AICHE JOURNAL
·
2022
·Vol. 69
·期 2
·e17877
·
IF 4.167
Tianjin Li,Bo Chen,Meifang Cao,Xinping Ouyang,Xueqing Qiu,Changzhi Li
The efficient utilization of lignin remains a great challenge due to its complex nonrepetitive structure and the lack of efficient catalyst. Herein, a single-atom catalyst Ni@N-C was designed via a facile chelation-anchored strategy. Ni atoms were immobilized on the N-doped carbon carrier by a two-stage pyrolysis of a mixture of d -glucosamine hydrochloride, nickel acetate, and melamine. d -glucosamine hydrochloride as a chelating agent prevented the aggregation of Ni 2+ , and melamine provided enough N to anchor Ni by forming Ni–N 4 structure. Ni@N-C gave a 31.2% yield of aromatic compounds from lignin hydrogenolysis, which was twice higher than that achieved by Ni cluster catalyst. Based on the experimental and density functional theory (DFT) calculation results, the higher activity of Ni@N-C was attributed to its lower H 2 dissociation energy and the reduced energy barriers of the transition states. The strategy described opens an efficient green avenue for preparing single-atom catalyst that possesses outstanding activity in lignin depolymerization.
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INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Wei Zhang,Jiandong Shen,Pei Gao,Qixing Jiang,Wenshui Xia
Spherical lignin nanoparticles (LNPs) offer more possibilities for high value-added use of lignin, but un-ecofriendly organic solvents used for preparing LNPs must be addressed. This study reported a green and simple method to produce LNPs using a betaine:lactic acid deep eutectic solvent (DES) via self-assembly induced by dropping water. The critical water content (41 vol%) at the beginning of self-assembly was determined by dynamic light scattering. The well-defined spherical colloid particles with an average size of 57.16 ± 1.43 nm were obtained after adding 80 vol% water content, followed by verifying the morphologies via scanning electron microscopy and transmission electron microscopy . A better water dispersibility of colloid particles was elucidated by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The stable LNPs were optimized at 5 mg/mL of initial lignin concentration, 1 mL/min of dropping speed, and 80 vol% water content. Compared with lignin, LNPs exhibited improved thermal stability, enhanced antioxidant activity , and lower minimum inhibitory concentration against Staphylococcus aureus (4.0 mg/mL). Further, 7.5 mg/mL of LNPs concentration demonstrated its potentiality as a stabilizer in Pickering emulsions. Furthermore, the produced LNPs displayed high potential in bio-based materials and emulsion, providing a critical foundation for broadening the further utilization of lignin.
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GREEN CHEMISTRY
·
2022
·Vol. 24
·期 17
·6619-6630
·
IF 11.034
Haichuan Zhang,Shiyu Fu
Catalytic transfer hydrogenolysis (CTH) has emerged as a sustainable and carbon-neutral biorefinery process due to the decrease in the carbon footprint and high atom and energy efficiency. Herein, heteropoly acids (HPAs) as green catalysts were used for the CTH of Kraft lignin (KL) into lignin oil under mild conditions. It is found that all the types of HPAs, Pd/C, H-donor solvent and reaction temperature affected significantly the conversion of Kraft lignin. SiW12 and PW12, respectively, afforded 95.0% and 83.8% KL conversion in isopropanol with Pd/C at 190 °C for 5 h. However, the degradation of eucalyptus Kraft lignin (EKL) provided phenolic monomers with the highest yield of 42.6% using SiW12 and Pd/C. Molecular dynamics (MD) simulation showed that SiW12 and PW12 in isopropanol are more likely to be close to lignin compared to n-propanol. The relative average molecular weight of the obtained lignin oil ranges from 100 Da to 700 Da, including phenolic monomers, dimers and trimers. The lignin monomer products are mainly composed of guaiacols and syringols with 0 to 3 carbon side chains. The simultaneous depolymerization and deoxygenation of KL during CTH led to a high-boiling organic fraction, analyzed with a Fourier transform-ion cyclotron resonance mass spectrometer (FT-ICR MS) equipped with an electrospray negative ion source (ESI−), maintaining highly aromatic structures and having lower O/C and higher H/C ratios compared to initial lignin. This work exhibits a prospective application of the CTH for the conversion of technical lignin to chemicals and biofuels.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Pengpeng Deng,Feixiang Chen,Haodong Zhang,Yun Chen,Jinping Zhou
