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基于铂原子修饰的 MnOOH/MnO 催化剂增强活性羟基和活性氧物种之间的协同降解室内甲醛作用。

Enhanced the synergistic degradation effect between active hydroxyl and reactive oxygen species for indoor formaldehyde based on platinum atoms modified MnOOH/MnO catalyst.

机构信息

The Key Laboratory of Advanced Functional Materials, Ministry of Education of China, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, People's Republic of China.

Key Laboratory of Beijing on Regional Air Pollution Control, Beijing University of Technology, Beijing 100124, People's Republic of China.

出版信息

J Colloid Interface Sci. 2022 Dec 15;628(Pt B):359-370. doi: 10.1016/j.jcis.2022.08.079. Epub 2022 Aug 17.

Abstract

Maintaining high activity during prolonged catalysis is always the pursuit in catalytic degradation of organic pollutants. For indoor formaldehyde (HCHO) degradation, the accumulation of intermediates is the major factor limiting the conversion of HCHO to final product CO (HCHO-to-CO conversion) and long-lasting catalysis. Herein, a three-dimensional radialized nanostructure catalyst self-assembled by MnOOH/MnO nanosheets anchored with Pt single atoms (Pt-MnOOH/MnO with a trace platinum loading amount of 0.09%) is developed by thermally assisted two-step electrochemical method, which achieves enhanced CO production in catalytic HCHO degradation at the room temperature by the collaborative action of active hydroxyl (OH*) and active oxygen species (O*). By boosting intermediates' decomposing, the catalyst implements real-time HCHO-to-CO conversion (∼85.7%) and long-term continuous HCHO removal (∼98%) during 100 h in a 15 ppm HCHO atmosphere at 25 °C under a weight hourly space velocity of 30000 mL/g∙h. Density functional theory calculation shows that the formation energy of O* from O over Pt-MnOOH/MnO is nearly half lower than that over Pt-MnO catalyst. And decomposing accumulated intermediates gives the credit to OH* species sustainably generated by the combined action of MnOOH and O*. The synergistic action between Pt and MnOOH contributes to the continuous production of O* and OH* for enhancing CO production in indoor catalytic formaldehyde degradation.

摘要

在有机污染物的催化降解中,保持长时间的高催化活性一直是人们追求的目标。对于室内甲醛(HCHO)的降解,中间产物的积累是限制 HCHO 转化为最终产物 CO(HCHO 到 CO 的转化率)和长时间持续催化的主要因素。在此,通过热辅助两步电化学方法开发了一种由 MnOOH/MnO 纳米片锚定的 Pt 单原子组成的三维放射状纳米结构催化剂(Pt-MnOOH/MnO 的铂载量痕量为 0.09%),通过活性羟基(OH*)和活性氧物种(O*)的协同作用,在室温下实现了催化 HCHO 降解中 CO 产量的提高。通过促进中间产物的分解,该催化剂在 25°C 下、15ppm HCHO 气氛中、重量时空速度为 30000mL/g·h 时,在 100h 内实现了实时 HCHO 到 CO 的转化率(约 85.7%)和长期连续的 HCHO 去除(约 98%)。密度泛函理论计算表明,Pt-MnOOH/MnO 上 O的形成能比 Pt-MnO 催化剂上的 O低近一半。而分解积累的中间产物使 MnOOH 和 O的共同作用持续产生 OH物种。Pt 和 MnOOH 之间的协同作用有助于 O和 OH的持续生成,从而提高室内催化甲醛降解中的 CO 产量。

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