Thermal coupled photoconductivity as a tool to understand the photothermal catalytic reduction of CO2  

利用光热耦合下的光电导研究TiO2光热催化还原CO2（英文）

作　　者：Dashuai Li Yu Huang Songmei Li Changhua Wang Yingying Li Xintong Zhang Yichun Liu 李大帅;黄誉;李松美;王长华;李莹莹;张昕彤;刘益春(东北师范大学紫外光发射材料与技术教育部重点实验室)

机构地区：[1]Key Laboratory of UV-Emitting Materials and Technology of Chinese Ministry of Education,Northeast Normal University,Changchun 130024,Jilin,China

出　　处：《Chinese Journal of Catalysis》2020年第1期154-160,共7页催化学报（英文）

基　　金：supported by the Natural Science Foundation of China(51072032,51372036,51102001);the Key Project of Chinese Ministry of Education(113020A);the 111 project(B13013);Jilin Province Science and Technology Development Plan(20180101175JC,20160520170JH)~~

摘　　要：Photocatalysis shows great promise in the field of solar energy conversion.One of the reasons for this is because it promotes the development of multi-field-coupled catalysis.In order to explore the principles of multi-field-coupled catalytic reactions,an in situ multi-field-coupled characterization technique is required.In this study,we obtained hydrogenated ST-01 TiO2 and observed enhanced catalytic activity by thermal coupled photocatalysis.In situ photoconductivity was employed to understand the activity enhancement.The effects of the reaction temperature,reaction atmosphere,and oxygen vacancy(Ov)on the photoconductivity of TiO2 were studied.After coupling thermal into photoconductivity measurement,highly active Ov-TiO2 displayed rapid decay of photoconductivity in a CO2 atmosphere and slow decay of photoconductivity in a N2 atmosphere.These phenomena revealed that photothermal coupling assisted the detrapping of electrons at the Ov surface and promoted electron transfer to CO2,which clearly explained the high photothermal catalytic activity of Ov-TiO2.This study demonstrated that photoconductivity is a useful tool to help understand photothermal catalytic phenomena.利用太阳能缓解能源危机和解决环境污染,是当前和未来的全球性课题.其中,光催化技术的研究步伐日渐加快.这不仅体现在光催化材料种类的增加,更体现在以光催化为基础的多场协同催化,特别是光热耦合作用成为增强光催化性能的一种高效、可靠的方法.氧空位的引入不仅可以拓宽催化剂对可见光的吸收、抑制载流子的复合、促进反应物的吸附以及降低反应的活化能,而且对于光热协同催化效率的提升有着重要的贡献.然而,目前光热协同催化的表征多局限于常规的光催化手段.开展光热耦合下的测量技术对深刻理解光热催化是十分必要的.本文研究温度、气氛、氧空位浓度对TiO2光电导的影响,构建光电导与光热催化活性之间的关系.我们将商用的ST-01 TiO2制成浆料,利用丝网印刷法将浆料覆盖在刻有沟槽的FTO上,并通过N2/H2混合气不同温度退火,得到不同氧空位含量的TiO2薄膜(Ov-TiO2).采用紫外-可见光谱(UV-Vis),拉曼光谱(Raman),电子顺磁共振(ESR)等手段对样品进行了表征.结果表明,N2/H2退火温度越高,氧空位浓度越高.我们对不同浓度氧空位的样品进行了光催化及光热协同催化CO2还原实验.结果表明,适量氧空位的样品(H2-150)光催化还原CO2性能最差,但光热协同催化还原CO2的性能最佳.我们对其光电导值的衰减情况进行了分析,看到H2-150样品在CO2气氛、光热条件下,电导衰减加快.由于光电导的衰减是由电荷复合和电荷参与的表面反应共同决定的,为确定是哪一因素决定了电导的衰减,我们进一步测试了H2-150样品在N2气氛下的电导衰减情况.结果发现,H2-150样品在N2气氛、光热条件下电导衰减反而变慢.这表明,造成H2-150样品在CO2气氛、光热条件下的电导衰减加快是光热条件下CO2还原速率加快,也验证了H2-150具有较好的光热催化CO2活性.与H2-150样品不同的是,大量氧空位样品

关 键 词：PHOTOCONDUCTION Photothermalcatalytic Titanium dioxide Oxygen vacancy Carbon dioxide reduction 

分 类 号：O64[理学—物理化学]