Chen Xiang, Guan Shuhui, Zhou Jianjiang, Shang Hengjun, Zhang Jingyuan, Lv Fujian, Yu Han, Li Hexing, Bian Zhenfeng
MOE Key Laboratory of Resource Chemistry and Shanghai Key Laboratory of Rare Earth Functional Materials, Shanghai Normal University, Shanghai, 200234, China.
College of Chemistry and Environmental Science, Qujing Normal University, Qujing, 655400, China.
Angew Chem Int Ed Engl. 2023 Nov 6;62(45):e202312734. doi: 10.1002/anie.202312734. Epub 2023 Sep 28.
Single-atom catalysts (SACs) have emerged as crucial players in catalysis research, prompting extensive investigation and application. The precise control of metal atom nucleation and growth has garnered significant attention. In this study, we present a straightforward approach for preparing SACs utilizing a photocatalytic radical control strategy. Notably, we demonstrate for the first time that radicals generated during the photochemical process effectively hinder the aggregation of individual atoms. By leveraging the cooperative anchoring of nitrogen atoms and crystal lattice oxygen on the support, we successfully stabilize the single atom. Our Pd /TiO catalysts exhibit remarkable catalytic activity and stability in the Suzuki-Miyaura cross-coupling reaction, which was 43 times higher than Pd/C. Furthermore, we successfully depose Pd atoms onto various substrates, including TiO , CeO , and WO . The photocatalytic radical control strategy can be extended to other single-atom catalysts, such as Ir, Pt, Rh, and Ru, underscoring its broad applicability.
单原子催化剂(SACs)已成为催化研究中的关键角色,引发了广泛的研究和应用。金属原子成核和生长的精确控制已引起了极大关注。在本研究中,我们提出了一种利用光催化自由基控制策略制备单原子催化剂的简单方法。值得注意的是,我们首次证明了光化学过程中产生的自由基有效地阻碍了单个原子的聚集。通过利用氮原子和晶格氧在载体上的协同锚定作用,我们成功地稳定了单原子。我们的Pd/TiO催化剂在铃木-宫浦交叉偶联反应中表现出显著的催化活性和稳定性,比Pd/C高43倍。此外,我们成功地将Pd原子沉积到各种基底上,包括TiO、CeO和WO。光催化自由基控制策略可以扩展到其他单原子催化剂,如Ir、Pt、Rh和Ru,突出了其广泛的适用性。