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Pt Nanoparticles on Beta zeolites for Catalytic Toluene Oxidation: Effect of the Hydroxyl Groups of Beta Zeolite
Zou, Run1,2; Chansai, Sarayute1; Xu, Shaojun1; An, Bing3; Zainal, Shima1; Zhou, Yangtao2; Xin, Ruojia1; Gao, Pan4; Hou, Guangjin4; D'Agostino, Carmine1; Holmes, Stuart M.1; Hardacre, Christopher1; Jiao, Yilai2; Fan, Xiaolei1
通讯作者Hardacre, Christopher(c.hardacre@manchester.ac.uk) ; Jiao, Yilai(yljiao@imr.ac.cn) ; Fan, Xiaolei(xiaolei.fan@manchester.ac.uk)
2023-10-25
发表期刊CHEMCATCHEM
ISSN1867-3880
页码12
摘要Stabilisation of metal species using hydroxyl-rich dealuminated zeolites is a promising method for catalysis. However, insights into the interactions between the hydroxyl groups in zeolite and noble metals and their effects on catalysis are not yet fully understood. Herein, comparative studies were conducted using Pt catalysts supported on hydroxyl-rich dealuminated Beta (deAl-Beta) and the pristine proton-form Beta (H-Beta) for catalytic oxidation of toluene. The findings suggest that during impregnation the Pt precursor (i. e., Pt(NH3)(4)(NO3)(2)) interacted with different sites on deAl-Beta and H-Beta, leading to the formation of supported Pt nanoparticles with different physicochemical properties. In detail, for H-Beta, the Pt precursor interacted with Al-OH and isolated external Si-OH sites, yielding Pt NPs with a higher Pt-0 proportion of similar to 71 % compared to similar to 57 % Pt-0 on deAl-Beta. Comparatively, abundant hydroxyl groups on deAl-Beta such as silanol nest and isolated internal Si-OH stabilised highly active Pt-O species. The resulting Pt/deAl-Beta exhibited improved activity and anti-coking ability than Pt/H-Beta in catalytic toluene oxidation. For example, the temperature for 50 % toluene conversion was 193 degrees C for Pt/deAl-Beta vs. 232 degrees C for Pt/H-Beta, and the coke deposition was 1.7 % vs. 6.7 % (after the 24-h longevity test), respectively. According to the toluene-temperature programmed desorption (toluene-TPD), H-1 nuclear magnetic resonance (H-1 NMR) relaxation and in situ diffuse reflection Fourier transform spectroscopy (in situ DRIFTS) characterisation, the enhanced performance of Pt/deAl-Beta could be ascribed to (i) the active Pt-O sites stabilised by hydroxyl groups, which interact with toluene easily for conversion, and (ii) the acid-free feature of the deAl-Beta support, which avoids the formation of coke precursors (such as benzoate species) on the catalyst surface. Findings of the work can serve as the design guidelines for making effective supported metal catalysts using zeolitic carriers.
关键词Beta zeolite Pt nanoparticles dealumination hydroxyl groups toluene oxidation
资助者This project has received funding from the European Unionapos;s Horizon 2020 research and innovation program under grant agreement No 872102. R.Z. thanks the China Scholarship Council (CSC, file no. 201906740020) and The University of Manchester f ; European Union ; China Scholarship Council (CSC) ; University of Manchester ; EPSRC
DOI10.1002/cctc.202300811
收录类别SCI
语种英语
资助项目This project has received funding from the European Unionapos;s Horizon 2020 research and innovation program under grant agreement No 872102. R.Z. thanks the China Scholarship Council (CSC, file no. 201906740020) and The University of Manchester f[872102] ; European Union[201906740020] ; China Scholarship Council (CSC) ; University of Manchester[EP/V026089/1] ; EPSRC
WOS研究方向Chemistry
WOS类目Chemistry, Physical
WOS记录号WOS:001091002200001
出版者WILEY-V C H VERLAG GMBH
引用统计
被引频次:5[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/177723
专题中国科学院金属研究所
通讯作者Hardacre, Christopher; Jiao, Yilai; Fan, Xiaolei
作者单位1.Univ Manchester, Sch Engn, Dept Chem Engn, Oxford Rd, Manchester M13 9PL, England
2.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Peoples R China
3.Univ Manchester, Sch Sci, Dept Chem, Oxford Rd, Manchester M13 9PL, England
4.Chinese Acad Sci, Dalian Inst Chem Phys, Collaborat Innovat Ctr Chem Energy Mat 2011, State Key Lab Catalysis,Natl Lab Clean Energy, Zhongshan Rd 457, Dalian 116023, Peoples R China
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GB/T 7714
Zou, Run,Chansai, Sarayute,Xu, Shaojun,et al. Pt Nanoparticles on Beta zeolites for Catalytic Toluene Oxidation: Effect of the Hydroxyl Groups of Beta Zeolite[J]. CHEMCATCHEM,2023:12.
APA Zou, Run.,Chansai, Sarayute.,Xu, Shaojun.,An, Bing.,Zainal, Shima.,...&Fan, Xiaolei.(2023).Pt Nanoparticles on Beta zeolites for Catalytic Toluene Oxidation: Effect of the Hydroxyl Groups of Beta Zeolite.CHEMCATCHEM,12.
MLA Zou, Run,et al."Pt Nanoparticles on Beta zeolites for Catalytic Toluene Oxidation: Effect of the Hydroxyl Groups of Beta Zeolite".CHEMCATCHEM (2023):12.
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