Designer topological-single-atom catalysts with site-specific selectivity

作者：Weibin Chen, Menghui Bao, Fanqi Meng, Bingbing Ma, Long Feng, Xuan Zhang, Zanlin Qiu, Song Gao, Rui‐Qin Zhong, Shibo Xi, Xiao Hai, Jiong Lu, Ruqiang Zou · 发表于：Nature Communications · 年份：2025 · DOI：10.1038/s41467-025-55838-6 · 被引用次数：38 · 研究领域：Catalytic Processes in Materials Science、Electrocatalysts for Energy Conversion、Catalysis and Oxidation Reactions

Designing catalysts with well-defined, identical sites that achieve site-specific selectivity, and activity remains a significant challenge. In this work, we introduce a design principle of topological-single-atom catalysts (T-SACs) guided by density functional theory (DFT) and Ab initio molecular dynamics (AIMD) calculations, where metal single atoms are arranged in asymmetric configurations that electronic shield topologically misorients d orbitals, minimizing unwanted interactions between reactants and the support surface. Mn1/CeO2 catalysts, synthesized via a charge-transfer-driven approach, demonstrate superior catalytic activity and selectivity for NOx removal. A life-cycle assessment (LCA) reveals that Mn1/CeO2 significantly reduces environmental impact compared to traditional V-W-Ti catalysts. Through in-situ spectroscopic characterizations combined with DFT calculations, we elucidate detailed reaction mechanisms. This study establishes T-SACs as a promising class of catalysts, offering a systematic framework to address catalytic challenges by defining site characteristics. The concept highlights their potential for advancing selective catalytic processes and promoting sustainable technologies. Designing catalysts with uniform, site-specific selectivity and activity is a significant challenge. This study introduces design principles for topological-single-atom catalysts that utilize electronic shielding to protect surfaces and control reaction pathways, achieving high...