JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2023
·
IF 6.1
Dingkai Wang,Mingyu Cui,Wei Zhao,Yanjun Li,Shangshang Ma,Zhijie Jiang,Xutang Liu,Chong Liang,Rujuan Li,Long Ma,Yanmin Song,Xian-Yong Wei
Lignin, the second largest component of biomass, is considered as an important alternative source of fossil reserves for the production of fuels and chemicals. Here, we developed a novel method to oxidatively degrade organosolv lignin into value-added four-carbon esters, particularly diethyl maleate (DEM), with the cooperative catalyst consisting of 1-(3-sulfobutyl) triethylammonium hydrogen sulfate ([BSTEA]HSO4) and 1-butyl-3-methylimidazolium ferric chloride ([BMIM]Fe2Cl7). Under optimized conditions (1.00 MPa initial O2 pressure, 160 °C, 5 h), the lignin aromatic ring was effectively cleaved by oxidation to form DEM with a yield of 15.85% and a selectivity of 44.25% in the presence of the synergistic catalyst of [BMIM]Fe2Cl7-[BSMIM]HSO4 (1/3, mol/mol). The structure and composition analysis of lignin residues and liquid products confirmed that the aromatic units in lignin were effectively and selectively oxidized. Furthermore, the catalytic oxidation of lignin model compounds was explored for obtaining a possible reaction pathway of oxidative cleavage of lignin aromatic units to DEM. This study provides a promising alternative method for the production of traditional petroleum-based chemicals.
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MOLECULES
·
2023
·Vol. 28
·期 7
·2923
·
IF 4.6
Enmin Zong,Xuanren Wang,Lirong Zhang,Jiayao Yang,Xiaohuan Liu
The application of lignin-based adsorbents in the efficient removal of phosphate from wastewater has attracted much attention and been intensively studied in recent years. However, most currently reported lignin-based adsorbents are difficult to recover and recycle. Herein, we have developed a recyclable, nanostructured bio-adsorbent, poly(ethyleneimine) (PEI)-modified lignin (LG) integrated with Fe3O4and Zr-La dual-metal hydroxide (LG-NH2@Fe3O4@Zr-La), by the Mannich reaction followed by the chemical coprecipitation method. Multilayer adsorption existed on the surface of LG-NH2@Fe3O4@Zr-La based on the isotherm fitting curve, and its adsorption capacity reached 57.8 mg P g−1, exhibiting a higher phosphate uptake than most reported metallic oxide-based composites. The adsorption process was dominated by inner-sphere complexation of ligand-exchange and electrostatic interactions. Moreover, LG-NH2@Fe3O4@Zr-La exhibited excellent selectivity against coexisting anions, and the adsorption was more efficient under acidic conditions. When the phosphate concentration was 2.0 mg P L−1, the removal efficiency of phosphate reached 99.5% and the residual concentration was only 10 μg P L−1, which meets the United States Environmental Protection Agency (USEPA) standard for eutrophication prevention. In addition, the LG-NH2@Fe3O4@Zr-La displayed excellent reusability, maintaining 91.8% of removal efficiency after five cycles. Importantly, owing to the magnetic properties of the loaded Fe3O4, the resulting composite could be separated within 30 s under an external magnetic field. Thus, the separable and recyclable biobased magnetic adsorbent developed in this work exhibited promising application in phosphate capture from real sewage. This research study provides a new perspective for lignin valorization in lignocellulose biorefineries and establishes an approach for developing an economical and efficient bio-adsorbent for phosphate removal from wastewater.Keywords:lignin;magnetic adsorbent;Zr hydroxides;La hydroxides;phosphate;recycle
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jun Deng,Chi Zhou,Yue Yang,Bing Nan,Lin Dong,Lingchao Cai,Lina Li,Zhu-Jun Wang,Xiaofei Yang,Zupeng Chen
The selective cleavage of the C C bonds in lignin is highly pursued to obtain aromatic monomers from renewable resources but remains challenging due to their high dissociation energies and steric hindrance between bulky aromatic groups. Herein, a mesoporous carbon nitride-supported ruthenium single-atom photocatalyst (Ru 1 /MCN) is reported for efficient oxidative C α -C β bonds scissoring towards lignin β -O-4 model compounds with high activity and selectivity under visible–light irradiation and room temperature. With this strategy, a nearly total conversion of > 99% and > 98% selectivity of C C bond cleavage can be achieved upon 2–phenoxy–1–phenylethanol. In-depth investigations verify that the C β -H extraction by photogenerated holes is the critical step of the transformation, which directly generates the C β radical intermediates and thus promotes the selective C α -C β bonds breaking by coupling with superoxide radicals induced by photogenerated electrons. This work explores the potential of single-atom catalysts for photocatalytic production of aromatics from renewable biomass feedstocks.
