JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Jianglin Liu,Jinhui Zhang,Haichao Zhou,Bowen Liu,Huafeng Dong,Xuliang Lin,Yanlin Qin
Developing noble-metal-free electrocatalysts for efficient oxygen evolution reactions (OER) is urgently desired to obtain green hydrogen by water electrolysis. Coupling FeNi catalysts with other transition metals is an effective strategy to improve the OER performance, but the electronic structure regulation of the catalytic center is challenging. Herein, heterostructures catalyst composed of MoC and FeNi alloy embedded in N -doped biochar (denoted as MoC–FeNi@NLC) was in situ synthesized by pyrolysis of lignin-metals coordination complex. MoC–FeNi@NLC displayed an overpotential of 198 mV and a long steady running time of 200 h at 10 mA·cm −2 in alkaline media. Furthermore, MoC-FeNi@NLC has demonstrated excellent Faradaic efficiency (FE) of over 90 %. A voltage of 1.50 V was required based on the MoC–FeNi@NLC and Pt/C coupling system, which was superior to that of commercial noble metal catalysts (Pt/C || Ir/C, 1.57 V). The density functional theory demonstrated that FeNi alloy balanced the adsorption energy of OER intermediates and regulated the orbital overlap of Mo above Fermi level. While the lignin-derived carbon layer prevented the deactivation and dissolution of catalytic center. The construction strategy of transition metal alloys and carbides heterojunction by the assistance of sustainable lignin derivatives and its structure–activity relationship toward OER electrocatalytic process provides a promising and cost-efficient pathway for the design of high-performance and stable OER catalysts.
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高影响因子
Biomaterials Science
·
2022
·Vol. 10
·期 15
·4284-4292
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IF 7.59
Ruixia Liu,Tingting Ding,Pingping Deng,Xiaofan Yan,Fuquan Xiong,Jienan Chen,Zhiping Wu
This work was carried out in order to broaden the application field of lignin and improve its additional value. The degraded deep eutectic solvent lignin-grafted poly(N-vinyl caprolactam) (DES-lignin-g-PNVCL) was synthesized by using modified DES-lignin and NVCL via activators regenerated by electron transfer-atom transfer radical polymerization (ARGET-ATRP). Aspirin was coated with DES-lignin-g-PNVCL through self-assembly by an ethanol/water anti-solvent method to obtain lignin thermosensitive polymer nanoparticle coated aspirin (aspirin@LTNP). X-ray electron spectroscopy (XPS), elemental analysis, scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), dynamic light scattering (DLS), and ultraviolet visible spectroscopy (UV) were used to characterize the composition, structure and morphology of DES-lignin-g-PNVCL and aspirin@LTNP. The releasing behavior of aspirin@LTNP at different temperatures and pH values was investigated. The safety was evaluated by cytotoxicity tests. The results indicated that aspirin@LTNP was mainly accumulated by the hydrophobic effect and π–π interaction in the process of self-assembly, and its morphology was an ellipsoid stacked layer by layer. The aspirin@LTNP hydrophilic chains were increased and had externally hydrophilic and internally hydrophobic structures. The particle size decreased slightly during the self-assembly process. The red-shift occurred at the π–π interaction wavelength of the lignin aromatic ring, which indicated a physical coating process. The coating rate of aspirin@LTNP was 88.87%. Aspirin@LTNP showed an obvious temperature response; the 96 h cumulative release rate at the LCST was 73.75 ± 1.16%, while the 96 h cumulative release rate above the LCST was 28.10 ± 0.92%. The 96 h cumulative release rate was 63.21 ± 0.57% at pH = 1.5 and 49.56 ± 0.48% at pH = 7.4. The dosage of aspirin@LTNP used in the experiment was safe. This study provided a strategy for drug coating and controlled release.
