School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510275, China.
Institute of Chemical Engineering, Guangdong Academy of Sciences, Guangzhou 510665, China.
Environ Sci Technol. 2023 Nov 21;57(46):17727-17736. doi: 10.1021/acs.est.3c00717. Epub 2023 Mar 2.
Ozone (O) pollution is highly detrimental to human health and the ecosystem due to it being ubiquitous in ambient air and industrial processes. Catalytic decomposition is the most efficient technology for O elimination, while the moisture-induced low stability represents the major challenge for its practical applications. Here, activated carbon (AC) supported δ-MnO (Mn/AC-A) was facilely synthesized via mild redox in an oxidizing atmosphere to obtain exceptional O decomposition capacity. The optimal 5Mn/AC-A achieved nearly 100% of O decomposition at a high space velocity (1200 L g h) and remained extremely stable under entire humidity conditions. The functionalized AC provided well-designed protection sites to inhibit the accumulation of water on δ-MnO. Density functional theory (DFT) calculations confirmed that the abundant oxygen vacancies and a low desorption energy of intermediate peroxide (O) can significantly boost O decomposition activity. Moreover, a kilo-scale 5Mn/AC-A with low cost (∼1.5 $/kg) was used for the O decomposition in practical applications, which could quickly decompose O pollution to a safety level below 100 μg m. This work offers a simple strategy for the development of moisture-resistant and inexpensive catalysts and greatly promotes the practical application of ambient O elimination.
臭氧(O)污染由于在环境空气中和工业过程中无处不在,对人类健康和生态系统具有高度危害性。催化分解是消除 O 的最有效技术,而水分引起的低稳定性是其实际应用的主要挑战。在这里,通过在氧化气氛中进行温和的氧化还原反应,简便地合成了负载在活性炭(AC)上的 δ-MnO(Mn/AC-A),从而获得了出色的 O 分解能力。最佳的 5Mn/AC-A 在高空间速度(1200 L g h)下几乎达到了 100%的 O 分解率,并且在整个湿度条件下都保持着极高的稳定性。功能化的 AC 提供了精心设计的保护位点,以抑制 δ-MnO 上水的积累。密度泛函理论(DFT)计算证实,丰富的氧空位和中间过氧化物(O)的低解吸能显著提高了 O 分解活性。此外,还使用了具有低成本(约 1.5 美元/公斤)的公斤级 5Mn/AC-A 进行实际应用中的 O 分解,可迅速将 O 污染降低到安全水平以下的 100μg m。这项工作为开发耐湿和廉价催化剂提供了一种简单的策略,极大地推动了环境 O 消除的实际应用。