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However, conventional SACs typically exhibit a symmetric electron density distribution, which leads to poor adsorption\/desorption and activation of reaction intermediates and thus limits catalytic efficiency. In this study, we designed and synthesized a novel spatially asymmetric SACs through ligand steric hindrance engineering, which involves the post\u2011synthetic introduction of a bulky, conformationally constrained ligand of 2,2\u2019:6\u2019,2\u2033\u2010terpyridine (Tpy), into a vinylene\u2010linked covalent organic framework pre\u2011anchored with single Co atoms, thereby creating a non\u2011planar, asymmetric coordination environment around the Co center to afford COF\u2011Co\u2011Tpy. Unlike SACs with planar or spatially symmetric structures, COF\u2010Co\u2010Tpy possesses a spatially asymmetric structure imparted by the terpyridine moiety, which not only induces a low\u2010spin state at the Co center, but also creates a unique reaction microenvironment where intermediates are adsorbed at the Co sites perpendicular to the mass transfer direction. The synergistic effect significantly reduces the adsorption energy barrier of the *OH intermediates. Consequently, COF\u2010Co\u2010Tpy exhibits remarkable oxygen reduction reaction (ORR) performance with a half\u2010wave potential up to 0.90\u00a0V, and its intrinsic catalytic activity is 22.46 and 6.15 times higher than those of planarly and spatially symmetric SACs, respectively.<\/jats:p>","DOI":"10.1002\/anie.5047569","type":"journal-article","created":{"date-parts":[[2026,8,31]],"date-time":"2026-08-31T05:09:46Z","timestamp":1788152986000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ligand Steric Hindrance\u2010Engineered Spatially Asymmetric Single\u2010Atom Catalysts: A New Platform for Electrochemical Oxygen Reduction"],"prefix":"10.1002","volume":"65","author":[{"given":"Kai","family":"Cui","sequence":"first","affiliation":[{"name":"State Key Laboratory of Natural Product Chemistry, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering Lanzhou University  Lanzhou P. 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