Applied Surface Science ( IF 6.3 ) Pub Date : 2022-06-26 , DOI: 10.1016/j.apsusc.2022.154056 Shiqi Peng , Rong Li , Yu Huang , Yufei Zhang , Jun-ji Cao , Shuncheng Lee
Producing the strong metal-support interaction (SMSI) interface and highly reactive oxygen species is a great challenge for catalytic oxidation of formaldehyde (HCHO) at room temperature over supported metal catalysts. Herein, we report a conceptual oxygen vacancy (VO) associated SMSI interface of Pt-ZrO2 nanoparticles for HCHO catalysis at room temperature, exhibiting interfacial dependent reactive oxygen species (O*) formation. The VO on the ZrO2 support captures and activates the molecular O2, then proceeds to generating the reactive oxygen atom (O*) with a lower activation barrier of 0.3 eV. The generated O* tends to link the (1 1 0) surface of ZrO2 and the (1 1 1) surface of Pt as an electronic transmission channel for the selective catalytic oxidation of HCHO adsorbed on the (1 1 0) surface of ZrO2, accelerating the direct generation of formate species and mineralization of HCHO. The Pt-VO-ZrO2 achieves high HCHO removal and HCHO conversion (>95%) at 20 °C. These findings will consolidate the fundamental theories of room temperature catalytic reactions via constructing the SMSI interface engineering for wide environmental applications.
中文翻译:
在 Pt-ZrO2 纳米颗粒上产生界面依赖性活性氧,用于室温下催化氧化甲醛
产生强金属-载体相互作用 (SMSI) 界面和高活性氧物种是在负载金属催化剂上在室温下催化氧化甲醛 (HCHO) 的巨大挑战。在此,我们报告了在室温下用于 HCHO 催化的 Pt-ZrO 2纳米粒子的概念性氧空位 ( VO ) 相关 SMSI 界面,表现出界面依赖性活性氧 ( O *) 形成。ZrO 2载体上的V O捕获并活化分子O 2,然后继续生成具有0.3 eV的较低活化势垒的活性氧原子(O*)。生成的 O* 倾向于连接ZrO的 (1 1 0) 表面 2和Pt的(1 1 1)表面作为电子传输通道选择性催化氧化吸附在ZrO 2 (1 1 0)表面的HCHO ,加速了甲酸盐的直接生成和HCHO的矿化。Pt -V O -ZrO 2在 20 °C 时实现了高 HCHO 去除率和 HCHO 转化率 (>95%)。这些发现将通过构建适用于广泛环境应用的 SMSI 界面工程来巩固室温催化反应的基本理论。