Article
Chemistry, Multidisciplinary
Ngoc Tuan Tran, Youngpyo Ko, Sungsoo Kim, Janghyuk Moon, Jae-Wook Choi, Kwang Ho Kim, Chang Soo Kim, Jeong-Myeong Ha, Heesuk Kim, Keunhong Jeong, Hyunjoo Lee, Chun-Jae Yoo
Summary: In this study, microwave irradiation was used for the phenolation of acid-insoluble Klason lignin. Microwave irradiation significantly reduced the reaction temperature and time without affecting the chemical structure of the phenolated lignin. Increasing the reaction temperature led to lignin decomposition, crosslinking, and phenolation. Increasing the phenol-to-lignin ratio enhanced lignin fragmentation and decreased molecular weight and glass transition temperature of the phenolated lignin. Density functional theory was used to explain the thermal and non-thermal effects of the electromagnetic field on the phenolation of Klason lignin. Phenolation greatly improved the solubility of Klason lignin in tetrahydrofuran and methanol, allowing for its adhesive application on various substrates.
Article
Engineering, Environmental
Wangqiyue Sun, Tamar L. Greaves, Maazuza Z. Othman
Summary: Inorganic additives such as NaCl and water were found to enhance the electro-assisted organosolv pretreatment process, allowing it to be completed in 30 minutes at 25% biomass loading. The residual biomass produced significant amounts of reducing sugar (up to 204.4 mg/g), approximately 10-fold higher than untreated biomass, while the regenerated solvent showed only a minor decrease (10%) in total reducing sugar yield after four cycles of recycling.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Nanoscience & Nanotechnology
Fangfang Su, Jinliang Xie, Xiaoqian Li, Zhongjie He, Hongni Wang, Jing Zhang, Yangyang Xin, Aibo Zhang, Dongdong Yao, Yaping Zheng
Summary: Solar energy, as a renewable energy, has received extensive attention, especially in the field of solar thermal utilization. Nanofluid-based direct absorption solar collectors (DASCs) are considered an important alternative method for improving solar thermal efficiency. This study proposes a novel Ti3C2Tx-IL-based nanofluid with excellent stability, wide spectrum absorption, and efficient solar energy conversion performance. The nanofluids maintain liquid state in a wide temperature range and exhibit low viscosity. Preliminary exploration of their application in photosensitive inks shows potential in fields such as injectable biomedical materials and anti-ice coatings.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Energy & Fuels
Wan Suzaini Wan Hamzah, Chong Fai Kait, Nurul Asyikin Baharuddin, Asyraf Hanim Abdul Rahim, Khairulazhar Jumbri, Cecilia Devi Wilfred, Zakaria Man, Alamin Idris
Summary: This study aims to optimize the parametric microwave conditions for the catalytic degradation of lignin model compounds, and found that microwave-assisted conversion in imidazolium-based ionic liquids is more promising than conventional methods.
BIOMASS CONVERSION AND BIOREFINERY
(2023)
Article
Chemistry, Analytical
Lijuan Zhang, Cheolyong Choi, Hiroshi Machida, Koyo Norinaga
Summary: The study proposes an integrated process for valorizing lignin, which involves catalytic hydrogenation and subsequent fast pyrolysis. Hydrogenated lignin shows increased reactivity in thermal decomposition, with higher yields of light olefins and promotion of alkanes, benzene, and toluene formation. This novel and efficient pretreatment method provides valuable insights for future research on lignin valorization.
