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Understanding effects of Ni particle size on steam methane reforming activity by combined experimental and theoretical analysis

Wang, Yalan; Wang, Hongmin; Dam, Anh Hoang; Xiao, Ling; Qi, Yanying; Niu, Juntian; Yang, Jia; Zhu, Yi-An; Holmen, Anders; Chen, De
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URI
https://hdl.handle.net/11250/2660915
Date
2019
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  • Institutt for kjemisk prosessteknologi [1428]
  • Publikasjoner fra CRIStin - NTNU [26746]
Original version
Catalysis Today. 2019, 1-9.   10.1016/j.cattod.2019.04.040
Abstract
Fundamental understanding of the size-dependent activity is essential to harness powers of the nanocatalysts. Here we report an experimental and theoretical study of the Ni particle size effect on activity of steam methane reforming (SMR) to achieve a better understanding of the size dependence of kinetic behavior at an atomic level. A kinetic study illustrated the higher forward methane turnover frequency on the smaller sized Ni particles. The size-dependent activity was well reproduced by microkinetic modeling on a truncated octahedron model with the kinetic parameters estimated by the improved unity bond index-quadratic exponential potential (UBI-QEP) and the Brønsted–Evans–Polanyi (BEP) relationship. Microkinetic modeling suggested that the size-dependent activity of Ni catalysts is associated with the surface-dependent activity. Much higher activity of Ni(2 1 1) than Ni(1 1 1) and Ni(1 0 0) accompanied by decreased Ni(2 1 1) surface fraction results in reduced Ni activity as particle size increases. The activity of Ni(1 1 1) is limited by high free energy barriers, while that of Ni(1 0 0) is limited by site blockage by C* and CH*. This work offers a feasible approach to gain insight into size-dependent activity and to aid rational catalyst design for SMR in which preparing extremely small Ni particles (≤6 nm) might be a good strategy.
Publisher
Elsevier
Journal
Catalysis Today

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