- Bipolar electrocatalytic pairing of anodic phenol oxidation with cathodic p-nitrophenol reduction yields p-benzoquinone (84.5%) and p-aminophenol (96.3%).
- CeF3-modified Ni(OH)2 anode induces interfacial charge redistribution, reconstructing Ni(OH)2 to active NiOOH; operando XAFS reveals dynamic Ni-O evolution.
- Paired PhOR||NPRR achieves Faradaic efficiency 129.3% and energy consumption 1.06 kWh kg-1; validated with high-purity product recoveries 83.1% and 87.9%.
Angew Chem Int Ed Engl. 2026 Aug 24:e8237151. doi: 10.1002/anie.8237151. Online ahead of print.
ABSTRACT
Electrocatalytic valorization of organic pollutants into value-added chemicals offers a sustainable strategy for wastewater treatment and resource recovery; however, achieving high Faradaic and energy efficiency remains challenging. Herein, we report a bipolar electrocatalytic strategy integrating anodic phenol oxidation (PhOR) with cathodic p-nitrophenol reduction (NPRR) for simultaneously producing p-benzoquinone (p-BQ) and p-aminophenol (p-AP). The tailored Ni(OH)2/CeF3 anode and Cu(OH)2/Ni(OH)2 cathode achieve p-BQ and p-AP yields of 84.5% and 96.3%, respectively. Specifically, incorporation of CeF3 induces the interfacial charge redistribution of Ni site and then facilitates Ni(OH)2 reconstruction into active NiOOH. Operando x-ray absorption fine structure (XAFS) reveals that the potential-driven dynamic Ni-O evolution optimizes the binding strength of reaction intermediates to boost PhOR performance. The cathode with Cu and Ni sites favors the surface-adsorbed H* formation for efficient NPRR via an indirect electron transfer pathway. The PhOR||NPRR system achieves an exceptional Faradaic efficiency of 129.3% with a low energy consumption of 1.06 kWh kg– 1. The practical applicability was validated through the successful production of high-purity p-BQ and p-AP from phenolic pollutants with respective recovery efficiency of 83.1% and 87.9%. This work provides a viable approach for facilitating a sustainable recovery of phenolic wastewaters.
PMID:42638214 | DOI:10.1002/anie.8237151
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