Fang Ling, Lu Shun, Wang Sha, Yang Xiaohui, Song Cheng, Yin Fengjun, Liu Hong
Chongqing Institute of Green and Intelligent Technology, Chinese Academy of Sciences, 1400714, Chongqing, China.
University of Chinese Academy of Sciences, 100049, Beijing, China.
Chemistry. 2024 Apr 5;30(20):e202303249. doi: 10.1002/chem.202303249. Epub 2024 Jan 30.
Electrocatalytic nitrate (NO ) reduction to ammonia (NH) is a "two birds-one stone" method that targets remediation of NO -containing sewage and production of valuable NH. The exploitation of advanced catalysts with high activity, selectivity, and durability is a key issue for the efficient catalytic performance. Among various strategies for catalyst design, defect engineering has gained increasing attention due to its ability to modulate the electronic properties of electrocatalysts and optimize the adsorption energy of reactive species, thereby enhancing the catalytic performance. Despite previous progress, there remains a lack of mechanistic insights into the regulation of catalyst defects for NO reduction. Herein, this review presents insightful understanding of defect engineering for NO reduction, covering its background, definition, classification, construction, and underlying mechanisms. Moreover, the relationships between regulation of catalyst defects and their catalytic activities are illustrated by investigating the properties of electrocatalysts through the analysis of electronic band structure, charge density distribution, and controllable adsorption energy. Furthermore, challenges and perspectives for future development of defects in NORR are also discussed, which can help researchers to better understand the defect engineering in catalysts, and also inspire scientists entering into this promising field.
电催化硝酸盐（NO₃⁻）还原为氨（NH₃）是一种“一石二鸟”的方法，既针对含NO₃⁻污水的修复，又能生产有价值的NH₃。开发具有高活性、选择性和耐久性的先进催化剂是实现高效催化性能的关键问题。在各种催化剂设计策略中，缺陷工程因其能够调节电催化剂的电子性质并优化活性物种的吸附能，从而提高催化性能而受到越来越多的关注。尽管此前已有进展，但对于NO₃⁻还原中催化剂缺陷调控的机理仍缺乏深入了解。在此，本综述对NO₃⁻还原的缺陷工程进行了深刻解读，涵盖其背景、定义、分类、构建及潜在机制。此外，通过分析电子能带结构、电荷密度分布和可控吸附能来研究电催化剂的性质，阐明了催化剂缺陷调控与其催化活性之间的关系。此外，还讨论了NO₃⁻还原反应（NORR）中缺陷未来发展面临的挑战和前景，这有助于研究人员更好地理解催化剂中的缺陷工程，也能激励科学家进入这一充满前景的领域。
