Electron Reservoir-Modulated Edge Hosted Sites for Ampere-Level H₂O₂ Production and Simultaneous Waste Plastic...

The edge-distributed metal sites are potential for efficient hydrogen peroxide (H₂O₂) 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/Al₁-O-C@edge), enabling efficient H₂O₂ electrosynthesis at ampere-level current. The Al_NCs/Al₁-O-C@edge delivers a direct outlet H₂O₂ 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/Al₁-O-C@edge can be operated at currents of 1-10 A in a 10 × 10 cm² 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 H₂O₂ 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 H₂O₂ 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.