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

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 (AlNCs/Al1-O-C@edge), enabling efficient H2O2 electrosynthesis at ampere-level current. The AlNCs/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 gcat. -1 at 1.6 A cm-2. The AlNCs/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.