Defect-Rich Regulatory Activity Strategy: Disordered Structure for Enhanced Catalytic Interfacial Reaction of Chlorobenzene

doi:10.1021/acs.est.4c08387

	Defect-Rich Regulatory Activity Strategy: Disordered Structure for Enhanced Catalytic Interfacial Reaction of Chlorobenzene
	Zhu, Yuxue 1; Liang, Wenjun 1; Zhang CH(张晨航)1,2; Bin F(宾峰)2 ; Tao, Qianyu 1
通讯作者	Liang, Wenjun([email protected])
发表期刊	ENVIRONMENTAL SCIENCE & TECHNOLOGY
	2024-10-14
卷号	58 期号:43 页码:19385-19396
ISSN	0013-936X
摘要	In contrast to previous defect engineering methods, the preparation of amorphous materials can obtain abundant defect sites through a simple way, which is expected to effectively degrade Volatile Organic Compounds (VOCs) under milder conditions. However, in-depth and systematic studies in this area are still lacking. Novel types of amorphous CeMn x catalysts with abundant defects were prepared through simple hydrothermal synthesis and used for Cl-VOCs catalysis for the first time. Experimental characterizations and DFT calculations proved that Ce doping induced MnO2 lattice distortion, which led to the transformation of CeMn x into an amorphous structure and the formation of abundant defect sites. It was observed that CeMn0.16 was able to eliminate chlorobenzene (CB) at 200 degrees C, and the CO(2 )yields and the selectivity of inorganic chlorine was significantly higher than that of MnO2. The O-18 isotope kinetic experiments revealed that the interfacial reaction process followed the MVK mechanism. The large number of oxygen vacancies accelerated the migration of lattice oxygen from the interior to the exterior, enhancing the ability to trap gas-phase oxygen. Mn4+ acted as the main active center to participate in CB catalysis, and the resulting reactive oxygen species (ROS) and Mn3+-[O2-]-Ce4+ further accelerated the entire oxidation cycle.
关键词	catalytic oxidation chlorobenzene amorphous oxygen vacancy isotopic
DOI	10.1021/acs.est.4c08387
收录类别	SCI ; EI
语种	英语
WOS记录号	WOS:001334329900001
关键词[WOS]	OXYGEN VACANCIES ; OXIDATION ; DEGRADATION ; PERFORMANCE ; COMBUSTION ; TOLUENE ; VOCS ; OXIDES
WOS研究方向	Engineering ; Environmental Sciences & Ecology
WOS类目	Engineering, Environmental ; Environmental Sciences
资助项目	National Natural Science Foundation of China[22378008] ; State Environmental Protection Key Laboratory of Odor Pollution Control[20210504]
项目资助者	National Natural Science Foundation of China ; State Environmental Protection Key Laboratory of Odor Pollution Control
论文分区	一类
力学所作者排名	2
RpAuthor	Liang, Wenjun
引用统计
文献类型	期刊论文
条目标识符	http://dspace.imech.ac.cn/handle/311007/97009
专题	高温气体动力学国家重点实验室
作者单位	1.Beijing Univ Technol, Key Lab Beijing Reg Air Pollut Control, Beijing 100124, Peoples R China; 2.Chinese Acad Sci, State Key Lab High Temp Gas Dynam, Inst Mech, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Zhu, Yuxue,Liang, Wenjun,Zhang CH,et al. Defect-Rich Regulatory Activity Strategy: Disordered Structure for Enhanced Catalytic Interfacial Reaction of Chlorobenzene[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2024,58,43,:19385-19396.Rp_Au:Liang, Wenjun
APA	Zhu, Yuxue,Liang, Wenjun,张晨航,宾峰,&Tao, Qianyu.(2024).Defect-Rich Regulatory Activity Strategy: Disordered Structure for Enhanced Catalytic Interfacial Reaction of Chlorobenzene.ENVIRONMENTAL SCIENCE & TECHNOLOGY,58(43),19385-19396.
MLA	Zhu, Yuxue,et al."Defect-Rich Regulatory Activity Strategy: Disordered Structure for Enhanced Catalytic Interfacial Reaction of Chlorobenzene".ENVIRONMENTAL SCIENCE & TECHNOLOGY 58.43(2024):19385-19396.