BIORESOURCE TECHNOLOGY
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2023
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IF 11.4
Jing Gao,Zhi-Qing Wang,Biao Li,Wei Zhao,Zhong-Ren Ba,Zhe-Yu Liu,Jie-Jie Huang,Yi-Tian Fang
The study reports the economic and sustainable syntheses of a lignin-based porous carbon (LPC) for CO 2 capture application. The pH values of hydrothermal solution affected the polymerization and aromatization of spheroidization, with morphological changes from blocky to microsphere. In addition, the reliable mechanisms of CO 2 adsorption were proposed by combining experiments with Gaussian16 simulations based on DFT. The electrostatic attraction of oxygen-containing functional groups and the diffusivity resistance of CO 2 in the pores are the key factors for the CO 2 adsorption. The carboxyl groups have the strongest electrostatic attraction to CO 2 . LPC-pH 1 has the highest carboxyl group content, possessing a CO 2 adsorption capacity of up to 5.10 mmol/g at 0℃, 1 bar. Furthermore, CO 2 diffusion resistance became a main factor as the adsorption temperature increases. The innovative combination of quantum chemical calculations and microscopic properties provides a viable pathway for an insight into the future control of lignin-based carbon formation.
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Daihong Gao,Denghao Ouyang,Xuebing Zhao
Lignin was oxidized and depolymerized by a direct biomass fuel cell (DBFC) for electricity generation and production of aromatic aldehydes. The yield of aromatic aldehydes could be easily controlled by changing the anodic catalyst, cathodic oxidants and external loading. Cobalt and (VO 2 ) 2 SO 4 were screened as the most suitable anodic catalyst and cathodic oxidant, respectively. A maximum power density of 199.8 mW/cm 2 was obtained under the optimized conditions for electricity generation; however, the yield of the aromatic aldehydes was greatly dependent on the type of lignin used, reaction conditions and the external loading (output voltage) of the DBFC. At a lignin concentration of 0.5 g/L, aromatic aldehydes yield of 7.8 % was obtained at an output voltage of 0.9 V. The formation of aromatic aldehydes was mainly caused by cleavage of β-O-4 linkage and oxidation of side chains by the hydroxyl radicals formed via oxidation of OH – by Co 3+ on the anode.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Lijun Guo,Liangqiong Peng,Jiheng Li,Wenhua Zhang,Bi Shi
The simultaneous removal and selective separation of U(VI) and Th(IV) via adsorption remain challenging due to their strong mobility, reactivity, and similar chemical properties. Thus, a surface-functioned lignin nanoparticle (AL-PEI) was synthesized to adsorb U(VI)/Th(IV) in a unitary system via a pH-dependent process. In alkaline solution, AL-PEI exhibited excellent adsorption performance, and the maximum adsorption capacities for U(VI) and Th(IV) reached 392 and 396 mg/g, respectively. Discrepantly in acidic solution, the adsorption performance of AL-PEI for U(VI) could still reach a high capacity (332 mg/g), whereas highly limited adsorption capacity (less than 40 mg/g) for Th(IV) was obtained, and the separation factor of U(VI) from U(VI)-Th(IV) matrix significantly reached 6662 in 3 M of the HNO 3 medium. The simultaneously efficient adsorption in alkaline solution and highly selective separation performance in acidic solution of AL-PEI also showed excellent anti-ions interference capacities, high reusability, and strong stability. This study is the first to apply lignin fabricating radiation-resistant adsorbent material, and the adsorbent displays good performance for U(VI)/Th(IV) removal and selective separation via a novel pH-dependent process, which is important to the green and sustainable development of nuclear energy and environmental protection.
