Recently, a research team led by Prof. Wang Jinlan and Prof. Ling Chongyi from the School of Physics, SEU, has made significant progress in studying the structure–

performance relationship of single-atom catalysts (SACs). The related findings were published in Angewandte Chemie International Edition, one of the top international 

chemistry journals, with the title of “Beyond Local Coordination: How Global Structure Governs the Selectivity of Single Atom Catalysts for CO? Reduction.”

The principle that “structure determines properties” is fundamental to material design and optimization. Based on this principle, the local structure of a catalyst—particularly 

the geometric and electronic characteristics of the active site—has long been regarded as the key factor determining catalytic performance. However, in complex catalytic 

systems, performance often deviates from what local-structure-based predictions would suggest: even with similar active sites, performance can differ drastically. Taking the 

CO? reduction reaction as an example, experiments have shown that two types of single-atom catalysts with identical CoN? active centers—nitrogen-doped carbon-

supported Co single-atom catalysts (CoNC) and phthalocyanine-supported Co single-atom catalysts (CoPc)—exhibit completely different product selectivity. Specifically, CoPc

tends to produce CO, whereas CoNC mainly generates H?. This phenomenon highlights the limitations of local structural descriptions and underscores the urgent need for a 

new theoretical framework that incorporates global structural effects to fully elucidate the regulatory mechanisms of catalytic performance.

To address this issue, the team combined constantpotential density functional theory with ab-initio molecular dynamics simulations to systematically investigate the electronic 

structures and interfacial behaviors of CoNC and CoPc. The results show that although the geometric and electronic structures of their local active centers are very similar, 

differences in overall structural environments significantly affect the catalyst’s potential of zero charge (PZC) and interfacial charge distribution, thereby modulating electron

carrying capacity and the orientation of interfacial water molecules. These differences ultimately lead to completely opposite selectivity in the CO? reduction reaction. Further 

studies also revealed that the strength of the “global structure effect” depends on the sensitivity of the local active site to overall structural changes. This work exposes the 

limitations of the “l(fā)ocal structure alone determines catalytic performance” paradigm and proposes a new strategy for tuning catalytic selectivity by engineering the global 

structure of the support (e.g., introducing carbon vacancies), offering fresh insights for the rational design of singleatom catalysts.

The first author of the paper is Dr. Cui Yu from SEU, with Prof. Wang Jinlan and Prof. Ling Chongyi from the School of Physics, SEU, serving as corresponding authors. This 

research was supported by the National Key R&D Program of China, the National Natural Science Foundation of China (Key and Excellent Young Scholar Projects), among 

other funding sources.

Source: School of Physics, SEU

Tranlated by: Melody Zhang

Proofread by: Gao Min

Edited by: Li Xinchang