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高影响因子
FUEL PROCESSING TECHNOLOGY
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2022
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IF 8.129
Yuan-Yuan Yu,Zhong-Qiu Liu,Guo-Qiang Zhang,Yu-Jing Liu,Zhao-Shun Zhang,Tian-Sheng Zhao,Xian-Yong Wei,Anguo Ying
Efficient and selective conversion of lignin into aromatic monomers (AMs) is extremely essential for the economic feasibility of biorefinery . Nevertheless, the high catalytic efficiency of solid acid catalysts (SACs) for lignin conversion into AMs is remarkably weakened by the present of water produced during the above reaction leading to the deactivation and leaching of acidic sites. More importantly, the directional preparation of SACs with well-defined mesopores , hydrophobicity , and Brønsted-Lewis acidic sites still remains a grand challenge for heterogeneous catalyst development. To overcome these limitations, a desired multifunctional poly(ionic liquid)s (MFPILs) with above-mentioned structural and chemical properties were successfully constructed by an innovative synergistic regulation-induced co -polymerization. Then, MFPILs exhibit more excellent catalytic performance than poly(ionic liquid)s containing Lewis acidic site, Brønsted acidic site, or hydrophilicity alone with 47.9% conversion of lignin and 24.6 wt% yield of AMs, which is the excellent yield reported for the catalytic hydroconversion of lignin using non-precious-metal catalysts. The high catalytic performance of MFPILs for the production of lignin-derived AMs are attributed to the synergistic co-catalysis of the hydrophobic micro-environment, Brønsted-Lewis acidic sites, and mesoporous confinement, which was further confirmed by water contact angle, H 2 temperature programmed desorption , and adsorption experiment. Further, MFPILs featuring magnetic recovery properties can be recycled for at least 10 run times without a significant lower catalytic activity . The work not only sheds some light on fabricating the novel SACs, but also develops a powerful new strategy to produce lignin-derived AMs.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2022
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IF 6.449
Jinsong Wang,Farzad Seidi,Yang Huang,Huining Xiao
Incorporating corrosion inhibitors in the formulation of coatings can yield active coatings which are able to provide a sustained release of the corrosion inhibitor in the case of emergence of microcrack in the structure of the coating. Herein, we developed bio-based polyurethane sublayer coatings with strong anticorrosion performances. First, lignin-corrosion inhibitor (LCI) conjugate was obtained through conjugation of nicotinic acid to lignin through hydrolytically cleavable ester linkage to afford the steady release of low concentrations of corrosion inhibitor in case of the emergence of microcracks. Subsequently, solution polyaddition of LCI with diisocyanates and polypropylene glycol and coating on the stainless steel surface afford the polyurethane coatings. Coating with a thickness of 16 µm increased the E corr from − 481 mV (for bare steel) to + 187 mV and reduced both I corr and corrosion rate more than 6700 times. As an added benefit, after creating artificial cracks on the surface of the coating, the release of corrosion inhibitors gradually increased the impedance value, indicating a thin barrier layer has formed within the cracks.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2022
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IF 8.025
Lan Chen,Zhanming Liang,Xiaoxuan Zhang,Liming Zhang,Shuangfei Wang,Changzhou Chen,Ling Zeng,Douyong Min
Lignin is the most naturally abundant source of aromatics for phenolic chemicals, bioenergy sources, and functional materials. Recent works are devoted to the acid-catalyzed organosolv extraction for improving the lignin valorization. However, β –aryl ethers are mostly cleaved to form carbon–carbon bonds under the acidic condition. In this work, lignin isolated with methanolic hydrochloric acid (MHL) was compared with conventional milled wood lignin (MWL). The methanol incorporated into lignin as α –OCH 3 to prevent the cleavage of β –aryl ethers. As a result, the yield of MHL was over 12 times that of MWL. The MHL appeared a regular granular structure with an average diameter of 100 nm. Analysis of 13 C– 1 H HSQC NMR spectra showed that MHL contained 42.6 % β –O–4 linkages whereas 35.9 % for the MWL, as well as 6.5 % β –5 and 3.2 % β – β , which was less than MWL. Moreover, 13 C NMR spectroscopy confirmed that MHL was mainly isolated by the cleavage of the associated carbohydrates rather than the degradation of β –aryl ether bonds. Therefore, MHL can be utilized more as a native lignin representative than MWL for studying the physicochemical properties and the interior structures of the protolignin.
