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Anchoring highly dispersed metal nanoparticles by strong electrostatic adsorption (SEA) on a dealuminated beta zeolite for catalysis

文献类型：期刊论文

作者Zou, Run3,4; Bramley, Gabriel A.5; Xu, Shanshan3; Chansai, Sarayute3; Panchal, Monik6; Chen, Huanhao7; Zhou, Yangtao4; Gao, Pan1; Hou, Guangjin1; Holmes, Stuart M.3
刊名CATALYSIS SCIENCE & TECHNOLOGY
出版日期2023-11-27
页码10
ISSN号2044-4753
DOI10.1039/d3cy01334k
通讯作者Jiao, Yilai(Yljiao@imr.ac.cn) ; Logsdail, Andrew J.(LogsdailA@cardiff.ac.uk) ; Fan, Xiaolei(Xiaolei.fan@manchester.ac.uk)
英文摘要Zeolites with defects can be combined with appropriate synthetic protocols to beneficially stabilise metallic clusters and nanoparticles (NPs). In this work, highly dispersed Ni NPs were prepared on a defect-rich dealuminated beta (deAl-beta) zeolite through strong electrostatic adsorption (SEA) synthesis, which enabled strong interactions between the electronegative deAl-beta and cationic metal ammine complexes (e.g., Ni(NH3)62+) via the framework silanol nests. Ni NPs with diameters of 1.9 +/- 0.2 nm were formed after SEA and reduction in H2 at 500 degrees C and showed good activity in CO2 methanation (i.e., specific reaction rate of 3.92 x 10-4 mol s-1 gNi-1 and methane selectivity of 99.8% at 400 degrees C under GHSV of 30 000 mL g-1 h-1). The mechanism of the SEA synthetic process was elucidated by ex situ XAFS, in situ DRIFTS, and DFT. XAFS of the as-prepared Ni catalysts (i.e., unreduced) indicates that SEA leads to the exchange of anions in Ni precursors (e.g., Cl- and NO3-) to form Ni(OH)2, while in situ DRIFTS of catalyst reduction shows a significant decrease in the signal of IR bands assigned to the silanol nests (at similar to 960 cm-1), which could be ascribed to the strong interaction between Ni(OH)2 and silanol nests via SEA. DFT calculations show that metallic complexes bind more strongly to charged defect sites compared to neutral silanol nest defects (up to 150 kJ mol-1), confirming the enhanced interaction between metallic complexes and zeolitic supports under SEA synthesis conditions. The results provide new opportunities for preparing highly dispersed metal catalysts using defect-rich zeolitic carriers for catalysis. Enhanced interaction between metal precursors and silanol nests was demonstrated on a silanol-rich dealuminated beta zeolite by strong electrostatic adsorption, leading to the formation of highly dispersed Ni nanoparticles for effective catalysis.
资助项目University Postgraduate Programme[872102] ; European Union[201906740020] ; China Scholarship Council ; University of Manchester[MR/T018372/1] ; UKRI Future Leaders Fellowship program ; Advanced Research Computing at Cardiff (ARCCA) under the Supercomputing Wales - European Regional Development Fund (ERDF) via Welsh Government[EP/V029053/1] ; Engineering and Physical Sciences Research Council
WOS研究方向Chemistry
语种英语
WOS记录号WOS:001112671400001
出版者ROYAL SOC CHEMISTRY
资助机构University Postgraduate Programme ; European Union ; China Scholarship Council ; University of Manchester ; UKRI Future Leaders Fellowship program ; Advanced Research Computing at Cardiff (ARCCA) under the Supercomputing Wales - European Regional Development Fund (ERDF) via Welsh Government ; Engineering and Physical Sciences Research Council
源URL[http://ir.imr.ac.cn/handle/321006/177318]  
专题金属研究所_中国科学院金属研究所
通讯作者Jiao, Yilai; Logsdail, Andrew J.; Fan, Xiaolei
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, 2011 Collaborat Innovat Ctr Chem Energy Mat, State Key Lab Catalysis,Natl Lab Clean Energy, Zhongshan Rd 457, Dalian 116023, Peoples R China
2.Univ Nottingham Ningbo China, Nottingham Ningbo China Beacons Excellence Res & I, 211 Xingguang Rd, Ningbo 315100, Peoples R China
3.Univ Manchester, Sch Engn, Dept Chem Engn, Oxford Rd, Manchester M13 9PL, England
4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Peoples R China
5.Cardiff Univ, Cardiff Catalysis Inst, Sch Chem, Pk Pl, Cardiff CF10 3AT, Wales
6.Univ Durham, Dept Chem, Stockton Rd, Durham DH1 3LE, England
7.Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 211816, Peoples R China
推荐引用方式
GB/T 7714		 Zou, Run,Bramley, Gabriel A.,Xu, Shanshan,et al. Anchoring highly dispersed metal nanoparticles by strong electrostatic adsorption (SEA) on a dealuminated beta zeolite for catalysis[J]. CATALYSIS SCIENCE & TECHNOLOGY,2023:10.
APA Zou, Run.,Bramley, Gabriel A..,Xu, Shanshan.,Chansai, Sarayute.,Panchal, Monik.,...&Fan, Xiaolei.(2023).Anchoring highly dispersed metal nanoparticles by strong electrostatic adsorption (SEA) on a dealuminated beta zeolite for catalysis.CATALYSIS SCIENCE & TECHNOLOGY,10.
MLA Zou, Run,et al."Anchoring highly dispersed metal nanoparticles by strong electrostatic adsorption (SEA) on a dealuminated beta zeolite for catalysis".CATALYSIS SCIENCE & TECHNOLOGY (2023):10.

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来源：金属研究所

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