The abuse of antibiotics induces the emergence of drug-resistant bacteria, which greatly increases the difficulty of clinical treatment of infected wounds. It is urgent to design a multifunctional wound dressing independent of antibiotics. In this work, we designed multifunctional hydrogels based on lignin and cellulose in natural polymers. Lignin with antioxidant properties could reduce silver nanoparticles in situ and could also be used as a crosslinking agent to construct hydrogels between hydroxypropyl cellulose modified with phenylboric acid by a dynamic borate bond. Hydrogels have excellent properties such as self-healing, shape adaptability, biocompatibility, blood compatibility, antioxidant properties, excellent broad-spectrum antimicrobial properties, good tissue adhesion, and electrical conductivity. The tissue adhesion of hydrogels endows them with an excellent hemostasis property in a rat liver injury model. In vivo experiments demonstrated that hydrogels can maintain a moist healing environment, reduce inflammatory cell infiltration, promote M2 macrophage polarization, accelerate collagen deposition, promote the regeneration of new blood vessels, and significantly speed up the wound healing of methicillin-resistant Staphylococcus aureus (MRSA)-infected wounds. Therefore, these multifunctional hydrogels are an excellent candidate to treat multiple stages of wound healing and have a broad application prospect in the medical field.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Changsong Li,Yijing Li,Qiang Li,Junling Duan,Juying Hou,Qin Hou,Shiyun Ai,Houshen Li,Yuechao Yang
Phosphates and organophosphorus cause environmental pollution , and excessive phosphate leads to water eutrophication . Glyphosate , an organophosphorus herbicide, harms the environment and human health. In this study, regenerable magnetic AL/Fe 3 O 4 /La(OH) 3 adsorbents were developed by modifying Fe 3 O 4 and La(OH) 3 on aminated lignin (AL) for phosphate and glyphosate removal. The adsorption capacity for phosphate and glyphosate reached 60.36 mg g −1 and 83.87 mg g −1 when the initial concentrations were 150 mg L −1 and 250 mg L −1 , respectively. The thermodynamic data showed that adsorption is a spontaneous and endothermic process. Adsorption can be applied at pH values ranging from 3 to 11 and is more suitable under acidic conditions. Fe 3 O 4 and La(OH) 3 both enhanced the adsorption capacities of phosphate and glyphosate. Phosphate and glyphosate compete slightly when coexisting in the adsorption process at low concentrations. Due to the magnetic properties of Fe 3 O 4 , the adsorbents can be separated rapidly and effectively with an external magnetic field. 89% adsorption capacity remained after four adsorption-desorption recycles. Thus, AL/Fe 3 O 4 /La(OH) 3 shows potential for phosphate and glyphosate removal as an effective and reusable adsorbent.
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Frontiers in Bioengineering and Biotechnology
·
2021
·
IF 5.89
Guo Wen-Jie,Xu Jia-Kun,Liu Jing-Jing,Lang Jia-Jia,Gao Shu-Qin,Wen Ge-Bo,Lin Ying-Wu
The conversion of Kraft lignin in plant biomass into renewable chemicals, aiming at harvesting aromatic compounds, is a challenge process in biorefinery. Comparing to the traditional chemical methods, enzymatic catalysis provides a gentle way for the degradation of lignin. Alternative to natural enzymes, artificial enzymes have been received much attention for potential applications. We herein achieved the biodegradation of Kraft lignin using an artificial peroxidase rationally designed in myoglobin (Mb), F43Y/T67R Mb, with a covalently linked heme cofactor. The artificial enzyme of F43Y/T67R Mb has improved catalytic efficiencies at mild acidic pH for phenolic and aromatic amine substrates, including Kraft lignin and the model lignin dimer guaiacylglycerol-β-guaiacyl ether (GGE). We proposed a possible catalytic mechanism for the biotransformation of lignin catalyzed by the enzyme, based on the results of kinetic UV-Vis studies and UPLC-ESI-MS analysis, as well as molecular modeling studies. With the advantages of F43Y/T67R Mb, such as the high-yield by overexpression in E. coli cells and the enhanced protein stability, this study suggests that the artificial enzyme has potential applications in the biodegradation of lignin to provide sustainable bioresource.
