| Anchoring highly dispersed metal nanoparticles by strong electrostatic adsorption (SEA) on a dealuminated beta zeolite for catalysis | |
| Zou, Run1,2; Bramley, Gabriel A.3; Xu, Shanshan1; Chansai, Sarayute1; Panchal, Monik4; Chen, Huanhao5; Zhou, Yangtao2; Gao, Pan6; Hou, Guangjin6; Holmes, Stuart M.1; Hardacre, Christopher1; Jiao, Yilai2; Logsdail, Andrew J.3; Fan, Xiaolei1,7 | |
| Corresponding Author | Jiao, Yilai(Yljiao@imr.ac.cn) ; Logsdail, Andrew J.(LogsdailA@cardiff.ac.uk) ; Fan, Xiaolei(Xiaolei.fan@manchester.ac.uk) |
| 2023-11-27 | |
| Source Publication | CATALYSIS SCIENCE & TECHNOLOGY
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| ISSN | 2044-4753 |
| Pages | 10 |
| Abstract | 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. |
| Funding Organization | 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 |
| DOI | 10.1039/d3cy01334k |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | 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 Research Area | Chemistry |
| WOS Subject | Chemistry, Physical |
| WOS ID | WOS:001112671400001 |
| Publisher | ROYAL SOC CHEMISTRY |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/177319 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Jiao, Yilai; Logsdail, Andrew J.; Fan, Xiaolei |
| Affiliation | 1.Univ Manchester, Sch Engn, Dept Chem Engn, Oxford Rd, Manchester M13 9PL, England 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Peoples R China 3.Cardiff Univ, Cardiff Catalysis Inst, Sch Chem, Pk Pl, Cardiff CF10 3AT, Wales 4.Univ Durham, Dept Chem, Stockton Rd, Durham DH1 3LE, England 5.Nanjing Tech Univ, Coll Chem Engn, State Key Lab Mat Oriented Chem Engn, Nanjing 211816, Peoples R China 6.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 7.Univ Nottingham Ningbo China, Nottingham Ningbo China Beacons Excellence Res & I, 211 Xingguang Rd, Ningbo 315100, Peoples R China |
| Recommended Citation 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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