Zhang Baojian, Liu Rui, Li Liangwei, Guo Weihong, Zhang Biluan, Chen Bosheng, Yuan Weidong, Li Pan, Zhang Shaowen, Wang Jinlong, Yang Ji, Luo Zhu, Guo Yanbing
Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, PR China.
Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education, Central China Normal University, Wuhan, PR China.
Nat Commun. 2025 Aug 22;16(1):7847. doi: 10.1038/s41467-025-63112-y.
Platinum-group metals (Pt) commonly used in thermal catalytic processes often suffer from catalyst deactivation, such as Pt sintering, Pt overoxidation, and Pt loss under high-temperature conditions. To address these, we present a novel Pt/CeZrO catalyst, featuring isolated Pt single atoms (Pt) on a CeZrO support with an ordered macroporous (OM) structure. Firstly, Zr-stabilized dynamic low-coordinated Pt releases more free d-electrons by reducing Pt-O bond occupation, thereby preserving peroxide activity at high temperatures and enhancing propane C-H activation. Additionally, the OM structure prevents Pt loss and reduces Pt loading to 0.4 g/L, compared with 0.9 g/L in commercial diesel oxidation catalysts. As a result, the Pt/CeZrO maintains 92% conversion at 450 °C even after 50 h aging at 800 °C with 10 vol.% HO. Finally, the catalyst is integrated into a 3.4-liter commercial cordierite monolith for developing and scaling robust catalytic converters.
热催化过程中常用的铂族金属（Pt）常常会出现催化剂失活的问题，比如在高温条件下Pt烧结、Pt过氧化以及Pt流失。为了解决这些问题，我们提出了一种新型的Pt/CeZrO催化剂，其特点是在具有有序大孔（OM）结构的CeZrO载体上有孤立的Pt单原子（Pt）。首先，Zr稳定的动态低配位Pt通过减少Pt-O键占有率释放出更多自由d电子，从而在高温下保持过氧化物活性并增强丙烷C-H活化。此外，与商用柴油氧化催化剂中0.9 g/L的Pt负载量相比，OM结构可防止Pt流失并将Pt负载量降低至0.4 g/L。结果，即使在800°C下用10 vol.% HO老化50小时后，Pt/CeZrO在450°C时仍保持92%的转化率。最后，将该催化剂集成到一个3.4升的商用堇青石整体中，以开发和扩大坚固耐用的催化转化器。
