Lignin-first biorefining of Nordic poplar to produce cellulose fibers could displace cotton production on agricultural lands

Adler, Avital; Kumaniaev, Ivan; Karačić, Almir; Baddigam, Kiran Reddy; Hanes, Rebecca; Subbotina, Elena; Bartling, Andrew; Huertas-Alonso, Alberto J.; Moreno, Andrés; Håkansson, Helena; Mathew, Aji P.; Beckham, Gregg T.; Samec, Joseph S. M.

doi:10.1016/j.joule.2022.06.021

Cited by 41 publications

(34 citation statements)

References 64 publications

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“…6 Besides, the solid loading during the "lignin first" method is hard to balance because low-solid loading is disadvantageous in scale-up production, while high-solid loading will lead to more condensation reactions because the solubilized lignin is unstable at high temperature which needs to immediately react with the catalyst. [6][7][8][9] Besides, side reactions such as lignin condensation could also be induced by lignin being directly brought into contact with the catalyst. Therefore, it is necessary to first obtain well-preserved lignin before lignin reductive fractionation to reduce the poisoning reactions.…”

Section: Introductionmentioning

confidence: 99%

A high-solid DES pretreatment using never-dried biomass as the starting material: towards high-quality lignin fractionation

et al. 2023

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Section: Introductionmentioning

confidence: 99%

A high-solid DES pretreatment using never-dried biomass as the starting material: towards high-quality lignin fractionation

et al. 2023

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“…As one of the three main components of lignocellulose, lignin has been recognized as the most abundant aromatic biopolymer on earth, thereby affording lignin being the most promising alternative to fossil-based aromatics (i.e., chemicals and materials) [5][6][7] . Especially, the concept of "lignin-first biorefinery" significantly promotes the development of lignin upgrading to produce useful chemicals and functional materials [8][9][10] . Generally, dissolution of lignin in an appropriate solvent is unavoidable to realize the goal of effectively utilizing lignin.…”

Section: Introductionmentioning

confidence: 99%

Biomass-Based Acidic Deep Eutectic Solvents for Efficient Dissolution of Lignin: Towards Performance and Mechanism Elucidation

Huang¹,

Chen²,

Zhao³

et al. 2023

Acta Physico Chimica Sinica

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Lignocellulose utilization has the unique feature of net-zero carbon emissions. Thus, the utilization of lignocellulose as a renewable alternative to fossil-based carbon resources is one of the most promising strategies to achieve "carbon neutrality". Lignin has been recognized as the most abundant aromatic biopolymer on Earth; hence, it could be the most promising alternative to fossil-based aromatics. The efficient dissolution of lignin is crucial for lignin upgrading, which relies on the design of innovative and robust solvents. Herein, we designed several biomass-derived acidic deep eutectic solvents (DESs) using choline chloride, betaine, and L-carnitine as hydrogen bond acceptors (HBAs), and four protic compounds as hydrogen bond donors (HBDs), namely, oxalic acid, benzoic acid, ethyl gallate, and 5-methoxysalicylic acid. The designed DESs can dissolve different types of lignin, including alkali lignin (AL), dealkaline lignin (DAL), enzymatic hydrolysis lignin (EHL), and Kraft lignin (KL). Lignin dissolution was found to be affected by the relative contents of three phenylpropanoid monomers in lignin: syringyl (S), guaiacyl (G), and p-hydroxyphenyl (H) units. More S and fewer H units in lignin could result in higher solubility. G-, S-, and H-type structural units were found in EHL, while AL, KL, and DAL had only G-type structural units. Therefore, EHL could be more easily dissolved than AL, KL, and DAL in the most developed DESs. The hydroxyl group content of the four lignin samples had a significant impact on lignin dissolution. AL (1.98 mmol•g −1 ) and EHL (1.93 mmol•g −1 ) had much higher contents of phenolic hydroxyl groups than DAL (0.62 mmol•g −1 ), implying that AL and EHL had higher polarity than DAL. This resulted in different dissolution behaviors in different DESs with varying polarities. However, the sulfonate groups afforded KL with much higher polarity, thus resulting in the special dissolution behavior of KL. It is to be noted that not all cases of dissolving lignin in the developed DESs conformed to the above rules. Therefore, it is necessary to further explore the effect of the properties of the DESs on the dissolution of different lignins. Choline chloride was the preferred HBA to construct DESs with good performance and adaptability to lignin dissolution, whereas suitable acidity enabled benzoic acid and ethyl gallate to be favorable HBDs. Systematic investigation revealed that an efficient DES for lignin dissolution should possess stronger hydrogen-bonding acidity (α > 0.95) and appropriate polarity matching with the dissolved lignin. In addition, the pKa value of the HBD and the acidity of the DESs were also efficient indices for estimating the performance of an acidic DES in dissolving lignin, and the pKa value and acidity could be well correlated with the polarity. Generally, HBDs (e.g., BA and EG in this study) with moderate pKa values can be employed to construct robust DESs to dissolve lignin with satisfactory solubility. Additionally, the viscosity of the DESs should have an impac...

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“…They are produced at high individual yields as primary products [9–20] . RCF also isolates high‐quality pulps from lignocellulosic materials [13,21,22] . Most of the research efforts put into the RCF process have focused on maximizing the yield of monomer products and controlling the degree of functionalization on the alkyl sidechain.…”

Section: Introductionmentioning

confidence: 99%

Lignin Stabilization and Carbohydrate Nature in H‐transfer Reductive Catalytic Fractionation: The Role of Solvent Fractionation of Lignin Oil in Structural Profiling**

2022

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Reductive Catalytic Fractionation (RCF) of lignocellulosic materials produces lignin oil rich in monomer products and high‐quality cellulosic pulps. RCF lignin oil also contains lignin oligomers/polymers and hemicellulose‐derived carbohydrates. The variety of components makes lignin oil a complex matrix for analytical methods. As a result, the signals are often convoluted and overlapped, making detecting and quantifying key intermediates challenging. Therefore, to investigate the mechanisms underlining lignin stabilization and elucidate the structural features of carbohydrates occurring in the RCF lignin oil, fractionation methods reducing the RCF lignin oil complexity are required. This report examines the solvent fractionation of RCF lignin oil as a facile method for producing lignin oil fractions for advanced characterization. Solvent fractionation uses small volumes of environmentally benign solvents (methanol, acetone, and ethyl acetate) to produce multigram lignin fractions comprising products in different molecular weight ranges. This feature allows the determination of structural heterogeneity across the entire molecular weight distribution of the RCF lignin oil by high‐resolution HSQC NMR spectroscopy. This study provides detailed insight into the role of the hydrogenation catalyst (Raney Ni) in stabilizing lignin fragments and defining the structural features of hemicellulose‐derived carbohydrates in lignin oil obtained by the H‐transfer RCF process.

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Lignin-first biorefining of Nordic poplar to produce cellulose fibers could displace cotton production on agricultural lands

Cited by 41 publications

References 64 publications

A high-solid DES pretreatment using never-dried biomass as the starting material: towards high-quality lignin fractionation

A high-solid DES pretreatment using never-dried biomass as the starting material: towards high-quality lignin fractionation

Biomass-Based Acidic Deep Eutectic Solvents for Efficient Dissolution of Lignin: Towards Performance and Mechanism Elucidation

Lignin Stabilization and Carbohydrate Nature in H‐transfer Reductive Catalytic Fractionation: The Role of Solvent Fractionation of Lignin Oil in Structural Profiling**

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