Al‐Induced Cu 2+ ‐Cu + Polarization in Ampere‐Level Waste‐Treating‐Waste Electrocatalysis for Concurrent CO 2
Feng Ming Yap, Jian Yiing Loh, Elton Song‐Zhe Mah, Shaoyu Yuan, Xianhai Zeng, Wee‐Jun OngABSTRACT
This study introduces a pair‐electro‐reforming strategy that integrates polyethylene terephthalate (PET) upcycling with CO 2 reduction, enabling the concurrent generation of value‐added chemicals under energy‐efficient conditions. Central to this study is the self‐supported AlCuIn nanorod/N‐doped graphene oxide (ACI/NG) electrocatalyst, synthesized via a dual‐hydrothermal approach. The strategic incorporation of Al induces a strong Cu 2+ ‐to‐Cu + polarization effect, significantly enhancing catalytic activation by optimizing the *CO interaction, thereby promoting efficient CO 2 ‐to‐C 2 conversion. This polarization‐driven enhancement enables tunable product selectivity, achieving faradaic efficiencies (FE) of 91.2% for C 1 products (CI/NG) and 93.8% for C 2 products (ACI/NG). Furthermore, the system demonstrates ampere‐level performance, maintaining a high current density of −0.65 A cm −2 for over 100 h. PET hydrolysate oxidation proceeds with nearly 100% selectivity toward formic acid, highlighting its efficacy in electrochemical valorization. DFT analysis and in‐situ spectroscopy reveal *CO dimerization and key intermediate formation, offering mechanistic insights into polarization‐enhanced catalysis. Moreover, a solar‐powered CO 2 RR||PET hydrolysate oxidation system achieves η STF values of 17.01% and 16.31%, ensuring operational stability. Ultimately, this work provides a scalable, energy‐efficient platform for waste‐treating CO 2 and plastic waste, advancing sustainable electrocatalysis.