Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques

In recent years, studies focusing on the conversion of renewable lignin-derived oxygenates (LDOs) have emphasized their potential as alternatives to fossil-based products. However, LDOs, existing as complex aromatic mixtures with diverse oxygen-containing functional groups, pose a challenge as they...

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Main Authors: Xinru Wu, Hongwei Zhang, Cejun Hu, Xiaojun Bao, Pei Yuan
Format: Article
Language:English
Published: KeAi Communications Co., Ltd. 2025-02-01
Series:Green Energy & Environment
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Online Access:http://www.sciencedirect.com/science/article/pii/S2468025724001341
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author Xinru Wu
Hongwei Zhang
Cejun Hu
Xiaojun Bao
Pei Yuan
author_facet Xinru Wu
Hongwei Zhang
Cejun Hu
Xiaojun Bao
Pei Yuan
author_sort Xinru Wu
collection DOAJ
description In recent years, studies focusing on the conversion of renewable lignin-derived oxygenates (LDOs) have emphasized their potential as alternatives to fossil-based products. However, LDOs, existing as complex aromatic mixtures with diverse oxygen-containing functional groups, pose a challenge as they cannot be easily separated via distillation for direct utilization. A promising solution to this challenge lies in the efficient removal of oxygen-containing functional groups from LDOs through hydrodeoxygenation (HDO), aiming to yield biomass products with singular components. However, the high dissociation energy of the carbon–oxygen bond, coupled with its similarity to the hydrogenation energy of the benzene ring, creates a competition between deoxygenation and benzene ring hydrogenation. Considering hydrogen consumption and lignin properties, the preference is directed towards generating aromatic hydrocarbons rather than saturated components. Thus, the goal is to selectively remove oxygen-containing functional groups while preserving the benzene ring structure. Studies on LDOs conversion have indicated that the design of active components and optimization of reaction conditions play pivotal roles in achieving selective deoxygenation, but a summary of the correlation between these factors and the reaction mechanism is lacking. This review addresses this gap in knowledge by firstly summarizing the various reaction pathways for HDO of LDOs. It explores the impact of catalyst design strategies, including morphology modulation, elemental doping, and surface modification, on the adsorption–desorption dynamics between reactants and catalysts. Secondly, we delve into the application of advanced techniques such as spectroscopic techniques and computational modeling, aiding in uncovering the true active sites in HDO reactions and understanding the interaction of reactive reactants with catalyst surface-interfaces. Additionally, fundamental insights into selective deoxygenation obtained through these techniques are highlighted. Finally, we outline the challenges that lie ahead in the design of highly active and selective HDO catalysts. These challenges include the development of detection tools for reactive species with high activity at low concentrations, the study of reaction medium–catalyst interactions, and the development of theoretical models that more closely approximate real reaction situations. Addressing these challenges will pave the way for the development of efficient and selective HDO catalysts, thus advancing the field of renewable LDOs conversion.
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spelling doaj-art-daddbd2afca6461a9c7cc8c80af343b92025-08-20T02:43:39ZengKeAi Communications Co., Ltd.Green Energy & Environment2468-02572025-02-0110229232110.1016/j.gee.2024.05.004Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniquesXinru Wu0Hongwei Zhang1Cejun Hu2Xiaojun Bao3Pei Yuan4National Engineering Research Center of Chemical Fertilizer Catalyst, College of Chemical Engineering, Fuzhou University, Fuzhou, 350002, ChinaNational Engineering Research Center of Chemical Fertilizer Catalyst, College of Chemical Engineering, Fuzhou University, Fuzhou, 350002, ChinaCollege of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China; Corresponding authors.National Engineering Research Center of Chemical Fertilizer Catalyst, College of Chemical Engineering, Fuzhou University, Fuzhou, 350002, China; Qingyuan Innovation Laboratory, Quanzhou, 362801, ChinaNational Engineering Research Center of Chemical Fertilizer Catalyst, College of Chemical Engineering, Fuzhou University, Fuzhou, 350002, China; Qingyuan Innovation Laboratory, Quanzhou, 362801, China; Corresponding authors.In recent years, studies focusing on the conversion of renewable lignin-derived oxygenates (LDOs) have emphasized their potential as alternatives to fossil-based products. However, LDOs, existing as complex aromatic mixtures with diverse oxygen-containing functional groups, pose a challenge as they cannot be easily separated via distillation for direct utilization. A promising solution to this challenge lies in the efficient removal of oxygen-containing functional groups from LDOs through hydrodeoxygenation (HDO), aiming to yield biomass products with singular components. However, the high dissociation energy of the carbon–oxygen bond, coupled with its similarity to the hydrogenation energy of the benzene ring, creates a competition between deoxygenation and benzene ring hydrogenation. Considering hydrogen consumption and lignin properties, the preference is directed towards generating aromatic hydrocarbons rather than saturated components. Thus, the goal is to selectively remove oxygen-containing functional groups while preserving the benzene ring structure. Studies on LDOs conversion have indicated that the design of active components and optimization of reaction conditions play pivotal roles in achieving selective deoxygenation, but a summary of the correlation between these factors and the reaction mechanism is lacking. This review addresses this gap in knowledge by firstly summarizing the various reaction pathways for HDO of LDOs. It explores the impact of catalyst design strategies, including morphology modulation, elemental doping, and surface modification, on the adsorption–desorption dynamics between reactants and catalysts. Secondly, we delve into the application of advanced techniques such as spectroscopic techniques and computational modeling, aiding in uncovering the true active sites in HDO reactions and understanding the interaction of reactive reactants with catalyst surface-interfaces. Additionally, fundamental insights into selective deoxygenation obtained through these techniques are highlighted. Finally, we outline the challenges that lie ahead in the design of highly active and selective HDO catalysts. These challenges include the development of detection tools for reactive species with high activity at low concentrations, the study of reaction medium–catalyst interactions, and the development of theoretical models that more closely approximate real reaction situations. Addressing these challenges will pave the way for the development of efficient and selective HDO catalysts, thus advancing the field of renewable LDOs conversion.http://www.sciencedirect.com/science/article/pii/S2468025724001341HydrodeoxygenationLignin-derived oxygenatesTargeted deoxidationCatalyst designTechniques and theoretical calculation
spellingShingle Xinru Wu
Hongwei Zhang
Cejun Hu
Xiaojun Bao
Pei Yuan
Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques
Green Energy & Environment
Hydrodeoxygenation
Lignin-derived oxygenates
Targeted deoxidation
Catalyst design
Techniques and theoretical calculation
title Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques
title_full Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques
title_fullStr Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques
title_full_unstemmed Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques
title_short Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques
title_sort advances in enhancing hydrodeoxygenation selectivity of lignin derived oxygenates from synthetic strategies to fundamental techniques
topic Hydrodeoxygenation
Lignin-derived oxygenates
Targeted deoxidation
Catalyst design
Techniques and theoretical calculation
url http://www.sciencedirect.com/science/article/pii/S2468025724001341
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AT cejunhu advancesinenhancinghydrodeoxygenationselectivityofligninderivedoxygenatesfromsyntheticstrategiestofundamentaltechniques
AT xiaojunbao advancesinenhancinghydrodeoxygenationselectivityofligninderivedoxygenatesfromsyntheticstrategiestofundamentaltechniques
AT peiyuan advancesinenhancinghydrodeoxygenationselectivityofligninderivedoxygenatesfromsyntheticstrategiestofundamentaltechniques