Tailoring the Delocalization State in Electrocatalysts for Efficient NO x Reduction: Recent Advances and Perspectives

作者：Jiacheng Jayden Wang, Jiacheng Jayden Wang, Ximeng Lv, Junqing Ma, Hanxiao Du, Zhuoran Lv, Jiacheng Wang, Jiacheng Wang, Fuqiang Huang · 发表于：ACS Catalysis · 年份：2025 · DOI：10.1021/acscatal.5c04518 · 被引用次数：9 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、CO2 Reduction Techniques and Catalysts、Catalytic Processes in Materials Science

Electrocatalytic reduction of nitrogen oxides (NO x ) into valuable chemicals and fuels is vital for environmental remediation and carbon–nitrogen cycle sustainability. Recent work has demonstrated that delocalization states tuning of the catalyst may enhance NO x reduction (NO x RR) by optimizing intermediate adsorption, cleavage, and electronic conductivity, thereby improving activity, selectivity, and stability. This comprehensive review details the fundamental definition, unique properties, and mechanistic role of delocalization states within the NO x RR pathway. It then synthesizes recent advances across the catalyst lifecycle: synthesis strategies, cutting-edge characterization techniques probing electronic structure, and diverse applications. Applications are systematically categorized into four key regulatory approaches: exploiting intrinsic material delocalization, modulation via tailored organic ligands, engineering through heteroatom doping and heterojunction formation, and external field activation using photo-, electric-, or magnetic fields. Finally, the review identifies key NO x RR delocalization engineering challenges (e.g., unclear dynamic evolution, imbalanced delocalization-activity-selectivity, poor catalyst scalability) and targeted solutions: (1) operando multicharacterization + machine learning-DFT; (2) ligand engineering + external fields for product-specific tuning. It aims to frame next-generation NO x RR catalyst design, advancing environmental reme...