Xie Ruyu, Li Kaitao, Tian Rui, Lu Chao
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology Beijing 100029 China
Quzhou Institute for Innovation in Resource Chemical Engineering Quzhou 324000 China.
Chem Sci. 2024 Oct 7;15(43):18085-92. doi: 10.1039/d4sc03763d.
Catalytic activities of single-atom catalysts are strongly dependent on their d-band centers. However, it is a long-standing challenge to provide a cost-effective and accurate evaluation for the positions of d-band centers of these catalysts due to the fact that the widely applicable photoelectron spectroscopy methodologies require complicated sampling and spectral unfolding processes. In this contribution, we have proposed oxygen intermediate-boosted electrochemiluminescence (ECL) for rapid spotting of the d-band centers of single-atom catalysts, involving single atomic Au, Ag, Cu and Fe. It was disclosed that the d-band centers of single-atom catalysts closer to the Fermi level could facilitate the interaction between catalysts and oxygen intermediates, leading to higher luminol ECL intensities as a result of the promoted adsorption and reduction ability towards oxygen intermediates. Moreover, this correlation was also adapted for other metal catalysts such as Au and Ag nanoparticles. This correspondence could be utilized for an accurate identification of d-band centers of single-atom catalysts. It is anticipated that the proposed strategy could be beneficial for a deep understanding of microstructure studies of single-atom catalysts to achieve advanced catalytic performances.
单原子催化剂的催化活性强烈依赖于其d带中心。然而，由于广泛应用的光电子能谱方法需要复杂的采样和光谱解卷积过程，因此为这些催化剂的d带中心位置提供经济高效且准确的评估一直是一项长期挑战。在本论文中，我们提出了氧中间体增强电化学发光（ECL）方法，用于快速测定单原子催化剂（包括单原子Au、Ag、Cu和Fe）的d带中心。结果表明，单原子催化剂的d带中心越接近费米能级，越能促进催化剂与氧中间体之间的相互作用，由于对氧中间体的吸附和还原能力增强，导致鲁米诺ECL强度更高。此外，这种相关性也适用于其他金属催化剂，如Au和Ag纳米颗粒。这种对应关系可用于准确识别单原子催化剂的d带中心。预计所提出的策略将有助于深入理解单原子催化剂的微观结构研究，以实现先进的催化性能。
