Electron Reservoir‐Modulated Edge Hosted Sites for Ampere‐Level H 2 O 2 Production and Simultaneous Waste Plastic Upcycling

ABSTRACT The edge‐distributed metal sites are potential for efficient hydrogen peroxide (H 2 O 2 ) electrosynthesis due to their excellent intrinsic activity, but simultaneously achieving high catalytic activity and durability remains challenging. Herein, we propose an electron reservoir strategy by integrating Al‐based nanoclusters to stabilize edge‐hosted Al atomic sites (Al NCs /Al 1 ‐O‐C@edge), enabling efficient H 2 O 2 electrosynthesis at ampere‐level current. The Al NCs /Al 1 ‐O‐C@edge delivers a direct outlet H 2 O 2 concentration of 7.53 wt% and a mass‐normalized production rate reaching 60.1 mol h −1 g cat. −1 at 1.6 A cm −2 . The Al NCs /Al 1 ‐O‐C@edge can be operated at currents of 1–10 A in a 10 × 10 cm 2 reactor, and maintains excellent long‐term stability for 240 h. DFT calculations, durability tests, and in situ analysis demonstrate that the Al‐based nanoclusters act as electron reservoirs, enabling a compressed redox swing of single atom Al centers by regulating the electron accumulation‐release process, which sustains key *OOH intermediate generation. Moreover, coupling H 2 O 2 synthesis with waste plastic upcycling lowers the cell voltage from 7.2 V to 6.1 V at 300 mA cm −2 , while sustaining Faradaic efficiencies above 90% for both H 2 O 2 and glycolic acid production. Techno‐economic analysis reveals a substantially higher revenue for the coupled system than the conventional system, demonstrating its economic and environmental superiority for sustainable chemical co‐production.