催化作用
铂金
化学
甲醛
吸附
离解(化学)
氧气
氧化还原
铂纳米粒子
二氧化钛
空间速度
无机化学
光化学
化学工程
物理化学
有机化学
选择性
工程类
作者
Kumar Vikrant,Myoung Won Chung,Danil W. Boukhvalov,Philippe M. Heynderickx,Ki‐Hyun Kim,Seunghyun Weon
标识
DOI:10.1016/j.cej.2023.146007
摘要
Minimal use of noble metals is ideal in developing catalytic systems against carcinogenic formaldehyde (FA) in air. Although single-atom catalysts (SACs) have been proposed to maximize atomic utilization, metals dispersed to the single-atom limit are less durable in redox environments. A highly dispersed platinum (Pt) ensemble (Ptn) on titanium dioxide (TiO2) was synthesized and validated to achieve 100% conversion of 100 ppm FA in dry air at room temperature (RT) at a gas hourly space velocity of 47,771 h−1. In contrast, Pt SAC (Pt1/TiO2) and a reference Pt nanoparticle catalyst (PtNP/TiO2) exhibited much lower performances. The turnover frequencies (TOFs) of Ptn/TiO2, Pt1/TiO2, and PtNP/TiO2 for the RT FA oxidation reaction were 0.03, 0.01, and 0.005 s−1, respectively. The critical role of the surface lattice oxygen (Olatt) in the overall reaction was supported by the prominence of the Mars van Krevelen kinetics in FA oxidation by the Ptn catalyst. The performance of the PtNP catalyst matched with Ptn only when the Pt loading in the former was raised to 2 wt%. Hence, the Pt dose can be reduced by one-fourth through the ensemble form dispersed at the sub-nanometer scale. The density functional theory simulation also distinguished the roles of different Pt catalysts. The Ptn sites could serve as an oxygen reservoir (effective dissociation of molecular oxygen) to promote proximate reactions (between the adsorbed –CHO and surface Olatt species). Conversely, Pt1 is a single site that restricts proximate reactions with vulnerability to surface poisoning.
科研通智能强力驱动
Strongly Powered by AbleSci AI