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ACS Biomaterials Science & Engineering
·
2022
·
IF 5.395
Yuanxiang Xie,Chuchu Gan,Zhixian Li,Weifeng Liu,Dongjie Yang,Xueqing Qiu
Antibiotic-resistant bacteria and biofilms are among the most difficult challenges in infection treatment. Herein, lignin-copper sulfide (LS-CuS) nanocomposites were incorporated into a poly(vinyl alcohol) (PVA) hydrogel to fabricate a LS-CuS@PVA composite hydrogel with near-infrared-activated photothermal, photodynamic, and peroxidase-like performance. The antibacterial tests of LS-CuS@PVA exhibited the highest antibacterial rate that caused 3.8-log and 4.8-log reductions of colony forming units (CFUs) against Escherichia coli and Staphylococcus aureus in the presence of H2O2 under near-infrared (NIR) light irradiation for 10 min. The significantly improved bactericidal performance could be attributed to the synergistic effects of hyperthermia and reactive oxygen species (ROS). Furthermore, the LS-CuS@PVA hydrogel could eradicate the already formed biofilm and inhibit biofilm formation. Considering the highly effective antibacterial and antibiofilm activity of the LS-CuS@PVA hydrogel, this work could provide new insights for the design of poly(vinyl alcohol)-based composite hydrogels for wound healing and wound dressing.
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ENERGY & FUELS
·
2023
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IF 5.3
Xinyuan Xu,Jinqiang Zhang,Hong Wu,Lei Shi,Jie Zhang,Kuan Ding,Shu Zhang,Shuaijun Wang,Shaobin Wang,Hongqi Sun
Photoreforming of lignin has been explored as a fascinating technology to generate clean hydrogen energy and value-added aromatic monomers from biomass. However, its upscaling is impeded by unsatisfactory selectivity due to the lack of mechanistic investigations in the uncontrollable reaction pathways. Herein, we successfully controlled the concentration and position of sulfur vacancies within the ultrathin ZnIn2S4 nanosheets to optimize the photo-driven lignin model reforming process. The competition of proton transfer between the hydrogen evolution and dissociation of the β-O-4 linkage in the model compound of lignin was identified, and the modulation of the proton migration pathway was realized through S vacancy engineering in ZnIn2S4 nanosheets toward target products. As such, excellent selectivity for hydrogen and chemical monomers was achieved with a high concentration of S vacancies in the bulk and on the surface of ZnIn2S4, respectively. This study endows new mechanistic insights into the biomass photoreforming process and elucidates the structure/chemistry-catalysis correlation of ZnIn2S4 photocatalysts, which are beneficial for photocatalyst design and rational solar fuel production.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Yan-Hong Li,Fang-Jing Liu,Jia-Pei Guo,Fan Yin,Shan-Shan Gao,Yao Lu,Rui Song,Yan-Ming Yu,Juan-Juan Zheng,Yun-Peng Zhao,Ri-Guang Zhang,Zai-Xing Huang,Jing-Pei Cao,Xian-Yong Wei,Maohong Fan
Low temperature and highly selective hydrogenation of the lignin-derived aromatics to obtain high-value chemicals and clean liquid fuels is a significant step for lignin valorization in the chemical industry. Developing efficient catalysts with high activity and selectivity for hydrogenation of lignin-derived aromatic rings at low temperature remains a big challenge. Herein, a well-dispersed Ru-Fe bimetallic nanoparticle catalyst supported on porous nitrogen-doped carbon was developed through a facile impregnation method. It showed excellent catalytic activity for hydrogenation of lignin-derived aromatics, such as diaryl ethers, phenolic monomers and arenes to corresponding alicyclic compounds with high selectivity, under surprisingly mild conditions (≤50 °C, ≤2 h and 1 MPa H 2 ). Hydrogenation of aromatic rings took precedence over the cleavage of C-O bond for the lignin-derived aromatics. The resulting alicyclic compounds are key raw materials for synthesizing polymer, pharmaceutical intermediates and resins, and clean liquid fuels. The strong interactions between metal and support improved the anti-oxidation and anti-sintering ability of the catalyst, and significantly improve the hydrogenation performance. Additionally, the phenols in the lignin oil were effectively converted into cyclohexanol and its derivatives at 90 °C over the Ru-Fe bimetallic catalyst , with selectivity up to 53.3% in the hydrogenated lignin oil. The development of this catalyst for selective hydrogenation of lignin-derived aromatics at low temperature provides a green, low carbon footprint and sustainable approach for the value-added utilization of lignin and its derivatives.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Xiaoyu Shi,Kai Wang,Shishuai Gao,Daihui Zhang,Chenhuan Lai,Can Jin,Mi Li,Chunpeng Wang,Qiang Yong,Fuxiang Chu
