Hailili Reshalaiti, Gan Yiming
Beijing Key Laboratory of Heat Transfer and Energy Conversion, Beijing University of Technology, Beijing 100124, P. R. China.
ACS Appl Mater Interfaces. 2025 Jul 16;17(28):39809-39844. doi: 10.1021/acsami.5c06606. Epub 2025 Jul 2.
Nitrogen oxides (NO) severely threaten human health and ecosystems. Photocatalytic technology offers a promising solution for eliminating low-concentration yet highly toxic NO. However, it faces challenges in catalyst stability, control of intermediate and final products, reaction selectivity, and disclosure of interfacial mechanisms. The key to surmounting these hurdles is effective carrier separation, vital for distinct redox reactions in photocatalysts. Additionally, the charge carrier efficiency (formation, transfer, separation, and further dynamics) and catalyst photocorrosion upon light irradiation significantly influence the photocatalytic performance and long-term stability of metal oxide-based systems. Heterojunctions, with their superior charge carrier separation efficiency, can effectively regulate the reaction pathways during NO conversion. Moreover, heterojunction engineering has been proven to mitigate photocorrosion by optimizing interfacial charge transfer and reducing the level of charge accumulation on vulnerable active sites. Despite the proliferation of reviews on photocatalytic heterojunctions, a critical gap exists in works that systematically unify the classification, synthesis, and application of diverse heterojunctions specifically for NO removal, while explicitly linking multiscale interfacial engineering, e.g., atomic-level defects, nanoscale band alignment, molecular adsorption to the precise control of reaction pathways and selectivity. Addressing this gap, this review establishes an innovative, unified framework that integrates heterojunction principles, classifications, and construction methods with their operational performance in NO removal, with an emphasis on their latest advancements. Uniquely, it maps design strategies directly to overcome real-world bottlenecks, such as byproduct suppression, relative humidity resistance, and selectivity enhancement. It interprets the state-of-the-art applications, highlighting how interfacial engineering synergistically enhances carrier efficiency and product control. By emphasizing the significance of improving carrier efficiency and controlling intermediate/final product formation by reactive oxygen species generation, this review provides valuable insights to guide future research toward securing higher NO conversions and reaction selectivity. Additionally, it lays the groundwork for the development of more effective and eco-friendly environmental cleanup technologies.
氮氧化物(NO)严重威胁人类健康和生态系统。光催化技术为消除低浓度但剧毒的NO提供了一种有前景的解决方案。然而,它在催化剂稳定性、中间产物和最终产物的控制、反应选择性以及界面机理的揭示方面面临挑战。克服这些障碍的关键是有效的载流子分离,这对于光催化剂中不同的氧化还原反应至关重要。此外,电荷载流子效率(形成、转移、分离及进一步的动力学过程)以及光照射下催化剂的光腐蚀对基于金属氧化物的体系的光催化性能和长期稳定性有显著影响。异质结具有卓越的电荷载流子分离效率,能够在NO转化过程中有效调控反应路径。此外,已证明异质结工程可通过优化界面电荷转移和减少易损活性位点上的电荷积累水平来减轻光腐蚀。尽管关于光催化异质结的综述众多,但专门针对NO去除系统地统一各种异质结的分类、合成及应用,并明确将多尺度界面工程(如原子级缺陷、纳米级能带排列、分子吸附)与反应路径和选择性的精确控制联系起来的研究仍存在关键空白。为填补这一空白,本综述建立了一个创新的统一框架,将异质结原理、分类、构建方法与其在NO去除中的运行性能相结合,重点关注其最新进展。独特的是,它直接规划设计策略以克服实际瓶颈,如副产物抑制、耐相对湿度性和选择性增强。它阐释了最新应用,突出了界面工程如何协同提高载流子效率和产物控制。通过强调提高载流子效率以及通过活性氧生成控制中间产物/最终产物形成的重要性,本综述提供了有价值的见解,以指导未来研究实现更高的NO转化率和反应选择性。此外,它为开发更有效且环保的环境净化技术奠定了基础。