一种用于同时产氢以及将苯甲醇选择性氧化为苯甲醛的二元哑铃状可见光驱动光催化剂。
A binary dumbbell visible light driven photocatalyst for simultaneous hydrogen production with the selective oxidation of benzyl alcohol to benzaldehyde.
作者信息
Tayyab Muhammad, Mansoor Seemal, Akmal Zeeshan, Khan Mazhar, Zhou Liang, Lei Juying, Zhang Jinlong
机构信息
Key Laboratory for Advanced Materials, Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, PR China; Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, Guangdong 518055, PR China.
Key Laboratory for Advanced Materials, Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, PR China.
出版信息
J Colloid Interface Sci. 2024 Jul;665:911-921. doi: 10.1016/j.jcis.2024.03.190. Epub 2024 Mar 29.
Photocatalytic H production with selective oxidation of organic moieties in an aqueous medium is a fascinating research area. However, the rational design of photocatalysts and their photocatalytic performance are still inadequate. In this work, we efficiently synthesized the MoS tipped CdS nanowires (NWs) photocatalyst using soft templates via the two-step hydrothermal method for efficient H production with selective oxidation of benzyl alcohol (BO) under visible light illumination. The optimized MoS tipped CdS NWs (20 % MoS) photocatalyst exhibits the highest photocatalytic H production efficiency of 13.55 mmol g h with 99 % selective oxidation of BO, which was 42.34 and 2.21 times greater photocatalytic performance than that of pristine CdS NWs and MoS/CdS NWs, respectively. The directional loading of MoS at the tips of CdS NWs (as compared to nondirectional MoS at CdS NWs) is the key factor towards superior H production with 99 % selective oxidation of BO and has an inhibitory effect on the photo corrosion of pristine CdS NWs. Therefore, the amazing enhancement in the photocatalytic performance and selectivity of optimized MoS tipped CdS NWs (20 % MoS) photocatalyst is due to the spatial separation of their photoexcited charge carriers through the Schottky junction. Moreover, the unique structure of the MoS flower at the tip of 1D CdS NWs offers separate active sites for adsorption and surface reactions such as H production at the MoS flower (confirmed by Pt photo deposition) and subsequently the selective oxidation of BO at the stem of CdS NWs. This rational design of a photocatalyst could be an inspiring work for the further development of an efficient photocatalytic system for H production with selective oxidation of BO (a strategy of mashing two potatoes with one fork).
在水介质中通过光催化产氢并选择性氧化有机部分是一个引人入胜的研究领域。然而，光催化剂的合理设计及其光催化性能仍显不足。在这项工作中，我们通过两步水热法，使用软模板高效合成了MoS包覆的CdS纳米线（NWs）光催化剂，用于在可见光照射下通过选择性氧化苯甲醇（BO）高效产氢。优化后的MoS包覆的CdS NWs（20% MoS）光催化剂表现出最高的光催化产氢效率，为13.55 mmol g⁻¹ h⁻¹，对BO的选择性氧化率为99%，其光催化性能分别是原始CdS NWs和MoS/CdS NWs的42.34倍和2.21倍。与CdS NWs上无定向的MoS相比，MoS在CdS NWs尖端的定向负载是实现99% BO选择性氧化并实现卓越产氢的关键因素，并且对原始CdS NWs的光腐蚀具有抑制作用。因此，优化后的MoS包覆的CdS NWs（20% MoS）光催化剂在光催化性能和选择性方面的惊人提升归因于其光激发载流子通过肖特基结的空间分离。此外，一维CdS NWs尖端的MoS花的独特结构为吸附和表面反应提供了独立的活性位点，例如在MoS花处产氢（通过Pt光沉积证实），随后在CdS NWs的茎部对BO进行选择性氧化。这种光催化剂的合理设计对于进一步开发用于通过选择性氧化BO产氢的高效光催化系统可能是一项鼓舞人心的工作（一种一举两得的策略）。
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