Towards Lignin-Derived Chemicals Using Atom-Efficient Catalytic Routes

Sudarsanam, Putla; Ruijten, Dieter; Liao, Yuhe; Renders, Tom; Koelewijn, S.-F.; Sels, Bert F.

doi:10.1016/j.trechm.2020.07.011

Cited by 27 publications

(21 citation statements)

References 103 publications

(136 reference statements)

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“…Among these, reductive catalytic fractionation (RCF) or catalytic hydrogenolysis of isolated lignin have been intensively studied as a lignin‐first bio‐refinery strategy with the potential to produce valuable alkyl phenolic monomers from lignin [23] . Various catalytic systems with metal‐based catalysts have been explored to produce functional aromatic monomers from different biomasses, and the product portfolio was shown to be tunable by the choice of catalyst and reaction conditions [24–26] . The monomers can be converted to marketable added‐value chemicals by catalytic funneling [22,27] .…”

Section: Introductionmentioning

confidence: 99%

“… [23] Various catalytic systems with metal‐based catalysts have been explored to produce functional aromatic monomers from different biomasses, and the product portfolio was shown to be tunable by the choice of catalyst and reaction conditions. [ 24 , 25 , 26 ] The monomers can be converted to marketable added‐value chemicals by catalytic funneling. [ 22 , 27 ] These monomers are mainly obtained by the cleavage of the β‐O‐4 linkage and thus monomer yields closely correlate with the structure and composition of the staring material.…”

Section: Introductionmentioning

confidence: 99%

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Catalytic Hydrogenolysis of Lignin: The Influence of Minor Units and Saccharides

Wang

Deuss

2021

ChemSusChem

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The precise elucidation of native lignin structures plays a vital role for the development of “lignin first” strategies such as reductive catalytic fractionation. The structure of lignin and composition of the starting material has a major impact on the product yield and distribution. Here, the differences in structure of lignin from birch, pine, reed, and walnut shell were investigated by combining detailed analysis of the whole cell wall material, residual enzyme lignin, and milled wood lignin. The results of the 2D heteronuclear single quantum coherence NMR analysis could be correlated to the product from Ru/C‐catalyzed hydrogenolysis if monomeric products from ferulate and p‐coumaryl and its analogous units were also appropriately considered. Notably, residual polysaccharide constituents seemed to influence the selectivity towards hydroxy‐containing monomers. The results reinforced the importance of adequate structural characterization and compositional analysis of the starting materials as well as distinct (dis)advantages of specific types of structural characterization and isolation methods for guiding valorization potential of different biomass feedstocks.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Catalytic Hydrogenolysis of Lignin: The Influence of Minor Units and Saccharides

Wang

Deuss

2021

ChemSusChem

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“…Lignin is a phenolic polymer which is composed of three major phenylpropanol units, namely p -coumaryl alcohol, coniferyl alcohol, and sinapyl alcohol (Figure D). , Depolymerization of lignin using either chemical, physicochemical, or biological processes or combined processes can liberate substantial amounts of phenolic monomers including monomeric phenols, phenolic aldehydes, and phenolic acids (Figure E). − The phenolic monomers are generally obtained as mixed compounds, in which their specific structures depend upon the depolymerization method used and the plant sources . A method enabling reductive catalytic fractionation (RCF), known as the lignin-first approach, has recently been developed as a one-pot process for extraction and in situ catalytic conversion of the lignin released from lignocellulose into aromatic monomers. , The method enables extraction and catalytic processing of lignin to obtain high yields of aromatic monomers without modifying their structures.…”

Section: Introductionmentioning

confidence: 99%

Enzymes, In Vivo Biocatalysis, and Metabolic Engineering for Enabling a Circular Economy and Sustainability

et al. 2021

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Since the industrial revolution, the rapid growth and development of global industries have depended largely upon the utilization of coal-derived chemicals, and more recently, the utilization of petroleum-based chemicals. These developments have followed a linear economy model (produce, consume, and dispose). As the world is facing a serious threat from the climate change crisis, a more sustainable solution for manufacturing, i.e., circular economy in which waste from the same or different industries can be used as feedstocks or resources for production offers an attractive industrial/business model. In nature, biological systems, i.e., microorganisms routinely use their enzymes and metabolic pathways to convert organic and inorganic wastes to synthesize biochemicals and energy required for their growth. Therefore, an understanding of how selected enzymes convert biobased feedstocks into special (bio)chemicals serves as an important basis from which to build on for applications in biocatalysis, metabolic engineering, and synthetic biology to enable biobased processes that are greener and cleaner for the environment. This review article highlights the current state of knowledge regarding the enzymatic reactions used in converting biobased wastes (lignocellulosic biomass, sugar, phenolic acid, triglyceride, fatty acid, and glycerol) and greenhouse gases (CO 2 and CH 4 ) into value-added products and discusses the current progress made in their metabolic engineering. The commercial aspects and life cycle assessment of products from enzymatic and metabolic engineering are also discussed. Continued development in the field of metabolic engineering would offer diversified solutions which are sustainable and renewable for manufacturing valuable chemicals.

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“… 4 Lignin acts as a binder in lignocellulose and holds cellulose and hemicellulose together. 5 More specifically, lignin is a three-dimensional reticulated macromolecular structure made up of randomly crosslinked oxygenated aromatic units. By crosslinking with cellulose and hemicellulose, lignin provides strength, rigidity, and flexibility with lignocellulose as well as aiding in water transport and protecting against attack by marauding insects and microorganisms.…”

Section: Introductionmentioning

confidence: 99%

“…Among them, hemicellulose and cellulose are composed of five-carbon and six-carbon sugars, but the structure of lignin is very complicated and there is no exact structural model . Lignin acts as a binder in lignocellulose and holds cellulose and hemicellulose together . More specifically, lignin is a three-dimensional reticulated macromolecular structure made up of randomly crosslinked oxygenated aromatic units.…”

Section: Introductionmentioning

confidence: 99%

A New Structural Model of Enzymatic Lignin with Multiring Aromatic Clusters

Wang

Hou

et al. 2022

ACS Omega

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Lignin is a natural aromatic compound in plants. Several lignin structural models have been proposed in the past years, but all the models cannot be converted to benzene carboxylic acids (BCAs) for all aromatic rings connected to oxygen. This inspired us to explore the structures of lignin. Based on the yields of BCAs, the results of 13 C NMR and ethanolysis residues, and gas chromatography–mass spectrometry and electrospray ionization mass spectrometry of ethanolysis of lignin, we have constructed a structural model of lignin with a formula C 6407 H 6736 O 2590 N 147 S 3 . The model not only satisfies the results of analyses, but also explains the generation of BCAs from lignin oxidation and the ethanolysis products. Importantly, double-ring and triple-ring aromatic clusters are found in lignin, and some of them are connected by alkyl bridges, which results in conventional low conversions of lignin. Our findings in the structures of lignin may significantly influence the structures and applications of lignin.

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Towards Lignin-Derived Chemicals Using Atom-Efficient Catalytic Routes

Cited by 27 publications

References 103 publications

Catalytic Hydrogenolysis of Lignin: The Influence of Minor Units and Saccharides

Catalytic Hydrogenolysis of Lignin: The Influence of Minor Units and Saccharides

Enzymes, In Vivo Biocatalysis, and Metabolic Engineering for Enabling a Circular Economy and Sustainability

A New Structural Model of Enzymatic Lignin with Multiring Aromatic Clusters

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