Stabilizing Cu ⁰ ─Cu ^δ+ Active Centers via Strong Metal–Support Interaction Enforced Intermetallic Cu ₃ Pt‐Cu Heterointerfaces for Self–Powered Waste to Wealth Catalysis

ABSTRACT Developing a self–sustained catalytic system capable of transforming chemical wastes into useful fuels and chemicals represents a vital step toward sustainable energy conversion. Herein, we design strong metal–support interaction (SMSI) enforced intermetallic Cu 3 Pt‐Cu heterointerface that stabilize Cu 0 –Cu δ+ active centers by enabling ohmic contact and interfacial charge coupling. The formation of heterointerface of Cu 3 Pt‐Cu and coexistence of Cu 0 ─Cu δ+ dual states were directly evidenced by XAFS analysis, where wavelet transform contour plots revealed Cu─Cu and Cu─Pt scattering features alongside weak Cu–O features indicative of controlled partial oxidation of the Cu core. The stabilized Cu 0 ─Cu δ+ interfaces facilitate gem–diol mediated furfural oxidation and selective nitrate reduction by bidirectional H * regulation. The “Furfural–Nitrate” coupled self–powered galvanic cell was efficiently actuated by Cu 3 Pt‐Cu/CF bifunctional catalyst. The constructed cell achieves a near–theoretical open–circuit voltage of ∼0.76 V and record peak power density (19.31 mW cm −2 ) while producing NH 3 (FE 59.9%), H 2 (FE 72.1%), and furoic acid (FE 79.5%), yielding 12.13 kWh kg −1 electricity. This work establishes a strategy to tune interfacial electronic interactions via SMSI for kinetic–promoted electrocatalysis, achieving a benchmark for the innovative hydrogen–ammonia co–production system with simultaneous electricity generation.