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
(2021)
Article
Engineering, Environmental
Filippo Brienza, Korneel Van Aelst, Francois Devred, Delphine Magnin, Maxim Tschulkow, Philippe Nimmegeers, Steven Van Passel, Bert F. Sels, Patrick Gerin, Damien P. Debecker, Iwona Cybulska
Summary: This study discusses a dithionite-assisted organosolv fractionation (DAOF) method for the conversion of lignocellulose into cellulosic pulp and mono-/oligo-aromatics. The results show that DAOF is a viable fractionation method for the sustainable upgrading of lignocellulosic biomass.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Agricultural Engineering
Anindita Das, Kaustubha Mohanty
Summary: In order to achieve a sustainable biorefinery, reducing the recalcitrance of lignocellulosic biomass is crucial. This study investigated an integrated pretreatment method to recover high-quality lignin and cellulose-rich pulp. Optimization studies showed that ultrasound treatment combined with organosolv pretreatment resulted in high lignin yield and purity. Ultrasound treatment enhanced delignification and increased cellulose crystallinity, maintaining the quality of lignin. The extracted lignin contained a significant amount of β-O-4 linkages, which is favorable for downstream valorization.
BIORESOURCE TECHNOLOGY
(2023)
Article
Materials Science, Paper & Wood
Eun-Ah Lee, Jeong-Ki Kim, Rajkumar Bandi, Ramakrishna Dadigala, Song-Yi Han, Gu-Joong Kwon, Jaegyoung Gwon, Won-Jae Youe, Ji-Soo Park, Chan-Woo Park, Nam-Hun Kim, Seung-Hwan Lee
Summary: Ionic liquids have been widely used for lignocellulose fractionation and lignin isolation, and this study explored the chemical structure of lignin isolated by imidazolium based ILs. The study found that increasing the treatment temperature led to higher lignin yield but lower molecular weight and hydroxyl group content. Esterification of the isolated lignin with [EMIM]Ac was successful and extended its applicability.
Review
Agricultural Engineering
Chihe Sun, Guojie Song, Zhenying Pan, Maobing Tu, Mahshid Kharaziha, Xueming Zhang, Pau-Loke Show, Fubao Sun
Summary: The valorization of organosolv pretreatment (OP) is essential for the industrialization of enzyme-mediated lignocellulosic biorefinery. Recent studies have shown that OP can modify the soluble components into valuable active compounds, such as organosolv modified lignin (OML) and organosolv modified sugars (OMSs), while protecting them from degradation. OML can be transformed into phenolic compounds with a highly reactive lignin structure, while OMSs have potential applications in cosmetics, foods, and healthcare. The valorization of these active compounds in OP holds great promise for cost reduction. The review covers recent advances in organosolv modified components and discusses future challenges.
BIORESOURCE TECHNOLOGY
(2023)
Article
Agricultural Engineering
Yongjian Zhang, Thomas L. Eberhardt, Bo Cai, Mingqi Wu, Xiangxin Xu, Junfeng Feng, Hui Pan
Summary: A pilot scale microwave fractionation system (PMFS) was developed for the organosolv fractionation of bamboo sawdust. The PMFS achieved higher lignin and hemicellulose removal rates without serious cellulose degradation. The recovered lignin had a relatively narrow molecular weight distribution and the process showed good utilization efficiency of the bamboo feedstock.
INDUSTRIAL CROPS AND PRODUCTS
(2022)
Review
Chemistry, Multidisciplinary
Bram Jacobs, Yawen Yao, Ine Van Nieuwenhove, Dhanjay Sharma, Geert-Jan Graulus, Katrien Bernaerts, An Verberckmoes
Summary: The anthropologic impact on climate has reached a critical level due to reliance on non-renewable fossil resources. Lignins can help transition towards a sustainable and green approach. However, incorporating lignins alone is insufficient; the entire process from lignin biomass to final product needs to be considered. This review presents an assessment of valorization strategies, solvents, lignin modification and depolymerization strategies, as well as processing methods for lignins.
Article
Agricultural Engineering
Xudong Liu, Florent P. Bouxin, Jiajun Fan, Richard Gammons, Vitaliy L. Budarin, Changwei Hu, James H. Clark
Summary: By utilizing Fe(OTf)(3) as a Lewis acid and combining it with microwave heating, efficient delignification and depolymerization of lignin in birch sawdust were achieved, resulting in a high yield of monophenolic compounds.