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APPLIED CATALYSIS A-GENERAL
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2023
·
IF 5.5
Wenqi Zou,Heyu Li,Minghua Liu,Yuancai Lv
In this study, Cu was loaded on the surface of Ni-MOF by impregnation, and significantly improved the catalytic activity on lignin and its derivatives. The characterization showed that the non-noble bimetallic catalyst owned good dispersion, rich acid sites and stable structure was successfully synthesized. The introduced Cu reduced the reduction temperature of Ni, increased the acidity of the catalyst, and thus improved the catalytic performance and product selectivity of the catalyst. Under the mild conditions (120 °C), the conversion percentage of BPE was as high as 89.6 % using isopropyl alcohol as the hydrogen source. When the reaction temperature was 260 °C, the depolymerization percentage of corn cob lignin was 81.12 %, and the yield of phenol monomer could reach 11.46 wt. %. This work may provide an effective strategy for the preparation of efficient bimetallic catalysts for lignin hydrogenolysis .
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INDUSTRIAL CROPS AND PRODUCTS
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2023
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IF 5.9
Qianqian Tang,Hao Wu,Mingsong Zhou,Dongjie Yang
To remove Cr(VI) in water, a novel lignin-based anionic adsorption resin epichlorohydrin cross-linking lignin grafted by diethylenetriamine (E-DAL) was prepared by the direct cross-linking and curing of alkali lignin grafted by diethylenetriamine in aqueous solutions. Under the determined optimum synthesis conditions, E-DAL with higher nitrogen (7.46%) and lignin (32.78%) contents was obtained. Structural and physicochemical measurement results showed E-DAL was a macroporous resin, having a regular connected pore structure with porosity of 67.48% and pore size of 615.6 nm, also strong hydrophilicity, excellent acid-alkaline resistance and thermal stability. Adsorption experiment results indicated the adsorption isotherm of E-DAL to Cr(VI) was well-described by Langmuir model. E-DAL showed a higher adsorption capacity to Cr(VI), and the fitted maximum adsorption capacity reached up to 775.2 mg/g. Pseudo-second-order model could fit this adsorption process well, suggesting its chemisorption characteristics. The calculated thermodynamic parameters indicated a spontaneous and endothermic adsorption of E-DAL to Cr(VI). Dynamic column adsorption results showed E-DAL could completely remove Cr(VI) in wastewater. This whole preparation process only used a very small amount of cheaper amination agent and was relatively low-cost. This work provided efficient technical supports for the structural design of high-performance lignin-based anionic adsorption materials in water treatment field.
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COMPOSITES PART B-ENGINEERING
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2023
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IF 13.1
Bixia Zheng,Tao Liu,Jing Liu,Yilong Cui,Rongxian Ou,Chuigen Guo,Zhenzhen Liu,Qingwen Wang
Introducing microphase separation and dynamic bonds into the polymeric materials is an effective strategy to enhance the performance of polyurethane . Herein, a modified lignin-based polyol (MLOH) was developed via a facile one-step approach which greatly improved its reactivity and dispersibility compared to that of virgin lignin. Subsequently, inspired by the biphasic structure of natural spider silk , a high-performance modified lignin-based dynamic covalent polyurethane (MLPU) with lignin enhanced microphase separation was fabricated, exploiting the synthetic MLOH as the crosslinker and the dynamic oxime-carbamate bonds as the linkage. Besides possessing high repairing efficiency (3 min for 100%, 80 °C without pressure), and outstanding shape-memory capability, the optimized MLPU-2 demonstrated robust adhesive performance when applied as a polyurethane hot-melt adhesive, including a fast curing rate and high adhesive strength (10.50 MPa). Meanwhile, it also manifested remarkable solvent resistance , temperature tolerance from −30 °C to 60 °C, long-term durability for at least 3 months, on-demand debonding ability, and excellent reusability . The synergistic effect of lignin enhanced microphase separation and adjustable dynamic crosslinked structure endows the remarkable performance of this resultant dynamic covalent MLPU, which provides another way to develop green, sustainable polyurethane simultaneously with highly comprehensive performances for the potential practical application.
