School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan, Hubei 430070, P. R. China.
College of Chemistry, Central China Normal University, Wuhan, Hubei 430079, P. R. China.
Environ Sci Technol. 2024 Jul 9;58(27):12189-12200. doi: 10.1021/acs.est.4c01527. Epub 2024 Jun 5.
Ground-level ozone (O) pollution has emerged as a significant concern due to its detrimental effects on human health and the ecosystem. Catalytic removal of O has proven to be the most efficient and cost-effective method. However, its practical application faces substantial challenges, particularly in relation to its effectiveness across the entire humidity range. Herein, we proposed a novel strategy termed "dual active sites" by employing graphitized carbon-loaded core-shell cobalt catalysts (Co@CoO-C). Co@CoO-C was synthesized via the pyrolysis of a Co-organic ligand as the precursor. By utilizing this approach, we achieved a nearly constant 100% working efficiency of the Co@CoO-C catalyst for catalyzing O decomposition across the entire humidity range. Physicochemical characterization coupled with density functional theory calculations elucidates that the presence of encapsulated metallic Co nanoparticles enhances the reactivity of the cobalt oxide capping layer. Additionally, the interface carbon atom, strongly influenced by adjacent metallic Co nuclei, functions as a secondary active site for the decomposition of O decomposition. The utilization of dual active sites effectively mitigates the competitive adsorption of HO molecules, thus isolating them for adsorption in the cobalt oxide capping layer. This optimized configuration allows for the decomposition of O without interference from moisture. Furthermore, O decomposition monolithic catalysts were synthesized using a material extrusion-based three-dimensional (3D) printing technology, which demonstrated a low pressure drop and exceptional mechanical strength. This work provides a "dual active site" strategy for the O decomposition reaction, realizing O catalytic decomposition over the entire humidity range.
地面臭氧(O)污染因其对人类健康和生态系统的有害影响而成为一个重要的关注点。催化去除 O 已被证明是最有效和最具成本效益的方法。然而,其实际应用面临着重大挑战,特别是在整个湿度范围内的有效性方面。在此,我们提出了一种新的策略,称为“双活性位”,通过使用载石墨化碳的核壳钴催化剂(Co@CoO-C)来实现。Co@CoO-C 通过作为前体的 Co-有机配体的热解合成。通过采用这种方法,我们实现了 Co@CoO-C 催化剂在整个湿度范围内催化 O 分解的几乎恒定的 100%工作效率。物理化学特性分析结合密度泛函理论计算表明,封装的金属 Co 纳米颗粒的存在增强了钴氧化物覆盖层的反应性。此外,受相邻金属 Co 核强烈影响的界面碳原子充当 O 分解的次级活性位。双活性位的利用有效地减轻了 HO 分子的竞争吸附,从而将它们隔离在钴氧化物覆盖层中进行吸附。这种优化的结构允许 O 分解而不受水分的干扰。此外,还使用基于材料挤出的三维(3D)打印技术合成了 O 分解整体式催化剂,该催化剂表现出低压降和出色的机械强度。这项工作为 O 分解反应提供了一种“双活性位”策略,实现了整个湿度范围内的 O 催化分解。