maodu Chen;Xueming Yang
中科院分区：
文献类型：
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作者：
Chenbiao Xu;Wenshao Yang;Qing Guo;D. Dai;Maodu Chen;Xueming Yang
众所周知，在水中加入甲醇可以显著提高二氧化钛的产氢能力。最近，我们发现在400 nm波长下，甲醇在二氧化钛(110)表面上可以通过分步反应机制被光催化分解。然而，光催化的甲醇/二氧化钛(110)表面如何生成分子氢还不清楚。在这项工作中，我们用程序升温脱附(TPD)技术研究了在400 nm波长下，在TiO2光催化下，全氢甲醇(CD3OD)在TiO2光催化剂上生成重氢的反应。检测到光催化分解产物甲醛(CD2O)和BBO上的D-原子(通过D2O TPD产物)。除了通过加热光催化的甲醇/二氧化钛(110)表面生成D2O外，我们还观察到D2产物的生成。D2显然是通过光催化甲醇的BBO位上的D-原子热复合而形成的。实验结果表明，D2O的生成比D2的生成更重要，D2的生成明显受D2O生成过程的影响。
It is well established that adding methanol to water could significantly enhance H2 production by TiO2. Recently, we have found that methanol can be photocatalytically dissociated on TiO2(110) at 400 nm via a stepwise mechanism. However, how molecular hydrogen can be formed from the photocatalyzed methanol/TiO2(110) surface is still not clear. In this work, we have investigated deuterium formation from photocatalysis of the fully deuterated methanol (CD3OD) on TiO2(110) at 400 nm using a temperature programmed desorption (TPD) technique. Photocatalytic dissociation products formaldehyde (CD2O) and D-atoms on BBO sites (via D2O TPD product) have been detected. In addition to D2O formation by heating the photocatalyzed methanol/TiO2(110) surface, we have also observed D2 product formation. D2 is clearly formed via thermal recombination of the D-atoms on the BBO sites from photocatalysis of methanol. Experimental results indicate that D2O formation is more important than D2 formation and that D2 formation is clearly affected by the D2O formation process.