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Surfaces and Interfaces
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2022
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IF 6.137
Jin-Yu Wang,Zhong-Zhu Hu,Xin-Ting Sun,Ya-Qin Gao,Jun-Lin Wang,Jie Xu,Gan Jin
Photocatalytic cleavage of lignin C β -O-4 bonds is a very effective method to promote the high-value utilization of lignin because lignin can provide a large number of aromatics. However, the higher carrier recombination rate severely inhibits the efficiency of photocatalytic cleavage of C β -O-4 bonds in lignin model compound. Here, heterojunction photocatalysts CdS-C 3 N 4 were successfully synthesized through the photodeposition of different masses of CdS on the surface of C 3 N 4 . The obtained photocatalyst CdS-C 3 N 4 can effectively break the lignin C β -O-4 bonds in 2-Phenoxy-1-phenylethanol (lignin model compound) and the products formed are mainly phenol (Phol) and acetophenone (Ap). More importantly, the yields of Phol and Ap were up to 86.5% and 74.3%, after only irradiation for 1.5 h, respectively, under optimum conditions. A mechanistic study showed that photocatalytic reaction follows a photogenerated electron-hole coupled mechanism. The high photocatalytic performance of CdS-C 3 N 4 is mainly ascribed to the fast photogenerated electron-hole separation capability and good dispersion of CdS on C 3 N 4 . This work offers an idea for selective cleavage of lignin C β -O-4 bonds by constructing a heterojunction photocatalyst.
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Journal of Energy Chemistry
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2023
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IF 13.1
Baoyu Wang,Peng Zhou,Ximing Yan,Hu Li,Hongguo Wu,Zehui Zhang
In this work, a dual-size MOF-derived Co catalyst (0.2Co 1-NPs @NC) composed of single atoms (Co 1 ) and highly dispersed nanoparticles (Co NPs) was prepared by in-situ Zn evaporation for the high-performance conversion of lignin-derived o- methoxyphenols (lignin oil) to cyclohexanols (up to 97% yield) via cascade demethoxylation and dearomatization. Theoretical calculations elaborated that the dual-size Co catalyst exhibited a cooperative effect in the selective demethoxylation process, in which the Co NPs could initially dissociate hydrogen at lower energies while Co 1 remarkably facilitated the cleavage of the C Ar − OCH 3 bond. Moreover, the intramolecular hydrogen bonds formed in the o -methoxy-containing phenols were found to result in a decrease in the bond energy of the C Ar − OCH 3 bond, which was more prone to be activated by the dual-size Co sites. Notably, the pre-hydrogenated intermediate (e.g., 2-methoxycyclohexanol from guaiacol) is difficult to undergo demethoxylation, indicating that the selective C Ar − OCH 3 bond cleavage is a prerequisite for the synthesis of cyclohexanols. The 0.2Co 1-NPs @NC catalyst was highly recyclable with a neglect decline in activity during five consecutive cycles. This cooperative catalytic strategy based on the metal size effect opens new avenues for biomass upgrading via enhanced C O bond cleavage of high selectivity.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
·
IF 6
Qingqin Sun,Xu Fu,Peiru Wang,Kunlan Li,Ligang Wei,Shangru Zhai,Qingda An