As lignin is one of the most abundant renewable resources, utilization to fabricate functional hydrogels has gained increasing attention. However, the heterogeneous structure and the few available functional groups of lignin limited its applications. Herein, we presented a simple strategy to synthesize gallic acid (GA)-modified lignin as a key component to prepare conductive hydrogels. The addition of GA during the organic solvent pretreatment of poplar changed the structure of lignin and increased the total content of phenolic hydroxyl groups from 3.20 to 3.89 mmol/g (EOL-G30). Moreover, the enzymatic hydrolysis of pretreated poplar was enhanced from 49.1 to 55.2% (OP-G30) at a low enzyme loading of 5 FPU/g. When using GA-modified lignin to prepare hydrogels, the resulting hydrogel exhibited excellent self-adhesion to various substrates and demonstrated effective free radical scavenging capabilities. When incorporating sodium chloride (NaCl) as conductive ions, the hydrogels exhibit reliable strain-sensing capability. Moreover, they also displayed robust functionality in a low-temperature environment (−20 °C). This study has presented valuable insights to realize in situ modification of lignin and fabricate lignin-based functional materials, offering new perspectives for the biorefinery industry.
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BIORESOURCE TECHNOLOGY
·
2021
·
IF 9.642
Xiuhua Lin,Lihui Chen,Heyu Li,Yuancai Lv,Yifan Liu,Xuebin Lu,Minghua Liu
In this study, the sinocalamus oldhami alkali lignin was depolymerized into phenolic products in a combined system by using the composite alkali and Ni-W 2 C/activated carbon (AC) as catalysts. FT-IR, GPC, TG, 2D-HSQC and GC–MS were used to analyze the composition, structure and distribution of degradation products, and the synergistic effect of metal and alkali catalysts on the depolymerization of lignin was also studied. The results showed that Ni-W 2 C/AC and composite alkali could effectively improve the catalytic degradation efficiency of lignin under mild conditions, 94.4% of lignin was converted and 17.18% of phenolic monomers were obtained under 260 °C for 5 h. In this composite system, the synergism of the basic sites, the metal active sites and the Lewis acid sites could promote the cleavage of C–O bonds in the lignin molecule and lower the char formation during the base-catalyzed solvolysis. Phenolic monomers were mainly composed of phenol, 2-methyl-phenol and p -cresol etc.
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JOURNAL OF THE ENERGY INSTITUTE
·
2021
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IF 6.186
Lin Hu,Xian-Yong Wei,Zhi-Ming Zong
Recently hydrocarbons with high yield from the selective hydrodeoxygenation (HDO) of lignin-derived bio-oil under low temperature still encounters the great challenges. However, metal nanoparticles size and acid site can greatly influence the HDO activity of metal catalyst . Herein, the efficient bifunctional Ru/Hβ catalyst was prepared by modified deposition-precipitation (DP) method for the HDO reaction of guaiacol and catalytic isoproanolysis lignin-derived bio-oil. Notably, compared to the impregnated Ru 3% /Hβ-25 catalyst, Ru 3% /Hβ-25 (DP) catalyst exhibited the higher catalytic activity on the HDO of guaiacol, smaller Ru nanoparticles size, and more acid sites. It was observed that guaiacol can be completely converted to cyclohexane under 180 °C, 3 MPa H 2 , and 2 h in n -hexane. This Ru 3% /Hβ-25 (DP) catalyst proved to be the good recyclability in the HDO reaction of guaiacol, the conversion decreased slightly to 82.3% and the yield of cyclohexane decreased to 71.2 mol% after four recycle times. Furthermore, this high active catalyst was also applied to the upgradation of bio-oil derived from the catalysis isoproanolysis of lignin in the organic phase. As a result, after the upgradation, bio-oil contained high relative content (RC) of hydrocarbons, including 42.99% cycloalkanes and 50.74% arenes, and oxygenated compounds of raw bio-oil were almost removed. Overall, during upgradation of raw lignin-derived bio-oil over Ru 3% /Hβ-25 (DP) catalyst process, not only HDO reaction, but also cleavage of C-O bonds can be achieved in one-pot.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Jiabai Cai,Huan Li,Qi Jing,Debin Li,Yangyang Zhang
