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Nanoparticle proximity controls selectivity in benzaldehyde hydrogenation

Nature Catalysis volume 7, pages 172–184 (2024)Cite this article

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Abstract

Disentangling the effects of nanoparticle proximity and size on thermal catalytic performance is challenging with traditional synthetic methods. Here we adapt a modular raspberry-colloid-templating approach to tune the average interparticle distance of PdAu alloy nanoparticles, while preserving all other physicochemical characteristics, including nanoparticle size. By controlling the metal loading and placement of pre-formed nanoparticles within a 3D macroporous SiO2 support and using the hydrogenation of benzaldehyde to benzyl alcohol and toluene as the probe reaction, we report that increasing the interparticle distance (from 12 to 21 nm) substantially enhances selectivity towards benzyl alcohol (from 54% to 99%) without compromising catalytic performance. Combining electron tomography, kinetic evaluation and simulations, we show that interparticle distance modulates the local benzyl alcohol concentration profile between active sites, consequently affecting benzyl alcohol readsorption, which promotes hydrogenolysis to toluene. Our results illustrate the relevance of proximity effects as a mesoscale tool to control the adsorption of intermediates and, hence, catalytic performance.

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Fig. 1: Synthetic strategy to investigate the effect of NP proximity on catalytic hydrogenation of BA.
Fig. 2: Physical characterization of RCT catalysts.
Fig. 3: Liquid phase BA hydrogenation over RCT catalysts.
Fig. 4: Effect of NP proximity on local BOH concentration profile.

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Data availability

Data that support the findings of this study are available within the paper, Supplementary Information and Source data files. Additional data are available from the authors upon reasonable request. Source data are provided with this paper.

Code availability

The MATLAB script used to extract the centre-to-centre interparticle distance from the processed electron tomographic reconstructions is provided in Supplementary Note 1.

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Acknowledgements

This work was supported by the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under award number DE-SC0012573 (S.K.K. and J.A.), by the US Defense Threat Reduction Agency (DTRA) under award number HDTR1211001612 (K.R.G.L., H.W., S.G. and M.A.), and by the Starting PI Fund of the Electron Microscopy Center at Utrecht University (M.P.P. and J.E.S.v.d.H.). Electron microscopy, TGA, zeta potential measurements, infrared spectroscopy, XPS and CO chemisorption measurements were performed at the Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), which is supported by the National Science Foundation under NSF ECCS award number 1541959. K.R.G.L., M.A. and J.A. thank C. Friend for the use of her laboratory facilities to conduct the batch hydrogenation catalytic reactions. K.R.G.L. acknowledges financial support from the Agency for Science, Technology and Research (A*STAR) Singapore National Science Scholarship (PhD). S.K.K. acknowledges the Swiss National Science Foundation for the award of an Early Postdoc. Mobility fellowship (SNSF grant number P2EZP2_199972). K.R.G.L. thanks R. J. Madix, J. Gardener, S. Li, H. G. Lin and J. Hungerford for the helpful discussions on the analysis of catalytic, STEM–EDX, small-angle X-ray scattering, XPS and CO chemisorption data, respectively.

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Author notes

  1. These authors contributed equally: Kang Rui Garrick Lim, Selina K. Kaiser.

Authors and Affiliations

  1. Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA

    Kang Rui Garrick Lim, Selina K. Kaiser & Joanna Aizenberg

  2. John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA

    Kang Rui Garrick Lim, Selina K. Kaiser, Haichao Wu, Sadhya Garg, Michael Aizenberg & Joanna Aizenberg

  3. Materials Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Utrecht, the Netherlands

    Marta Perxés Perich & Jessi E. S. van der Hoeven

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Contributions

K.R.G.L. and S.K.K. contributed equally to this work. K.R.G.L. conceived the research idea and coordinated the work. K.R.G.L., S.K.K., M.A. and J.A. designed the experiments. K.R.G.L., supported by S.G., designed, synthesized, characterized and analysed the materials. K.R.G.L., guided by S.K.K., conducted catalysis testing and kinetic modelling and analysed the results. M.P.P., supervised by J.E.S.v.d.H., performed the electron tomography experiments and analysed the data. K.R.G.L., S.G. and M.P.P. calculated the interparticle distances. H.W. performed the COMSOL modelling. H.W. and K.R.G.L. analysed the COMSOL modelling results. K.R.G.L. and S.K.K. wrote the manuscript with input from all the authors. J.A. supervised the entire work. All authors have given approval to the final version of the manuscript.

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Correspondence to Joanna Aizenberg.

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Nature Catalysis thanks Yue Liu, Xin Gao and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Methods, Notes 1–8, Figs. 1–19, Tables 1–6 and references.

Supplementary Video 1

Reconstructed dark-field STEM tomogram of 5PdAu/SiO2 RCT catalyst. NPs are shown as bright spots on the grey SiO2 support.

Supplementary Video 2

Reconstructed dark-field STEM tomogram of 20PdAu/SiO2 RCT catalyst. NPs are shown as bright spots on the grey SiO2 support.

Supplementary Video 3

STEM tilt series of 5PdAu/SiO2 RCT catalyst used for tomographic reconstruction. NPs are shown as bright spots on the grey SiO2 support.

Supplementary Video 4

STEM tilt series of 20PdAu/SiO2 RCT catalyst used for tomographic reconstruction. NPs are shown as bright spots on the grey SiO2 support.

Source data

Source Data Fig. 2

Quantitative numerical data shown in Fig. 2.

Source Data Fig. 3

Quantitative numerical data shown in Fig. 3.

Source Data Fig. 4

Quantitative numerical data shown in Fig. 4.

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Lim, K.R.G., Kaiser, S.K., Wu, H. et al. Nanoparticle proximity controls selectivity in benzaldehyde hydrogenation. Nat Catal 7, 172–184 (2024). https://doi.org/10.1038/s41929-023-01104-1

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