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Sustainable Energy & Fuels
·
2021
·Vol. 5
·期 14
·3744-3754
·
IF 6.367
Wangda Qu,Zizhu Zhao,Jie Wang,Fengying Dong,Hui Xu,Xinzhi Sun,Hong Jin
A facile and additive-free approach was developed to synthesize pure lignin-derived porous carbon for highly flexible supercapacitor electrodes. Lignin was simply melted on a carbon cloth, and then subjected to direct laser writing (DLW). It was found that lignin was transformed into 3D porous graphene while bonding on the carbon cloth. The fabricated materials (LCE) under different laser powers were all confirmed as having a sharp (002) peak with small d002 spacing from the XRD profile, and a high IG/ID ratio from Raman spectra. The LCEs showed promising capacitive behaviors in electrochemical testing. The best LCE (i.e., LCE40) possesses a CA of 786 mF cm−2, and it was further characterized by XPS and HRTEM to determine its compositional and structural information. Moreover, LCE40 had super flexibility attributed to carbon cloth as the substrate. The CA of the LCE after bending remained at 93–97% under different current densities. When assembled into symmetric solid-state supercapacitors, the LCE40-based device showed an areal capacitance of 148.6 mF cm−2, which is much superior to all other reported laser-induced lignin-derived carbon. This one-step process is innovative and simpler than any other porous carbon fabrication and provides a method for fabricating lignin-derived flexible supercapacitors.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hao-Lin Wei,Jie Bu,Shi-Shui Zhou,Mao-Cheng Deng,Ming-Jun Zhu
This study aimed to develop a promising biorefinery technology for the value-added utilization of herb residues by using ionic liquid (IL) assisted by aromatic acid ( p -toluenesulfonic acid, TsOH) pretreatment. The result showed that the addition of low concentration of TsOH into IL could effectively deconstruct the recalcitrant intercellular structure of herb residues and rapidly extract the lignin fraction. Under the optimum conditions (79% IL, 1.0% TsOH, and 20% H 2 O at 130 °C and 2 h), the highest cellulose recovery yield of 96.4%, the lignin removal rate of 79.9% and ideal saccharification yield of 98.9% were achieved. Moreover, the main byproduct lignin exhibited comparable yield, high purity, and thermal stability, suggesting the potential application in the conversion of bio-based chemicals and materials. Furthermore, the IL was successfully recycled three times and the recovery rate was at least 95% each time. High saccharification yields and lignin recovery were maintained during all cycles. The hemicellulose-derived saccharides were the main impurities detected in the recycled IL. Overall, this work presents a novel green pretreatment process that can effectively utilize herb residues.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xue Wang,Huanxin Guo,Zonghao Lu,Xue Liu,Xiongfei Luo,Shujun Li,Shouxin Liu,Jian Li,Yongzhen Wu,Zhijun Chen
Films with the capacity for photoluminescence and haze, which can convert UV to visible light and enhance light management, are of great importance for optoelectronic devices. Here, taking advantage of the inherent fluorescence and self-assembly properties of lignin, we have developed a sustainable lignin-derived multifunctional dopant (L-MS-NPs) for fabricating optical films with haze, fluorescence, and room-temperature phosphorescence (RTP) together with poly(vinyl alcohol) (PVA). The optical films are used to improve the light-harvesting efficiency of solar cells. Specifically, attributed to the robust morphology in the film matrix, L-MS-NPs cause a rough morphology in the surface of an L-MS-NPs/PVA composite film, which eventually triggers the great optical haze. Additionally, L-MS-NPs inherit fluorescence properties from lignin and show fluorescence emission when embed in the film matrix. Moreover, the PVA film matrix can stabilize the excited triplet state, which finally induces RTP of L-MS-NPs. The combined haze, fluorescence, and RTP properties of the L-MS-NPs/PVA composite film enhances the power conversion efficiency (PCE) of dye-sensitized solar cells from ∼3.9 to ∼4.1%.
