Peng Shengpan, Ma Ziran, Ma Jing, Wang Hongyan, Chen Jingyun, Wei Hui, Li Yonglong, Ao Zhimin, Wang Baodong
National Institute of Clean-and-Low-Carbon Energy, Beijing, China.
School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, China.
Front Chem. 2022 Aug 23;10:978698. doi: 10.3389/fchem.2022.978698. eCollection 2022.
Pd/AlO catalysts modified by different chemical elements (Mg, Si, Ce, and Zr) were tested for methane (CH) catalytic combustion, and PdO nanoparticles loaded on modified AlO were systematically studied. These conditions assess the carrier effects of Pd/AlO and acid strength influences on CH combustion. We observed carrier effects on activation energy through tuning Pd 3d binding energies (BEs) and on pre-exponential factors (A) through Pd dispersion and acidity on supports. When the BE of Pd 3d is 337.3 eV, PdO nanoparticles loaded on modified AlO have excellent activity in cracking the C-H bond of CH, which leads to the lowest activation energy ( ), regardless of the size effect of the PdO nanoparticle. Furthermore, a theoretical construction that acid sites on catalysts promote the reversible elementary step (2Pd-OH ↔ Pd-O* + Pd* + HO) right shifts improving the A dependency on the quantity of exposed Pd* and Pd-O*. As a result, AlO, as the carrier, not only modifies the electronic characteristics and size of supported PdO nanoparticles but also participates in the reaction process acid sites on the surface of AlO.
对由不同化学元素(镁、硅、铈和锆)改性的钯/氧化铝催化剂进行了甲烷催化燃烧测试,并对负载在改性氧化铝上的氧化钯纳米颗粒进行了系统研究。这些条件评估了钯/氧化铝的载体效应以及酸强度对甲烷燃烧的影响。我们通过调整钯3d结合能(BEs)观察到对活化能的载体效应,并通过钯在载体上的分散度和酸度观察到对指前因子(A)的影响。当钯3d的BE为337.3电子伏特时,负载在改性氧化铝上的氧化钯纳米颗粒在裂解甲烷的碳氢键方面具有优异的活性,这导致了最低的活化能( ),而与氧化钯纳米颗粒的尺寸效应无关。此外,一种理论构建表明,催化剂上的酸位点促进可逆基元步骤(2Pd-OH ↔ Pd-O* + Pd* + HO)向右移动,提高了A对暴露的Pd和Pd-O数量的依赖性。结果,氧化铝作为载体,不仅改变了负载的氧化钯纳米颗粒的电子特性和尺寸,而且还通过氧化铝表面的酸位点参与反应过程。