INDUSTRIAL CROPS AND PRODUCTS
(2021)
Article
Engineering, Chemical
Carlos A. Vega-Aguilar, Carina Costa, Maria Filomena Barreiro, Alirio E. Rodrigues
Summary: This study investigates the utilization of microwave-assisted reaction for the wet peroxide oxidation of lignins. The results show that the TS-1 catalyst improves the yield of succinic acid from lignins. Additionally, microwave heating enhances the conversion of Lignol lignin to malic acid, making it an attractive method for future valorization.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Agricultural Engineering
Carlos A. Pena, Lina F. Ballesteros, Hector Rodriguez, Eva Rodil, Jose A. Teixeira, Michele Michelin
Summary: This study investigates the valorisation of lignin in a biorefinery based on lignocellulosic biomass by treating technical lignin with recombinant laccase and mediator. The treatment resulted in a preferential reduction of guaiacyl units in the recovered lignin. Phenolic compounds deriving from guaiacyl or p-hydroxyphenyl units were identified in the aqueous phases, with higher concentrations observed when an ionic liquid was involved in the treatment.
BIOMASS & BIOENERGY
(2023)
Article
Biochemistry & Molecular Biology
Elodie Melro, Alexander Riddell, Diana Bernin, Ana M. Rosa da Costa, Artur J. M. Valente, Filipe E. E. Antunes, Anabela Romano, Magnus Norgren, Bruno Medronho
Summary: Levulinic acid was used as a green solvent to selectively extract high-quality lignin from pine wood sawdust. The addition of catalytic concentrations of inorganic acids significantly reduced the extraction temperature and time without compromising the purity of the lignin. This environmentally friendly procedure shows promise in replacing traditional less sustainable methodologies.
Article
Agricultural Engineering
Oscar Oyola-Rivera, Jiayue He, George W. Huber, James A. Dumesic, Nelson Cardona-Martinez
Summary: This study investigated the catalytic conversion of cellulose to levoglucosenone (LGO) using a combination of dilute sulfuric acid and propylsulfonic acid functionalized SBA-15 (PS-SBA-15) in tetrahydrofuran (THF). The addition of small amounts of liquid acid catalyst such as sulfuric acid was found to complement the use of solid acid catalyst for cellulose conversion, leading to an increase in LGO yield. The main role of the solid Bronsted acid catalyst was to dehydrate the generated levoglucosan (LGA) into LGO, demonstrating a more environmentally friendly approach for LGO production.
BIOMASS & BIOENERGY
(2022)
Article
Chemistry, Multidisciplinary
Weizi Zhang, Xinxin Li, Shaoru Liu, Jianhao Qiu, Jiahuan An, Jianfeng Yao, Songlin Zuo, Bo Zhang, Haian Xia, Changzhi Li
Summary: In this study, Ag/TiO2 materials with different interfacial structures were prepared and used for the photocatalytic conversion of biomass-derived 5-HMF to value-added HMFCA. It was found that low-temperature reduction could enhance the photoinduced charge separation efficiency and the localized surface plasmon resonance effects. The 2.5% Ag/TiO2-LTR showed the highest HMFCA selectivity of 96.7% under visible-light illumination. However, the photocatalytic efficiency decreased significantly when the reduction temperature increased due to the encapsulation of Ag NPs by a thicker TiOx overlay.
Article
Chemistry, Multidisciplinary
Elise B. Gilcher, Hochan Chang, George W. Huber, James A. Dumesic
Summary: The hydrogenation of a biomass-derived platform molecule, 5-hydroxymethyl furfural (HMF)-acetone-HMF (HAH), was studied over Pd, Ru, and Cu based catalysts at temperatures ranging from 313-393 K. Different catalysts exhibited varying levels of selectivity and reaction pathways for hydrogenation. Kinetic modeling was used to quantify the behavior of the hydrogenation reactions. This study provides insights for optimizing catalyst selection and reaction conditions to improve the yield of hydrogenation products.
