| 1. |
- Abdelaziz, Omar Y., et al.
(författare)
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On the Oxidative Valorization of Lignin to High-Value Chemicals : A Critical Review of Opportunities and Challenges
- 2022
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 15:20
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Forskningsöversikt (refereegranskat)abstract
- The efficient valorization of lignin is crucial if we are to replace current petroleum-based feedstock and establish more sustainable and competitive lignocellulosic biorefineries. Pulp and paper mills and second-generation biorefineries produce large quantities of low-value technical lignin as a by-product, which is often combusted on-site for energy recovery. This Review focuses on the conversion of technical lignins by oxidative depolymerization employing heterogeneous catalysts. It scrutinizes the current literature describing the use of various heterogeneous catalysts in the oxidative depolymerization of lignin and includes a comparison of the methods, catalyst loadings, reaction media, and types of catalyst applied, as well as the reaction products and yields. Furthermore, current techniques for the determination of product yields and product recovery are discussed. Finally, challenges and suggestions for future approaches are outlined.
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| 2. |
- Argyropoulos, Dimitris D. S., et al.
(författare)
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Kraft Lignin: A Valuable, Sustainable Resource, Opportunities and Challenges
- 2023
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Ingår i: ChemSusChem. - : John Wiley and Sons Inc. - 1864-5631 .- 1864-564X. ; 16:23
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Forskningsöversikt (refereegranskat)abstract
- Kraft lignin, a by-product from the production of pulp, is currently incinerated in the recovery boiler during the chemical recovery cycle, generating valuable bioenergy and recycling inorganic chemicals to the pulping process operation. Removing lignin from the black liquor or its gasification lowers the recovery boiler load enabling increased pulp production. During the past ten years, lignin separation technologies have emerged and the interest of the research community to valorize this underutilized resource has been invigorated. The aim of this Review is to give (1) a dedicated overview of the kraft process with a focus on the lignin, (2) an overview of applications that are being developed, and (3) a techno-economic and life cycle asseeements of value chains from black liquor to different products. Overall, it is anticipated that this effort will inspire further work for developing and using kraft lignin as a commodity raw material for new applications undeniably promoting pivotal global sustainability concerns.
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| 3. |
- Budnyak, Tetyana M., et al.
(författare)
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Lignin-Inorganic Interfaces : Chemistry and Applications from Adsorbents to Catalysts and Energy Storage Materials
- 2020
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 13:17, s. 4344-4355
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Forskningsöversikt (refereegranskat)abstract
- Lignin is one the most fascinating natural polymers due to its complex aromatic‐aliphatic structure. Phenolic hydroxyl and carboxyl groups along with other functional groups provide technical lignins with reactivity and amphiphilic character. Many different lignins have been used as functional agents to facilitate the synthesis and stabilization of inorganic materials. Herein, the use of lignin in the synthesis and chemistry of inorganic materials in selected applications with relevance to sustainable energy and environmental fields is reviewed. In essence, the combination of lignin and inorganic materials creates an interface between soft and hard materials. In many cases it is either this interface or the external lignin surface that provides functionality to the hybrid and composite materials. This Minireview closes with an overview on future directions for this research field that bridges inorganic and lignin materials for a more sustainable future.
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| 4. |
- Galkin, Maxim V., et al.
(författare)
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Lignin Valorization through Catalytic Lignocellulose Fractionation : A Fundamental Platform for the Future Biorefinery
- 2016
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 9:13, s. 1544-1558
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Forskningsöversikt (refereegranskat)abstract
- Current processes for the fractionation of lignocellulosic biomass focus on the production of high-quality cellulosic fibers for paper, board, and viscose production. The other fractions that constitute a major part of lignocellulose are treated as waste or used for energy production. The transformation of lignocellulose beyond paper pulp to a commodity (e.g., fine chemicals, polymer precursors, and fuels) is the only feasible alternative to current refining of fossil fuels as a carbon feedstock. Inspired by this challenge, scientists and engineers have developed a plethora of methods for the valorization of biomass. However, most studies have focused on using one single purified component from lignocellulose that is not currently generated by the existing biomass fractionation processes. A lot of effort has been made to develop efficient methods for lignin depolymerization. The step to take this fundamental research to industrial applications is still a major challenge. This review covers an alternative approach, in which the lignin valorization is performed in concert with the pulping process. This enables the fractionation of all components of the lignocellulosic biomass into valorizable streams. Lignocellulose fractions obtained this way (e.g., lignin oil and glucose) can be utilized in a number of existing procedures. The review covers historic, current, and future perspectives, with respect to catalytic lignocellulose fractionation processes.
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| 5. |
- Kärkäs, Markus D.
(författare)
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Lignin Hydrogenolysis: Improving Lignin Disassembly through Formaldehyde Stabilization
- 2017
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Ingår i: ChemSusChem. - : Wiley-VCH Verlagsgesellschaft. - 1864-5631 .- 1864-564X. ; 10:10, s. 2111-2115
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Forskningsöversikt (refereegranskat)abstract
- Lignocellulosic biomass is available in large quantities and constitutes an attractive feedstock for the sustainable production of bulk and fine chemicals. Although methods have been established for the conversion of its cellulosic fractions, valorization of lignin has proven to be challenging. The difficulty in disassembling lignin originates from its heterogeneous structure and its propensity to undergo skeletal rearrangements and condensation reactions during biorefinery fractionation or biomass pretreatment processes. A strategy for hindering the generation of these resistive interunit linkages during biomass pretreatment has now been devised using formaldehyde as a stabilizing agent. The developed method when combined with Ru/C‐catalyzed hydrogenolysis allows for efficient disassembly of all three biomass fractions: (cellulose, hemicellulose, and lignin) and suggests that lignin upgrading can be integrated into prevailing biorefinery schemes.
