Designer topological-single-atom catalysts with site-specific selectivity
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
Abstract
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 selectivity without compromising activity.