摘要
单原子催化剂(single-atom catalyst,SAC)可以最大化金属原子利用率,并具有独特的电子特性,已经在各种催化反应中进行了广泛的探索。然而,与纳米催化剂相比,贵金属SAC在烃类氧化反应中通常被认为是不活泼的。在本文中,证明了WO_(3)-TiO_(2)负载的Pt SAC(Pt1/WO_(3)-TiO_(2))在光热协同催化氧化C3H8和C3H6这两种典型的挥发性有机化合物(VOCs)中表现出比相应的纳米催化剂(PtNP/WO_(3)-TiO_(2))高得多的活性。研究发现,Pt1/WO_(3)-TiO_(2)和PtNP/WO_(3)-TiO_(2)都可以通过克服氧中毒来提高光热协同催化C3H8氧化的活性。值得注意的是,Pt1/WO_(3)-TiO_(2)的反应速率达到了3792μmol∙gPt−1∙s^(−1),这对C3H8氧化是一个新的突破。更有趣的是,由于C3H6在PtNP/WO_(3)-TiO_(2)上的强吸附导致催化剂C3H6中毒,因此PtNP/WO_(3)-TiO_(2)上的光热协同催化C3H6氧化无法进行。但是,得益于C3H6和Pt单原子之间适中的相互作用,Pt1/WO_(3)-TiO_(2)上的C3H6中毒在光照下可以被克服。因此,Pt1/WO_(3)-TiO_(2)在光热协同催化C3H6氧化中显示出更高的活性。这项工作表明,SAC的优势不仅在于节约贵金属,还在于可以根据其独特的电子特性发现新的催化反应。
Catalytic oxidation is a commonly employed technology in the industry for removing volatile organic compounds(VOCs)due to its exceptional efficiency under mild operating conditions.Although supported Pt-based nano-catalysts are recognized widely as one of the most promising and extensively used industrial catalysts for VOC abatement,their practical application,and development are restricted by their exorbitant cost.Single-atom catalyst(SAC)with maximized metal utilization and exclusive electronic character has been explored extensively in various catalytic reactions.However,Pt SAC is usually deemed to be inactive in hydrocarbon oxidation reactions in thermal catalysis,compared with its nanoparticle counterpart.Here,we demonstrate that the WO_(3)-TiO_(2) supported Pt SAC(Pt1/WO_(3)-TiO_(2))exhibits much higher activities than the corresponding nanoparticle catalyst(PtNP/WO_(3)-TiO_(2))in photo-thermo catalytic oxidation of C3H8 and C3H6,which represent different kinds of typical VOCs.A key finding is that the activities of Pt1/WO_(3)-TiO_(2) and PtNP/WO_(3)-TiO_(2) can be accelerated in photo-thermo catalytic C3H8 oxidation by overcoming oxygen poisoning.Upon the light irradiation,the apparent active energy(Ea)of the Pt1/WO_(3)-TiO_(2) and PtNP/WO_(3)-TiO_(2) decline from 116 to 60 kJ·mol−1 and from 103 to 30 kJ·mol−1,respectively,substantiating their effectiveness in photo-thermo catalysis.Notably,a substantially higher reaction rate of 3792μmol∙gPt−1∙s^(−1) on the Pt1/WO_(3)-TiO_(2) is achieved,which should be a benchmark for C3H8 oxidation.More intriguingly,photo-thermo catalytic C3H6 oxidation on the PtNP/WO_(3)-TiO_(2) is prohibited due to the strong adsorption-induced C3H6 poisoning on the Pt nanoparticles,for which the Ea of the PtNP/WO_(3)-TiO_(2) catalyst for C3H6 oxidation is maintained at approximately 55 kJ·mol−1,regardless of the light irradiation.In comparison,the C3H6 poisoning on the Pt1/WO_(3)-TiO_(2) can be mitigated by light illumination,where the Ea of the Pt1/WO_(3)-TiO_(2) c
作者
朱锐杰
康磊磊
李林
潘晓丽
王华
苏杨
李广亿
程鸿魁
李仁贵
刘晓艳
王爱琴
Ruijie Zhu;Leilei Kang;Lin Li;Xiaoli Pan;Hua Wang;Yang Su;Guangyi Li;Hongkui Cheng;Rengui Li;Xiao Yan Liu;Aiqin Wang(Dalian Institute of Chemical Physics,CAS Key Laboratory of Science and Technology on Applied Catalysis,iChEM,Chinese Academy of Sciences,Dalian 116023,Liaoning Province,China;University of Chinese Academy of Sciences,Beijing 100049,China;Chia Tai Energy Materials(Dalian)Co.,Ltd.,Dalian 116021,Liaoning Province,China;Dalian Institute of Chemical Physics,State Key Laboratory of Catalysis,Chinese Academy of Sciences,Dalian 116023,Liaoning Province,China;Dalian National Laboratory for Clean Energy,Dalian 116023,Liaoning Province,China.)
出处
《物理化学学报》
SCIE
CAS
CSCD
北大核心
2024年第1期26-27,共2页
Acta Physico-Chimica Sinica
基金
国家自然科学基金(22102180)
辽宁省兴辽英才计划(XLYC2007070)
中国科学院洁净能源创新研究院合作基金(DNL202002)
中央高校基本科研业务费专项资金(20720220009)资助项目。
关键词
单原子催化剂
光热协同催化
氧化反应
氧中毒
丙烯中毒
Single-atom catalyst
Photo-thermo catalysis
Oxidation reaction
Oxygen poisoning
Propylene poisoning