Article
Chemistry, Multidisciplinary
Raka G. Dastidar, Peter H. Galebach, Michael P. Lanci, Chengrong Wang, Yi Du, George W. Huber
Summary: Cellulose upgrading with methanol to produce fuel-range alcohols involves complex reactions, such as C-C coupling, C-O scission, and C-C scission, as observed in the conversion of 1,2-propanediol and methanol over CuMgAlOx catalyst. The selectivity of different products is influenced by the reaction orders with respect to hydrogen, 1,2-propanediol, and methanol, as well as the apparent activation energies for various pathways. The rate determining step in C-C coupling is found to be associated with the nucleophilic attack by 1,2-propanediol, and the co-feeding of formaldehyde affects the rates of C-C coupling, direct C-C scission, and esterification reactions.
Article
Chemistry, Physical
Paolo A. Cuello-Penaloza, Raka G. Dastidar, Shao-Chun Wang, Yi Du, Michael P. Lanci, Bradley Wooler, Christine E. Kliewer, Ive Hermans, James A. Dumesic, George W. Huber
Summary: A series of calcined MgAl mixed metal oxide catalysts with low Cu loadings were tested for ethanol oligomerization to distillate-range molecules. The low Cu loading catalysts showed high selectivity to linear chain alcohols and esters, with diesel fuel precursor selectivities over 75%.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Biotechnology & Applied Microbiology
Lisa Je, George W. Huber, Reid C. Van Lehn, Victor M. Zavala
Summary: Computational workflows combining molecular dynamics simulations and data-centric methods can expedite the screening and analysis of solvent systems. By utilizing data representations derived from MD simulations, DC techniques enable predictive modeling and experimental design for solvent effects on reaction outcomes.
CURRENT OPINION IN CHEMICAL ENGINEERING
(2022)
Article
Engineering, Chemical
Tianjin Li, Bo Chen, Meifang Cao, Xinping Ouyang, Xueqing Qiu, Changzhi Li
Summary: A single-atom catalyst Ni@N-C was successfully designed using a chelation-anchored strategy, which showed high activity and achieved a high yield of aromatic compounds in lignin depolymerization.
Article
Chemistry, Multidisciplinary
Feng Cheng, Sarah Liu, Steven D. Karlen, Hoon Kim, Fachuang Lu, John Ralph, Leida Vazquez M. Ramos, George W. Huber, James A. Dumesic
Summary: This paper describes an approach for producing high quality and high quantity of lignin through studying the structural change of lignin during treatment of poplar wood in gamma-valerolactone (GVL). The results show that multiple-step cycling of cosolvent-assisted hydrolysis can help preserve more of the virgin ether-bond structures of GVL-extracted poplar lignin.
Article
Chemistry, Multidisciplinary
Aurora del Carmen Munguia-Lopez, Dilara Goreke, Kevin L. Sanchez-Rivera, Horacio A. Aguirre-Villegas, Styliani Avraamidou, George W. Huber, Victor M. Zavala
Summary: Food packaging often uses multilayer plastic films to achieve specific food protection goals. However, the production of these films generates large amounts of unrecyclable plastic waste. A proposed technology called STRAP enables the separation and recycling of the polymers in the films. This study evaluates the environmental benefits of STRAP compared to virgin film production using life cycle assessment methods.
