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  • 刘新 ( 副教授 )

    的个人主页 http://faculty.dlut.edu.cn/xliu/zh_CN/index.htm

  •   副教授   博士生导师   硕士生导师
论文成果 当前位置: 中文主页 >> 科学研究 >> 论文成果
Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride

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论文类型:期刊论文
第一作者:Liu, Xin
合写作者:Zhu, Hongdan,Linguerri, Roberto,Han, Yu,Chambaud, Gilberte,Meng, Changgong
发表时间:2017-10-11
发表刊物:CHEMISTRYSELECT
收录刊物:SCIE
卷号:2
期号:29
页面范围:9412-9419
ISSN号:2365-6549
关键字:CO; Defects; h-BN; Monovacancy; Oxidation; Pt; Single Atom Catalysis
摘要:We compared the electronic structure and CO oxidation mechanisms over Pt atoms immobilized by both B-vacancies and N-vacancies on gas-exfoliated hexagonal boron nitride. We showed that chemical bonds are formed between the B atoms associated with dangling bonds around the vacancies and Pt atoms. These bonds not only alter the thermodynamics and kinetics for the aggregation and effectively immobilize Pt atoms, but also significantly change the composition and energetic distribution of the electronic states of the composites to circumvent CO poisoning and to favour coadsorption of CO and O-2, which further regulates the reactions to proceed through a Langmuir-Hinshelwood mechanism. The CO oxidation over Pt atoms immobilized at N-vacancies involves formation of an intermediate with -C(O)-O-O- bonded to Pt, the generation of CO2 by peroxo O-O bond scission and the reduction of the remnant oxygen, and the calculated energy barriers are 0.49, 0.23 and 0.18eV, respectively. Such small energy barriers are comparable to those over Pt atoms trapped at B-vacancies, showing the effectiveness of Pt/hexagonal boron nitride atomic composites as catalysts for CO oxidation. These findings also suggest the feasibility of regulating the reaction pathways over single atom catalysts via interfacial engineering.

 

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