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高影响因子
ChemistrySelect
·
2022
·Vol. 7
·期 31
·e202200638
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IF 2.307
Cheng Tang,Tao Hu,Yanglei Li,Xiaoli Hu,Kunpeng Song
Graphical We report a weaving strategy to adjust the backbone structure of alkaline lignin, by which porous materials with large specific surface area and uniform pore size distribution can be obtained, exhibiting good adsorption capacity for RhB. Lignin is widely found in nature and attracts increasing concern as the renewable carbon material. In this work, hyper-crosslinked lignin was successfully prepared and applied for adsorbing dyes such as rhodamine B (RhB), methylene blue (MB) and Congo Red (CR) in wastewater. The characteristics of the alkaline lignin and hyper-crosslinked lignin were identified by Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and N 2 adsorption and desorption measurements. The results show that the hyper-crosslinked lignin is composed of uniform and porous nanoparticles with smaller size as compared to the sheet and- block structure of alkaline lignin. The specific surface area and pore structure of the hyper-crosslinked lignin have been greatly optimized, while retaining the functional groups on the surface of the alkali lignin. The Brunner-Emmet-Teller (BET) surface area of the hyper-crosslinked lignin reaches up to 402.8 m 2 ⋅ g −1 , and the adsorption capacity of RhB is up to 1332 mg ⋅ g −1 . The isotherm model and thermodynamic results indicate that the adsorption process conforms to the Langmuir model, mainly showing a single-layer spontaneous chemical endothermic process. In addition, HCP−L showed good selective adsorption performance for cationic dyes with the adsorption amounts of 228 mg ⋅ g −1 for MB, while that of the anionic dye CR (89 mg ⋅ g −1 ) was comparatively low. The adsorption mechanism was hydrogen bonding and π-π stacking in addition to the electrostatic effect caused by the negative charge on the surface of HCP−L.
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INDUSTRIAL CROPS AND PRODUCTS
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2022
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IF 6.449
Liang Jiao,Mengya Sun,Jie Yang,Weisheng Yang,Hongqi Dai
Under the guidance of emission peak and carbon neutrality, flow battery has application prospects as a large-scale energy storage technology. As the most abundant aromatic compound in nature, lignin is rich in quinone groups and is a potential organic flow battery electrolyte material. In this work, density functional theory (DFT) is used to calculate the redox potential of lignin monomers (coniferaldehyde and sinapaldehyde), and the rationality of the simulation results are verified via cyclic voltammetry (CV). The results show that the lignin monomers realize energy storage through the structural transformation between hydroquinone (QH 2 ) and quinone (Q) in the redox process. At a current density of 40 mAcm −2 , the open circuit voltage of 0.01 mol/L coniferous aldehyde can reach 1.0 V, and the volumetric capacitance can reach 145 mAh·L −1 . After 200 cycles of charging and discharging, the capacitance still retains 87.4%, and the coulombic efficiency remains at 99.0%. The open circuit voltage can reach 1.5 V, at a current density of 10 mA·cm −2 of 0.01 mol/L. The volumetric capacity reaches 105mAh·L −1 and remains 75.0% after 200 cycles of cycling. DFT can predict the oxidation-reduction potential of lignin electrolyte and provide theoretical guidance for the application of lignin in the field of flow battery energy storage.
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高影响因子
Materials Today Chemistry
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2021
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IF 8.301
X. Lu,M. Yu,D. Wang,P. Xiu,C. Xu,A.F. Lee,X. Gu
A simple and environmentally benign synthetic route to lignin-based epoxy resins is highly desirable. Alkali lignin and glyoxal are promising renewable and sustainable alternatives to phenol and formaldehyde, respectively. Their use is demonstrated to produce lignin-phenol-glyoxal novolac epoxy resins (LPG-NERs) through a simple one-pot synthesis. Flame retardancy of LPG-NERs was improved by functionalization with a N, S modified 9, 10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO) material (termed DBS) obtained via nucleophilic reaction between DOPO and a N, S containing intermediate. FTIR and 1 H NMR analyses confirmed the successful fabrication of LPG-NERs and SBD. The introduction of lignin and SBD reduced crosslinking of the epoxy network, weakening mechanical properties , but conferred excellent flame retardancy (including vapor and condensed phases) as determined by LOI (34.5%), UL-94 (V-0 rating), and cone calorimetry tests (lower heat release and smoke production, and higher char formation). The SBD structure imparted a desirable vapor mechanism (blowing out phenomenon caused by the fire quenching effect of PO•/PO 2 • radicals and dilution effect from non-condensable gases such as NH 3 , N 2 , SO 2 ), while lignin (a natural biochar precursor) in synergy with SBD imparted superior charring performance.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2021
·
IF 5.645
Xiaotong Fu,Hairui Ji,Xiaohui Liu,Wenyuan Zhu
Herein, a physicochemical pretreatment method, namely, a combination of recyclable acid hydrotrope ( p -toluenesulfonic acid, p -TsOH) treatment and ultrasonic treatment (10 s), was employed to extract lignin-containing fibers (LFs) from wood material ( poplar ). The LFs were used to produce reinforced polyvinyl alcohol (PVA) hydrogels via a dissolution-regeneration process in LiBr⋅3H 2 O solution. After coating the produced hydrogel on the end face of a single-mode fiber (SMF), a fiber-optic relative humidity sensor (FORHS) was fabricated to monitor environmental humidity. A high sensitivity (4.7 dB) and good repeatability ( R 2 = 0.98, the confidence factor) were found within a humidity range from 45 % to 80 %. Therefore, this study provides a sustainable approach for valorization of lignocellulosic biomass.