To catalyze the degradation of lignin in refractory wastewater efficiently, a new nanocomposite with Ru nanoparticles embedded on the surface of TiZrO 4 hollow spheres was fabricated with three method a “sol-gel + calcination + vacuum-impregnation” template method, and the unique binary composition of TiZrO 4 /Ru prevented the aggregation of Ru and keep its high activity. During 3-h catalytic-oxidation at 160 °C and 2.0 MPa O 2 , 98% alkali lignin was degraded and 70% organic carbon was mineralized with the catalysis of TiZrO 4 /Ru, while the values were only 50% and 25% without analysts. The catalyst increased the catalytic-oxidation rate constant k 1 (h −1 ) of alkali lignin from 0.282 h −1 to 1.175 h −1 because of high-efficiency hydroxyl radical production, as determined by EPR. LC-OCD showed that the catalyst decomposed alkali lignin with molecular weight 1–2 kDa to small molecules. Butyl acetate was the main intermediate product, which should be derived from the auto synthesis of butanol and acetic acid. In addition to high conversion efficiency, the catalyst had good stability with 95% capability after five cycles. In real biogas slurry treatment, an increase of biochemical to COD ratio from 0.28 to 0.51, with obvious decoloration, indicated TiZrO 4 /Ru enhanced the biodegradability of the refractory wastewater significantly.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 20
·11508-11518
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IF 3.43
Jing Chen,Hanling Yang,Hongquan Fu,Hongyan He,Qiang Zeng,Xuehui Li
Electrochemical oxidation is a promising and effective method for lignin depolymerization owing to its selective oxidation capacity and environmental friendliness. Herein, the electrooxidation of non-phenolic alkyl aryl ether monomers and β-O-4 dimers was experimentally (by cyclic voltammetry, in situ spectroelectrochemistry, and gas chromatography-mass spectroscopy) and theoretically (by DFT calculations) explored in detail. Compared to the reported literature (T. Shiraishi, T. Takano, H. Kamitakahara and F. Nakatsubo, Holzforschung, 2012, 66(3), 303–309), 1-(4-ethoxyphenyl)ethanol showed a distinguishable oxidation pathway, where the resulting carbonyl product surprisingly underwent a bond cleavage on alkyl–aryl ether to ultimately produce a quinoid like compound. In contrast, β-O-4 dimers, like 2-phenoxy-1-phenethanol and 2-phenoxyacetophenone also demonstrated electrochemical oxidation induced by Cβ–O and Cα–Cβ bond cleavages. For the oxidation products, the presence of the Cα-hydroxyl group in dimers was the key to selectively generate aldehyde-containing species under mild electrochemical conditions, otherwise it produces alcohol-containing products following a different mechanism compared to the CαO containing dimers.
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BIORESOURCE TECHNOLOGY
·
2021
·
IF 9.642
Haichuan Zhang,Hui Zhang,Shenglong Tian,Shiyu Fu
In this work, near-complete conversion of lignocellulosic biomass and high products yields were achieved through catalytic transfer hydrogenolysis (CTH) in isopropanol using a heteropoly acid SiW 12 synergistic with Pd/C catalyst at a relatively mild condition. The performances of various heteropoly acids and catalytic conditions were extensively examined. The results confirmed that SiW 12 exhibited the highest activity on disrupting C–C linkages and C-O linkages than H 2 WO 4 , PW 12 , and PMo 12 . 34.91 wt% and 43.55 wt% monophenols were achieved for hydrogenolysis of bagasse and eucalyptus, respectively, at their optimal temperature for 5 h. Characterization studies on the lignin oil revealed that the notable structural changes were observed including the breaking of the side chain alkyl-aryl ether bonds and glycosidic bonds, while methoxyl groups were retained. Additionally, particle size of feedstock also has significant impact on the distribution and yields of the monophenols.
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