Ouyang Jie, Liu Xuan, Wang Bing-Hao, Pan Jin-Bo, Shen Sheng, Chen Lang, Au Chak-Tong, Yin Shuang-Feng
College of Chemistry and Chemical Engineering, State Key Laboratory of Chemo/Biosensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, Hunan University, Changsha 410082, P. R. China.
College of Chemical Engineering, Fuzhou University, Fuzhou 350002, P. R. China.
ACS Appl Mater Interfaces. 2022 May 25;14(20):23536-23545. doi: 10.1021/acsami.2c04608. Epub 2022 May 12.
The photoelectrocatalytic (PEC) oxidation of glycerol into highly value-added products is attractive, but it is extremely challenging to limit the oxidation products to the valuable C3 chemicals. The hole concentration and surface atomic arrangement of a photoanode can be modulated by controlling facet exposure, thus tuning the activity and selectivity. Herein, we report for the first time the formation of a WO photoanode with predominant exposure of {202} facets by a secondary hydrothermal method. The photoanode exhibits superior PEC glycerol conversion efficiency, giving an 80% selectivity to glyceraldehyde with a production rate of 462 mmol h m. Also, the faraday efficiency for the C3 product reaches 98.6%. We made comparison between the {202} facets and the commonly studied {200} facets using experimental and theoretical methods. It is disclosed that the former enhances not only the adsorption and activation of glycerol via the terminal hydroxyl groups but also the desorption of glyceraldehyde.
将甘油光电催化(PEC)氧化为高附加值产品很有吸引力,但将氧化产物限制为有价值的C3化学品极具挑战性。通过控制晶面暴露可以调节光阳极的空穴浓度和表面原子排列,从而调整活性和选择性。在此,我们首次报道了通过二次水热法形成主要暴露{202}晶面的WO光阳极。该光阳极表现出优异的PEC甘油转化效率,对甘油醛的选择性为80%,产率为462 mmol h m。此外,C3产物法拉第效率达到98.6%。我们使用实验和理论方法对{202}晶面和常用的{200}晶面进行了比较。结果表明,前者不仅增强了甘油通过末端羟基的吸附和活化,还增强了甘油醛的脱附。