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Xiangchen Kong,Chao Liu,Baolong Wang,Weicong Xu,Yuyang Fan,Ming Li,Rui Xiao
A complex copper acid catalyst (SA-Cu/CuMgAlOx) was developed with boosted catalytic activity for the hydrodeoxygenation (HDO) of lignin-derived phenolics. Remarkably, the yields of total monomers and cyclohexanes from the HDO of lignin pyrolysis bio-oil were significantly improved after the catalyst modification with salicylic acid, which increased by 17 and 40%, respectively, at 300 °C for 8 h. The catalyst characterizations revealed that acidic oxygen-containing functional groups (−OH and −COOH) were introduced onto the catalyst surface without corrosion to the metallic framework. The acidic groups contributed to the formation of surface Brønsted acid sites, which participated in the hydrogenolysis and dehydroxylation reactions of the phenolics in bio-oil. The catalyst was deactivated after four cycles of bio-oil HDO and could be recovered after the removal of carbon deposits and the reactivation of Cu species. The results offered appealing opportunities for tailoring more efficient copper-containing catalysts for the HDO of lignin-based phenolics.
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高影响因子
FUEL
·
2021
·
IF 6.609
Bo Chen,Ruiheng Rao,Meifang Cao,Chengzhi He,Yong Qian,Xueqing Qiu,Xinping Ouyang
An imperative current challenge for the production of renewable fuels is the development of efficient catalytic hydrodeoxygenation (HDO) of phenolic-rich bio-oils into hydrocarbons. In this work, a series of bifunctional ZrP 2 O 7(x) -Ni 12 P 5 (where × represents the molar ratio of Zr/Ni in the catalysts) catalysts were prepared for HDO of lignin-derived bio-oils (LBO). The characterization results show that among these bimetallic catalysts, ZrP 2 O 7(0.4) -Ni 12 P 5 possesses the largest specific surface area, pore volume and the highest amount of acid sites (Lewis and Brønsted) due to the introduction of appropriate amount of Zr species. Meanwhile, the interaction between Ni δ+ and Zr species on its surface creates new active sites for the promotion on the hydrogen adsorption and activation, thus endowing the most excellent catalytic performance. Using the optimized catalyst of ZrP 2 O 7(0.4) -Ni 12 P 5 , 95.8% cyclohexane yield could be obtained from the HDO of guaiacol as a model compound from bio-oil under mild condition (3 MPa H 2 and 250 ℃). Moreover, 36.1% hydrocarbon yield is achieved from HDO of lignin-derived bio-oils (LBO) under the same hydrogen pressure and temperature. These findings not only open a novel avenue for designing a cost-effective metal–acid bifunctional catalyst, but also provide a viable approach for converting lignocellulosic biomass feedstocks into valuable hydrocarbons.
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高影响因子
BIOMASS & BIOENERGY
·
2022
·
IF 5.774
Guojun Hao,Hongying Liu,Zhibing Chang,Kechen Song,Xin Yang,Han Ma,Wenjing Wang
In this work, lignin depolymerization was examined over CoMo sulfide catalysts supported on different carriers in supercritical ethanol system. The temperature, time, MoS 2 and carrier effects on the lignin depolymerization were investigated. 95.76% liquefaction yield with negligible char was achieved over Co–Mo–S/ZrO 2 at 340 °C for 150 min. The liquid product was mainly composed of C 4 –C 8 alcohols, C 4 –C 10 esters and C 7 –C 10 aromatic compounds . The synergistic effect of active sites and acid-base sites on support played an important role in lignin depolymerization. Furthermore, the Co–Mo–S/ZrO 2 catalyst is reusable with 8% loss in liquefaction yield after 5 cyclic runs. We believe that acid/base carriers or additives that can promote the medium to generate abundant free radicals or ions to replace external hydrogen pressure are one of the prospects for the design of depolymerization lignin catalysts.
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