Conversion of confined metal@ZIF-8 structures to intermetallic nanoparticles supported on nitrogen-doped carbon for electrocatalysis
- 472 Downloads
We report a facile strategy to synthesize intermetallic nanoparticle (iNP) electrocatalysts via one-pot pyrolysis of a zeolitic imidazolate framework, ZIF-8, encapsulating precious metal nanoparticles (NPs). ZIF-8 serves not only as precursor for N-doped carbon (NC), but also as Zn source for the formation of intermetallic or alloy NPs with the encapsulated metals. The resulting sub-4 nm PtZn iNPs embedded in NC exhibit high sintering resistance up to 1,000 °C. Importantly, the present methodology allows fine-tuning of both composition (e.g., PdZn and RhZn iNPs, as well as AuZn and RuZn alloy NPs) and size (2.4, 3.7, and 5.4 nm PtZn) of the as-formed bimetallic NPs. To the best of our knowledge, this is the first report of a metal-organic framework (MOF) with multiple functionalities, such as secondary metal source, carbon precursor, and size-regulating reagent, which promote the formation of iNPs. This work opens a new avenue for the synthesis of highly uniform and stable iNPs.
Keywordsintermetallic compounds cage confinement pyrolysis electrocatalysis sintering resistance
Acknowledgment is made to the donors of the American Chemical Society Petroleum Research Fund for support of this research. We thank Gordon J. Miller for the use of the X-ray diffractometer. We also thank Dapeng Jing at the Materials Analysis and Research Laboratory (MARL) of Iowa State University for the assistance on XPS measurement.
- Wang, Y. J.; Zhao, N. N.; Fang, B. Z.; Li, H.; Bi, X. T. T.; Wang, H. J. Carbon-supported Pt-based alloy electrocatalysts for the oxygen reduction reaction in polymer electrolyte membrane fuel cells: Particle size, shape, and composition manipulation and their impact to activity. Chem. Rev. 2015, 115, 3433–3467.CrossRefGoogle Scholar
- Qi, Z. Y.; Xiao, C. X.; Liu, C.; Goh, T. W.; Zhou, L.; Maligal-Ganesh, R.; Pei, Y. C.; Li, X. L.; Curtiss, L. A.; Huang, W. Y. Sub-4 nm PtZn intermetallic nanoparticles for enhanced mass and specific activities in catalytic electrooxidation reaction. J. Am. Chem. Soc. 2017, 139, 4762–4768.CrossRefGoogle Scholar
- Xiao, C. X.; Maligal-Ganesh, R. V.; Li, T.; Qi, Z. Y.; Guo, Z. Y.; Brashler, K. T.; Goes, S.; Li, X. L.; Goh, T. W.; Winans, R. E. et al. High-temperature-stable and regenerable catalysts: Platinum nanoparticles in aligned mesoporous silica wells. ChemSusChem 2013, 6, 1915–1922.CrossRefGoogle Scholar
- Maligal-Ganesh, R. V.; Xiao, C. X.; Goh, T. W.; Wang, L. L.; Gustafson, J.; Pei, Y. C.; Qi, Z. Y.; Johnson, D. D.; Zhang, S. R.; Tao, F. et al. A ship-in-a-bottle strategy to synthesize encapsulated intermetallic nanoparticle catalysts: Exemplified for furfural hydrogenation. ACS Catal. 2016, 6, 1754–1763.CrossRefGoogle Scholar
- Li, X. L.; Zhang, B. Y.; Fang, Y. H.; Sun, W. J.; Qi, Z. Y.; Pei, Y. C.; Qi, S. Y.; Yuan, P. Y.; Luan, X. C.; Goh, T. W. et al. Metal-organic-framework-derived carbons: Applications as solid-base catalyst and support for Pd nanoparticles in tandem catalysis. Chem.-Eur. J. 2017, 23, 4266–4270.CrossRefGoogle Scholar
- Chen, Y. J.; Ji, S. F.; Wang, Y. G.; Dong, J. C.; Chen, W. X.; Li, Z.; Shen, R. A.; Zheng, L. R.; Zhuang, Z. B.; Wang, D. S. et al. Isolated single iron atoms anchored on N-doped porous carbon as an efficient electrocatalyst for the oxygen reduction reaction. Angew. Chem., Int. Ed. 2017, 56, 6937–6941.CrossRefGoogle Scholar
- Song, H.; Rioux, R. M.; Hoefelmeyer, J. D.; Komor, R.; Niesz, K.; Grass, M.; Yang, P. D.; Somorjai, G. A. Hydrothermal growth of mesoporous SBA-15 silica in the presence of PVP-stabilized Pt nanoparticles: Synthesis, characterization, and catalytic properties. J. Am. Chem. Soc. 2006, 128, 3027–3037.CrossRefGoogle Scholar
- Massalski, T. B.; Okamoto, H.; Subramanian, P. R.; Kacprzak, L. Binary Alloy Phase Diagrams, 2nd ed.; ASM International: Ohio, 1990.Google Scholar