环境科学进展.pptVIP

Dynamics of photogenerated electrons in anatase/rutile catalysts photoexcited by 370 nm pump pulses 4:1anatase/rutile 10:1 anatase/rutile 40:1anatase/rutile at 1400 nm at 1400 nm at 1400 nm 1:1anatase/rutile rutile amount percentage of fast trapping process at 1400 nm Photocatalytic activity of TiO2 powder evaluated with degradation of MB effect of rutile in extending the photoactive range electron transfer from rutile to anatase Electron transfer in anatase/rutile catalyst Summary Electron transfer: Rutile Anatase 100 fs Different electron density Driving force: hv hv anatase rutile Electron transfer in anatase/rutile catalyst 谢谢大家！ * * 光催化是复杂过程，对其机理的认识非常有限 * Normalized transient profiles of average IR absorption of Pt/TiO2 (0.1 wt.%), Pt/TiO2 (1.0 wt.%) when the pretreated samples were exposed to ~ 20 Torr CH3OH the long-lived electrons in Pt/TiO2-200 (0.1-1.0 wt%) catalysts decay faster than those in Pt/TiO2-400 (0.1-1.0 wt%) catalysts when the Pt load- ing amount is the same * 甲醇吸附物种快速捕获空穴 Yoshiaki Tamaki, Akihiro Furube,* Miki Murai, Kohjiro Hara, Ryuzi Katoh, and M. Tachiya， JACS, 2005 Pt-TiO2 催化剂上光催化重整甲醇制氢反应机理研究 金红石-锐钛矿之间的电子转移过程研究 甲醇在TiO2及Pt/TiO2-400 (0.5wt.%)上吸附的红外光谱 两种吸附物种：CH3OH（a)和CH3O(a) 甲醇在Pt/TiO2-200样品上吸附的红外光谱图 甲醇在Pt/TiO2-400样品上吸附的红外光谱图 高温H2还原制得的Pt/TiO2样品中Pt原子占据TiO2表面活性位置 甲醇吸附随Pt担载量的变化 TiO2样品上吸附甲醇后经5 Hz、70 mW 355 nm 脉冲光照不同时间所得光照后与光照前的红外差谱图 TiO2样品上吸附甲醇和水后经5 Hz、70 mW 355 nm 脉冲光照不同时间所得光照后与光照前的红外差谱图 Pt/TiO2-400(0.5 wt.%)样品上吸附甲醇后经5 Hz、70 mW 355 nm 脉冲光照不同时间所得光照后与光照前的红外差谱图 Pt/TiO2-400(0.5 wt.%)样品上吸附甲醇和水后经5 Hz、70 mW 355 nm 脉冲光照不同时间所得光照后与光照前的红外差谱图 表面物种CH2O(a), CH2OO(a), HCOO(a) 等被观察到 担载Pt及添加水气显著促进该光催化反应 增加甲醇蒸气也能明显加快该光催化反应 HCOO(a)相对量随光照时间的变化曲线 及产氢表观量子效率 CH3OH → CH3O-(a) + H+ CH3O-(a) + h+ → CH3O·(a) CH3O·(a) + h+ → CH2O(a) + H+ …… H+ + e- → 1/2 H2 推测甲醇在Pt/TiO2样品上光催化制氢反应的可能机理 Pt 真空条件下Pt/TiO2-400 (0.2 wt.%)样品的时间分辨红外差谱图 不同条件下Pt/TiO2-400 (0.2 wt.%)中光生电子的衰减动力学曲线 CB hv e- e- e-