The study of atomically dispersed metal-nitrogen electrocatalysts is still limited in terms of understanding their catalytic mechanism because of the inability to precisely regulate the coordination number and type of N in combination with the metal elements. Inspired by the high catalytic activity and selectivity of natural enzymes, herein, we have designed and fabricated ultrathin carbon nanosheet-supported Mn single-atom catalysts (SACs) with a precise pyrrole-type Mn-N 4 (PT-MnN 4 ) configuration using a bio-mimicking strategy. The PT-MnN 4 SACs display outstanding oxygen reduction reaction (ORR) activity, with a half-wave potential (E 1/2 ) of 0.88 V (vs. revisible hydrogen electrode [RHE]) and extremely high stability in alkaline media. Moreover, superior ORR activities are also obtained, E 1/2 of 0.73 V and 0.63 V in acid and neutral electrolytes, respectively, indicating the efficient pHuniversal ORR performances. The assembled zinc-air battery using the PT-MnN 4 SACs as air cathodes exhibits a high peak power density (175 mW cm −2 ) and long-term stability up to 150 h, implying its promising application in metal-air batteries. This study has paved the way toward the rational design and precise regulation of single-atom electrocatalysts.

Composites‐based photocatalysis relies on the interfacial electron transfer between the metallic cocatalyst and photosensitizer (the semiconductor) to realize spatial separation of charge carriers. Herein, an ingenious heterojunction between Co‐CN single atom catalysts (SACs) and g‐C3N4 is constructed for heterogeneous photo‐Fenton‐like reactions. Driven by built‐in electric field across the heterojunctions, the separation and migration of the photogenerated charge carriers is promoted, leading to the fast electron transfer from the g‐C3N4 to the Co‐CN SACs. Theoretical calculations and transient absorption spectroscopy reveal the modulated charge transfer and trapping in the SA‐Co‐CN/g‐C3N4 heterostructure, resulting in the remarkably enhanced generation of reactive oxygen species via peroxymonosulfate activation under light irradiation. This ingenious SA‐Co‐CN/g‐C3N4/PMS/vis system is efficient for the oxidation of various antibiotics with high removal efficiency (>98%), a wide operating pH range (pH 3–11) and excellent stability in long‐term operation. This study provides a new tactic for rational design of SACs‐based heterojunctions to bridge photocatalysis and heterogeneous catalysis, attaining superior photoredox activity via interfacial coupling.

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Modulation of Charge Trapping In article number 2208688, Xiaoguang Duan, Xi‐Lin Wu, and co‐workers show here the Chinese legend “Carp jumps over the dragon gate”. The story is about a brave carp swimming upstream, jumping over the ‘dragon gate’, and turning into a powerful dragon. Their cover design is based on this legend, where the carp carriers one electron from g‐C3N4 at the bottom of the waterfall to a single‐atom Co catalyst under the ‘dragon gate’.