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| 6. |
- Liao, Rong-Zhen, et al.
(författare)
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Quantum Chemical Modeling of Homogeneous Water Oxidation Catalysis
- 2017
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 10:22, s. 4236-4263
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Forskningsöversikt (refereegranskat)abstract
- The design of efficient and robust water oxidation catalysts has proven challenging in the development of artificial photosynthetic systems for solar energy harnessing and storage. Tremendous progress has been made in the development of homogeneous transition-metal complexes capable of mediating water oxidation. To improve the efficiency of the catalyst and to design new catalysts, a detailed mechanistic understanding is necessary. Quantum chemical modeling calculations have been successfully used to complement the experimental techniques to suggest a catalytic mechanism and identify all stationary points, including transition states for both O-O bond formation and O-2 release. In this review, recent progress in the applications of quantum chemical methods for the modeling of homogeneous water oxidation catalysis, covering various transition metals, including manganese, iron, cobalt, nickel, copper, ruthenium, and iridium, is discussed.
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| 7. |
- Margalef, Jèssica, et al.
(författare)
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Assessing Methodologies to Synthesize α-Sulfenylated Carbonyl Compounds by Green Chemistry Metrics
- 2021
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 14:3, s. 808-823
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Forskningsöversikt (refereegranskat)abstract
- alpha-Sulfenylated carbonyl compounds are important both as active pharmaceutical ingredients and as intermediates in organic synthesis. Owing to their relevance in synthetic organic chemistry, this Minireview focuses on assessing the most relevant synthetic procedures based on green chemistry metrics. The Minireview starts with the traditional routes and then focuses on more recently developed methodologies. These routes include sulfenylating reagents using organocatalysis, cross-dehydrogenative couplings using in situ halogenations to prevent reactive intermediates in high concentrations, oxidative couplings using terminal oxidants such as DDQ or TEMPO, and redox-neutral couplings using transition metal catalysis. These methodologies have been evaluated on the basis of atom economy, E factor, and the safety and toxicity of the transformations and the solvents used. Besides using green metrics to evaluate these novel methodologies, the synthetic utility is also assessed with regard to the availability of starting materials and the generality of the reactions. This Minireview aims to inspire researchers to apply green assessments to other methodologies and also for them to take measures to increase the greenness of their developed transformations.
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| 8. |
- Sapountzaki, Eleftheria, et al.
(författare)
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Renewable Hydrogen Production and Storage Via Enzymatic Interconversion of CO2 and Formate with Electrochemical Cofactor Regeneration
- 2023
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Ingår i: ChemSusChem. - : John Wiley & Sons. - 1864-5631 .- 1864-564X. ; 16:17
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Forskningsöversikt (refereegranskat)abstract
- The urgent need to reduce CO2 emissions has motivated the development of CO2 capture and utilization technologies. An emerging application is CO2 transformation into storage chemicals for clean energy carriers. Formic acid (FA), a valuable product of CO2 reduction, is an excellent hydrogen carrier. CO2 conversion to FA, followed by H2 release from FA, are conventionally chemically catalyzed. Biocatalysts offer a highly specific and less energy-intensive alternative. CO2 conversion to formate is catalyzed by formate dehydrogenase (FDH), which usually requires a cofactor to function. Several FDHs have been incorporated in bioelectrochemical systems where formate is produced by the biocathode and the cofactor is electrochemically regenerated. H2 production from formate is also catalyzed by several microorganisms possessing either formate hydrogenlyase or hydrogen-dependent CO2 reductase complexes. Combination of these two processes can lead to a CO2-recycling cycle for H2 production, storage, and release with potentially lower environmental impact than conventional methods.
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| 9. |
- Tian, Haining
(författare)
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Molecular Catalyst Immobilized Photocathodes for Water/Proton and Carbon Dioxide Reduction
- 2015
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Ingår i: ChemSusChem. - Wiley : Wiley. - 1864-5631 .- 1864-564X. ; 8:22, s. 3746-3759
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Forskningsöversikt (refereegranskat)abstract
- As one of the components in a tandem photoelectrochemical cell for solar-fuel production, the photocathode carries out the reduction reaction to convert solar light and the corresponding substrate (e.g., proton and CO2) into target fuels. Immobilizing molecular catalysts onto the photocathode is a promising strategy to enhance the interfacial electron/hole-transfer process and to improve the stability of the catalysts. Furthermore, the molecular catalysts are beneficial in improving the selectivity of the reduction reaction, particularly for CO2 reduction. On the photocathode, the binding mode of the catalysts and the arrangement between the photosensitizer and the catalyst also play crucial roles in the performance and stability of the final device. How to firmly and effectively immobilize the catalyst on the photoelectrode is now becoming a scientific question. Recent publications on molecular catalyst immobilized photocathodes are therefore surveyed.
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