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Enhancing the performance of heterogeneous palladium based catalysts in the mild reductive depolymerization of soda lignin through addition of a non-noble metal and tuning of the preparation strategy

Tibo De Saegher (UGent) , Boyana Atanasova (UGent) , Pieter Vermeir (UGent) , Kevin Van Geem (UGent) , Jeriffa De Clercq (UGent) , An Verberckmoes (UGent) and Jeroen Lauwaert (UGent)
(2024) RSC SUSTAINABILITY. 2(5). p.1551-1567
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Abstract
Research towards mild reductive depolymerization of lignin is gaining momentum because of its potential for producing sustainable functionalized aromatics, but achieving high yields still relies on expensive noble metal catalysts. This study aims to improve the catalysts' cost effectiveness through addition of a non-noble metal to a Pd nanoparticle catalyst, supported on γ-Al2O3. Six Pd based catalysts (Pd, PdCu, PdNi, PdFe, PdCo, and PdMo) were synthesized and prepared through either calcination or thermal reduction, and their activity and selectivity in lignin depolymerization were evaluated as a function of batch time. Principal component analysis (PCA) of the entire datapool revealed that, albeit to varying degrees, the addition of a secondary metal shifts the behavior of a Pd catalyst more towards that of pure solvolysis and that the preparation strategy has no effect on Pd and PdMo. Regarding activity, it was found that the addition of Cu, Ni, Fe, Co and Mo significantly enhances the catalyst's activity and that the preparation strategy is also important, with calcination being preferred for PdCu and PdFe and thermal reduction for PdNi and PdCo. Using a plethora of analysis techniques to assess the selectivity at increasing depths, it was revealed that the shift in selectivity, as identified in the PCA results, is caused by variations in dehydration of aliphatic OH groups and hydrogenation of aliphatic double bonds. Moreover, due to a size exclusion effect during the reaction, differences in selectivity between the catalysts are most pronounced at lower molecular weights.
Keywords
KRAFT LIGNIN, MODEL COMPOUNDS, BOND-CLEAVAGE, HYDRODEOXYGENATION, FRACTIONATION, HYDROGENATION, ETHANOLYSIS, OXIDATION, CHEMICALS, POLYMERS

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MLA
De Saegher, Tibo, et al. “Enhancing the Performance of Heterogeneous Palladium Based Catalysts in the Mild Reductive Depolymerization of Soda Lignin through Addition of a Non-Noble Metal and Tuning of the Preparation Strategy.” RSC SUSTAINABILITY, vol. 2, no. 5, 2024, pp. 1551–67, doi:10.1039/d4su00054d.
APA
De Saegher, T., Atanasova, B., Vermeir, P., Van Geem, K., De Clercq, J., Verberckmoes, A., & Lauwaert, J. (2024). Enhancing the performance of heterogeneous palladium based catalysts in the mild reductive depolymerization of soda lignin through addition of a non-noble metal and tuning of the preparation strategy. RSC SUSTAINABILITY, 2(5), 1551–1567. https://doi.org/10.1039/d4su00054d
Chicago author-date
De Saegher, Tibo, Boyana Atanasova, Pieter Vermeir, Kevin Van Geem, Jeriffa De Clercq, An Verberckmoes, and Jeroen Lauwaert. 2024. “Enhancing the Performance of Heterogeneous Palladium Based Catalysts in the Mild Reductive Depolymerization of Soda Lignin through Addition of a Non-Noble Metal and Tuning of the Preparation Strategy.” RSC SUSTAINABILITY 2 (5): 1551–67. https://doi.org/10.1039/d4su00054d.
Chicago author-date (all authors)
De Saegher, Tibo, Boyana Atanasova, Pieter Vermeir, Kevin Van Geem, Jeriffa De Clercq, An Verberckmoes, and Jeroen Lauwaert. 2024. “Enhancing the Performance of Heterogeneous Palladium Based Catalysts in the Mild Reductive Depolymerization of Soda Lignin through Addition of a Non-Noble Metal and Tuning of the Preparation Strategy.” RSC SUSTAINABILITY 2 (5): 1551–1567. doi:10.1039/d4su00054d.
Vancouver
1.
De Saegher T, Atanasova B, Vermeir P, Van Geem K, De Clercq J, Verberckmoes A, et al. Enhancing the performance of heterogeneous palladium based catalysts in the mild reductive depolymerization of soda lignin through addition of a non-noble metal and tuning of the preparation strategy. RSC SUSTAINABILITY. 2024;2(5):1551–67.
IEEE
[1]
T. De Saegher et al., “Enhancing the performance of heterogeneous palladium based catalysts in the mild reductive depolymerization of soda lignin through addition of a non-noble metal and tuning of the preparation strategy,” RSC SUSTAINABILITY, vol. 2, no. 5, pp. 1551–1567, 2024.
@article{01HWA3JTTFBG51QCVVEY7AYR3B,
  abstract     = {{Research towards mild reductive depolymerization of lignin is gaining momentum because of its potential for producing sustainable functionalized aromatics, but achieving high yields still relies on expensive noble metal catalysts. This study aims to improve the catalysts' cost effectiveness through addition of a non-noble metal to a Pd nanoparticle catalyst, supported on γ-Al2O3. Six Pd based catalysts (Pd, PdCu, PdNi, PdFe, PdCo, and PdMo) were synthesized and prepared through either calcination or thermal reduction, and their activity and selectivity in lignin depolymerization were evaluated as a function of batch time. Principal component analysis (PCA) of the entire datapool revealed that, albeit to varying degrees, the addition of a secondary metal shifts the behavior of a Pd catalyst more towards that of pure solvolysis and that the preparation strategy has no effect on Pd and PdMo. Regarding activity, it was found that the addition of Cu, Ni, Fe, Co and Mo significantly enhances the catalyst's activity and that the preparation strategy is also important, with calcination being preferred for PdCu and PdFe and thermal reduction for PdNi and PdCo. Using a plethora of analysis techniques to assess the selectivity at increasing depths, it was revealed that the shift in selectivity, as identified in the PCA results, is caused by variations in dehydration of aliphatic OH groups and hydrogenation of aliphatic double bonds. Moreover, due to a size exclusion effect during the reaction, differences in selectivity between the catalysts are most pronounced at lower molecular weights.}},
  author       = {{De Saegher, Tibo and Atanasova, Boyana and Vermeir, Pieter and Van Geem, Kevin and De Clercq, Jeriffa and Verberckmoes, An and Lauwaert, Jeroen}},
  issn         = {{2753-8125}},
  journal      = {{RSC SUSTAINABILITY}},
  keywords     = {{KRAFT LIGNIN,MODEL COMPOUNDS,BOND-CLEAVAGE,HYDRODEOXYGENATION,FRACTIONATION,HYDROGENATION,ETHANOLYSIS,OXIDATION,CHEMICALS,POLYMERS}},
  language     = {{eng}},
  number       = {{5}},
  pages        = {{1551--1567}},
  title        = {{Enhancing the performance of heterogeneous palladium based catalysts in the mild reductive depolymerization of soda lignin through addition of a non-noble metal and tuning of the preparation strategy}},
  url          = {{http://doi.org/10.1039/d4su00054d}},
  volume       = {{2}},
  year         = {{2024}},
}
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