Zhai Mianmian, Zhang Yu, Xu Jixiang, Lin Haifeng, Xing Jun, Wang Lei
Key Laboratory of Eco-chemical Engineering, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, Qingdao University of Science and Technology, Qingdao 266042, China; College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
Key Laboratory of Eco-chemical Engineering, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, Qingdao University of Science and Technology, Qingdao 266042, China; College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
J Colloid Interface Sci. 2024 Nov;673:267-274. doi: 10.1016/j.jcis.2024.06.092. Epub 2024 Jun 11.
Catalysts composed of nanocluster and single-atom (SA) were extensively used to enhance electrocatalytic water splitting performance, whereas study of their photocatalytic hydrogen (H) evolution activity was limited. Herein, carbon nitride (CN) decorated by ruthenium (Ru) cocatalysts existed as SA + cluster, cluster + nanoparticles (NPs), and NPs were prepared by impregnation and calcination processes. The correlation between existential form, content of Ru cocatalyst and H evolution rate were carefully discussed. It was found that Ru NPs were favor for water molecule adsorption, whereas Ru SAs and clusters facilitated H desorption. Theoretical calculations revealed that Ru clusters + NPs cocatalyst were beneficial for H* intermediate formation. Water splitting tests found that 1.07 wt% Ru NPs + cluster modified CN showed the highest H evolution rate of 13.64 mmol h g, which was 266.4 and 1.5 times higher than those of CN and Ru NPs (2.33 wt%) decorated CN, respectively. This work deeply reveals the influences of existential form of Ru cocatalysts on photocatalytic water splitting of CN, and provides thought in designing new cocatalysts to largely enhance H evolution.
由纳米团簇和单原子（SA）组成的催化剂被广泛用于提高电催化析氢性能，而对其光催化析氢活性的研究却很有限。在此，由钌（Ru）助催化剂修饰的氮化碳（CN）以SA + 团簇、团簇 + 纳米颗粒（NPs）的形式存在，且NPs通过浸渍和煅烧过程制备。详细讨论了Ru助催化剂的存在形式、含量与析氢速率之间的关系。研究发现，Ru NPs有利于水分子吸附，而Ru SAs和团簇则促进氢脱附。理论计算表明，Ru团簇 + NPs助催化剂有利于H*中间体的形成。析氢测试发现，1.07 wt% Ru NPs + 团簇修饰的CN表现出最高的析氢速率，为13.64 mmol h g，分别是CN和Ru NPs（2.33 wt%）修饰的CN的266.4倍和1.5倍。这项工作深入揭示了Ru助催化剂的存在形式对CN光催化析氢的影响，并为设计新型助催化剂以大幅提高析氢性能提供了思路。