Correction
Chemistry, Multidisciplinary
Houqian Li, Horacio A. Aguirre-Villegas, Robert D. Allen, Xianglan Bai, Craig H. Benson, Gregg T. Beckham, Sabrina L. Bradshaw, Jessica L. Brown, Robert C. Brown, Victor S. Cecon, Julia B. Curley, Greg W. Curtzwiler, Son Dong, Soumika Gaddameedi, John E. Estela-Garcia, Ive Hermans, Min Soo Kim, Jiaze Ma, Lesli O. Mark, Manos Mavrikakis, Olumide O. Olafasakin, Tim A. Osswald, Konstantinos G. Papanikolaou, Harish Radhakrishnan, Marco Antonio Sanchez Castillo, Kevin L. Sanchez-Rivera, Khairun N. Tumu, Reid C. Van Lehn, Keith L. Vorst, Mark M. Wright, Jiayang Wu, Victor M. Zavala, Panzheng Zhou, George W. Huber
Summary: This article mainly discusses the chemical aspects, technology status, and challenges of expanding plastics recycling technologies.
Article
Chemistry, Multidisciplinary
Xiaohong Ren, Zhuohua Sun, Jiqing Lu, Jinling Cheng, Panwang Zhou, Xiaoqiang Yu, Zeming Rong, Changzhi Li
Summary: In this study, a novel method for upgrading biomass-derived phenolic monomers through hydrogen-free hydrodeoxygenation (HDO) was proposed and evaluated. The HDO process was combined with the activation of water and aqueous phase reforming of in situ generated methanol over a nano-porous Ni catalyst, resulting in a one-pot approach with high selectivity of bio-phenol. DFT calculations confirmed the crucial role of the Ni catalyst in activating water and facilitating the subsequent HDO process.
Article
Chemistry, Physical
Juan-Manuel Restrepo-Florez, Paolo Cuello-Penaloza, Emmanuel Canales, Dustin Witkowski, David A. Rothamer, George W. Huber, Christos T. Maravelias
Summary: This article introduces a sustainable approach of catalytic upgrading ethanol into diesel fuel through Guerbet coupling and etherification reactions, showing experimentally the feasibility of producing diesel fuel with superior properties. The use of lignocellulosic ethanol may lead to more than 50% reduction in greenhouse gas emissions, and in some instances, carbon neutral diesel fuel production is possible.
SUSTAINABLE ENERGY & FUELS
(2023)
Article
Chemistry, Physical
Weiyan Wang, Tao Xiao, Dan Wang, Hongyun Yang, Qian Qiang, Zhigang Shen, Yunquan Yang, Kui Wu, Changzhi Li
Summary: Catalysis is crucial for biomass valorization, and this study developed a robust and scalable CoS-MoS2 catalyst for efficient conversion of lignin-derived compounds into arenes. The catalyst features CoS-edge interfaces, enhancing reactant adsorption and reducing energy barriers. The catalyst showed high toluene yield and stability in deoxygenation reactions, and the preparation method can be easily scaled up without compromising activity.
Article
Engineering, Chemical
Xinxin Li, Qian Qiang, Yangming Ding, Yanan Xing, Jianwei Ji, Hua Wang, Xiaoli Pan, Bo Zhang, Changzhi Li
Summary: A recyclable Ni-ReOx/CeO2 catalyst was designed for the conversion of lignocellulosic biomass into aromatics or liquid fuels by tuning reaction parameters. The results showed that under appropriate conditions, lignin could be efficiently deconstructed into aromatic oil while cellulose and hemicellulose remained intact. Under harsher conditions, complete conversion of lignocellulosic biomass into alkanes was achieved.
CHEMICAL ENGINEERING SCIENCE
(2024)
Article
Chemistry, Physical
Haiwei Guo, Zhao Chen, Qiqi Yin, Tian Sun, Yuxuan Liu, Gengbo Ren, Changzhi Li
Summary: This study proposed a H2S-free fabrication method of bimetallic Fe-ZnS/NC using industrial lignin self S-doping, and investigated the synergistic effect of FeS and ZnS in lignin oxidation. The results showed that Fe-ZnS/NC 650 exhibited efficient oxidation activity and good S-resistance, and selectively converted lignin into carbonyl-containing aromatics under alkaline-free condition.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