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CARBOHYDRATE POLYMERS
·
2021
·
IF 9.381
Junxian Xie,Junjun Chen,Zheng Cheng,Shiyun Zhu,Jun Xu
This study investigated the process intensification strategies for the pretreatment of Radiata Pine with the green deep eutectic solvent (DES) system composed of benzyltrimethylammonium chloride/formic acid (BTMAC/FA). The results showed that DES pretreatment drastically improved the delignification and hemicelluloses-removal capacity. The conducted process acceptably remained most of the cellulose in pretreated biomass (88.3%–91.8%). Benefiting from the overcoming of recalcitrance, the enzymatic digestibility of pretreated residues reached 92.4%. The efficient conversion was mainly ascribed to the lignin and hemicelluloses co-extraction. Meanwhile, the lignin yield and enzymatic saccharification was still largely maintained after five reuses. Further structural characteristics of lignin nanoparticles revealed that the lignin possessed high purity (95.19–97.51%), medium molecular weight (9600 to 6495 g/mol), and low polydispersity (ca 2.0), which was attributed to cleavage of ether bonds in lignin as well as linkages between lignin and hemicelluloses. Overall, this study illustrated that DES pretreatment was promising to achieve an efficient fractionation of woody biomass into fermentable glucose and high-quality lignin.
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Processes
·
2021
·Vol. 9
·期 2
·384
·
IF 2.847
Cuicui Li,Chongxing Huang,Yuan Zhao,Chaojian Zheng,Hongxia Su,Lanyu Zhang,Wanru Luo,Hui Zhao,Shuangfei Wang,Li-Jie Huang
Deep eutectic solvents (DESs) is a newly developed green solvent with low cost, easy preparation and regeneration. Because of its excellent solubility and swelling effect in lignocellulose, it has received widespread attention and recognition. In this study, choline-based deep eutectic solvents (DESs)—choline chloride-urea (CC-U), choline chloride-ethylene glycol (CC-EG), choline chloride-glycerol (CC-G), choline chloride-lactic acid (CC-LA), and choline chloride-oxalic acid (CC-OA)—were used to extract and separate bagasse. The effects of hydrogen bond donors on lignin separation and the fiber and lignin structure were investigated. All five DESs could dissolve lignin from bagasse; acidic DESs exhibited higher solubility than basic DESs. CC-OA effectively separated lignin and hemicellulose. CC-LA showed weaker lignin separation ability than CC-OA. CC-G, CC-EG, and CC-U were more inclined to selectively separate lignin than hemicellulose. The crystalline cellulose II structure was retained after DES pretreatment. Acidic DESs effectively improved the crystallinity of bagasse fiber; the crystallinities for CC-OA and CC-LA pretreatment were 62.26% and 61.65%, respectively. The lignin dissolved in DES was mainly syringyl lignin. The lignin dissolved in CC-U, CC-LA, and CC-OA contained a small amount of guaiacyl lignin.Keywords:deep eutectic solvent;bagasse;lignin;cellulose;chemical structure
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NANOTECHNOLOGY
·
2020
·Vol. 32
·期 1
·015101
·
IF 3.551
Baoe Li,Xiaomei Xia,Jiatian Chen,Dan Xia,Ruodan Xu,Xianrui Zou,Hongshui Wang,Chunyong Liang
Electrospun composite nanofibrous scaffolds have been regarded as a potential carrier for local drug delivery to prevent tumor recurrence. Herein, a model drug (paclitaxel) was creatively loaded into lignin nanoparticles (PLNPs) and then encapsulated into the polymer of poly (vinyl alcohol)/polyvinyl pyrrolidone which has been fabricated into a composite nanofibrous membrane (PVA/PVP-PLNPs) for use as a drug carrier using the electrospinning technique. The fabricated PVA/PVP-PLNPs membranes exhibited good particle distribution, mechanical properties, thermal stability and biocompatibility. In vitro experiments showed that combining lignin nanoparticles by electrospinning not only improved the drug release profile, but also enhanced the hydrophilicity of nanofibrous membranes which was beneficial to cell adhesion and proliferation. Cellular experiments demonstrated that PVA/PVP-2%PLNPs membrane showed good cell inhibition ability, and the cell survival rate was only 21% at day 7. It indicates that the as-prepared PVA/PVP-PLNPs composite nanofibers are promising candidates for local anticancer therapy.
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