Carbon Nanofiber Growth Rates on NiCu Catalysts: Quantitative Coupling of Macroscopic and Nanoscale In Situ Studies

Tom A.J. Welling; Suzan E. Schoemaker; Krijn P. de Jong; Petra E. de Jongh

doi:10.1021/acs.jpcc.3c02657

Carbon Nanofiber Growth Rates on NiCu Catalysts: Quantitative Coupling of Macroscopic and Nanoscale In Situ Studies

Tom A.J. Welling, Suzan E. Schoemaker, Krijn P. de Jong, Petra E. de Jongh^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

Since recently, gas-cell transmission electron microscopy allows for direct, nanoscale imaging of catalysts during reaction. However, often systems are too perturbed by the imaging conditions to be relevant for real-life catalyzed conversions. We followed carbon nanofiber growth from NiCu-catalyzed methane decomposition under working conditions (550 °C, 1 bar of 5% H₂, 45% CH₄, and 50% Ar), directly comparing the time-resolved overall carbon growth rates in a reactor (measured gravimetrically) and nanometer-scale carbon growth observations (by electron microscopy). Good quantitative agreement in time-dependent growth rates allowed for validation of the electron microscopy measurements and detailed insight into the contribution of individual catalyst nanoparticles in these inherently heterogeneous catalysts to the overall carbon growth. The smallest particles did not contribute significantly to carbon growth, while larger particles (8-16 nm) exhibited high carbon growth rates but deactivated quickly. Even larger particles grew carbon slowly without significant deactivation. This methodology paves the way to understanding macroscopic rates of catalyzed reactions based on nanoscale in situ observations.

Original language	English
Pages (from-to)	15766-15774
Number of pages	9
Journal	Journal of Physical Chemistry C
Volume	127
Issue number	32
DOIs	https://doi.org/10.1021/acs.jpcc.3c02657
Publication status	Published - 17 Aug 2023

Bibliographical note

Funding Information:
T.A.J.W. and S.E.S. were funded by the Advanced Research Center for Chemical Building Blocks, ARC CBBC, which is cofounded and co-financed by the Dutch Research Council (NWO) and The Netherlands Ministry of Economic Affairs and Climate Policy. The electron microscopy experiments were performed in the Electron Microscopy Center Utrecht, and the authors thank Hans Meeldijk and Chris Schneijdenberg for the technical support. The authors also acknowledge the European Research Council, EU FP7 ERC Advanced Grant No. 338846. They furthermore thank Dennie Wezendonk for technical support for the TGA experiments, and Bennie Reesink, Alexander van Bavel, and Jovana Zečević for fruitful discussions.

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

Funding

T.A.J.W. and S.E.S. were funded by the Advanced Research Center for Chemical Building Blocks, ARC CBBC, which is cofounded and co-financed by the Dutch Research Council (NWO) and The Netherlands Ministry of Economic Affairs and Climate Policy. The electron microscopy experiments were performed in the Electron Microscopy Center Utrecht, and the authors thank Hans Meeldijk and Chris Schneijdenberg for the technical support. The authors also acknowledge the European Research Council, EU FP7 ERC Advanced Grant No. 338846. They furthermore thank Dennie Wezendonk for technical support for the TGA experiments, and Bennie Reesink, Alexander van Bavel, and Jovana Zečević for fruitful discussions.

Funders	Funder number
Advanced Research Center for Chemical Building Blocks, ARC CBBC - Dutch Research Council (NWO)
Netherlands Ministry of Economic Affairs and Climate Policy
European Research Council, EU FP7 ERC	338846

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abstract = "Since recently, gas-cell transmission electron microscopy allows for direct, nanoscale imaging of catalysts during reaction. However, often systems are too perturbed by the imaging conditions to be relevant for real-life catalyzed conversions. We followed carbon nanofiber growth from NiCu-catalyzed methane decomposition under working conditions (550 °C, 1 bar of 5% H2, 45% CH4, and 50% Ar), directly comparing the time-resolved overall carbon growth rates in a reactor (measured gravimetrically) and nanometer-scale carbon growth observations (by electron microscopy). Good quantitative agreement in time-dependent growth rates allowed for validation of the electron microscopy measurements and detailed insight into the contribution of individual catalyst nanoparticles in these inherently heterogeneous catalysts to the overall carbon growth. The smallest particles did not contribute significantly to carbon growth, while larger particles (8-16 nm) exhibited high carbon growth rates but deactivated quickly. Even larger particles grew carbon slowly without significant deactivation. This methodology paves the way to understanding macroscopic rates of catalyzed reactions based on nanoscale in situ observations.",

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note = "Funding Information: T.A.J.W. and S.E.S. were funded by the Advanced Research Center for Chemical Building Blocks, ARC CBBC, which is cofounded and co-financed by the Dutch Research Council (NWO) and The Netherlands Ministry of Economic Affairs and Climate Policy. The electron microscopy experiments were performed in the Electron Microscopy Center Utrecht, and the authors thank Hans Meeldijk and Chris Schneijdenberg for the technical support. The authors also acknowledge the European Research Council, EU FP7 ERC Advanced Grant No. 338846. They furthermore thank Dennie Wezendonk for technical support for the TGA experiments, and Bennie Reesink, Alexander van Bavel, and Jovana Ze{\v c}evi{\'c} for fruitful discussions. Publisher Copyright: {\textcopyright} 2023 The Authors. Published by American Chemical Society.",

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Carbon Nanofiber Growth Rates on NiCu Catalysts: Quantitative Coupling of Macroscopic and Nanoscale In Situ Studies

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