The oxidative depolymerization of alkali lignin (AL) catalyzed by copper-containing imidazolium-based ionic liquids ([C 4 C 1 im]CuCl 3 ) was investigated with CH 3 OH-H 2 O (9/1, v/v) as solvent under an initial oxygen pressure of 1.5 MPa at 150 °C for 3 h. Compared with other transition-metal chlorides and metal-containing ionic liquids (ILs), [C 4 C 1 im]CuCl 3 presented a relatively remarkable catalytic capacity for AL oxidative depolymerization due to the cooperative effects of [C 4 C 1 im] + and CuCl 3 − . [C 4 C 1 im]CuCl 3 molar concentration ( x McIL ) greatly influenced AL conversion and product selectivity. The highest AL conversion of 70.4% was achieved at x McIL = 0.18 mol.%. For the obtained small-molecule products, the highest selectivity of p -hydroxybenzaldehyde reached 51.3% at x McIL = 0.72mol.% (corresponding yield of 103.6 mg·g −1 ). The inter-unit linkages of lignin were effectively cleaved in the oxidative depolymerization catalyzed by [C 4 C 1 im]CuCl 3 , and the H unit in lignin was preferentially destroyed. The molecular interactions and microenvironment of [C 4 C 1 im]CuCl 3 –solvent (CH 3 OH-H 2 O) system were investigated with x McIL varied from 0.05 mol.% to 5.12 mol.% by using attenuated total reflectance-infrared spectroscopy and molecular-dynamics method, respectively. The catalytic properties of [C 4 C 1 im]CuCl 3 strongly depended on the interactions of [C 4 C 1 im]CuCl 3 and solvent molecules with changes in microstructure organization. The optimum catalytic capacity of [C 4 C 1 im]CuCl 3 was obtained when the ion pair formed through hydrogen bonding at x McIL = 0.18–0.36 mol.%. The solvation of solvent molecules on CuCl 3 − and the formation of ionic cluster with the hydrogen-bonding self-association of [C 4 C 1 im]CuCl 3 were unfavorable for the oxidative depolymerization of lignin.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
·
IF 8.2
Ying Chen,Xiaowei Lv,Yushu Wang,Jingyi Shi,Sihan Luo,Junjiang Fan,Bo Sun,Yupeng Liu,Quli Fan
Developing a straightforward method to produce conductive hydrogels with excellent mechanical properties, self-adhesion, and biocompatibility remains a significant challenge. While current approaches aim to enhance mechanical performance, they often require additional steps or external forces for fixation, leading to increased production time and limited practicality. A novel lignin-grafted polyacrylamide/hydroxypropyl cellulose hydrogel (L-g-PAM/HPC hydrogel) with a semi-interpenetrating polymer network structure had been developed in this research that boasted exceptional adhesion to the skin (∼68 kPa) and stretchability properties (∼1637 %) compared to PAM-based hydrogels. By incorporating conductive additives such as silver nanowires and carbon nanocages to construct a bridge-like structure within the hydrogel matrix, the resulting AgC@L-g-PAM/HPC hydrogel exhibited impressive electrical conductivity , surpassing that of other PAM-based hydrogels relying on MXene, with a maximum value of 0.76 S/m. Furthermore, the AgC@L-g-PAM/HPC hydrogel retained its efficient electrical signal transmission capability even under mechanical stress. These make it an ideal flexible strain sensor capable of detecting various human motions. In this study, a smart real-time monitoring system was successfully developed for tracking cervical spine bending, serving as an extension for monitoring human activities.
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RSC Advances
·
2023
·Vol. 13
·期 30
·21063-21070
·
IF 3.9
Yudan Zhong,Yulong Ma,Yonggang Sun,Liqiong Wang,Yuanyuan Li,Feng Lin,Yingbo Zhu
The lignin oil produced by rapid pyrolysis of lignin is considered a promising liquid fuel source. Hydrodeoxygenation (HDO) is a kind of efficient method to upgrade the lignin oil, and a high-performance catalyst is key to the hydrodeoxygenation of lignin oil. In this study, a high dispersion and small size Ru nanoparticle loaded N-doped carbon catalyst was derived by the direct pyrolysis of a mixture of ruthenium trichloride and melamine, and it could efficiently convert lignin oil. The lignin oil was completely transformed at 240 °C and 1 MPa H2, and 36.58% cyclohexane was obtained. The formation, surface area, and nitrogen species of the catalyst could be controlled by changing the precursor of the nitrogen-doped carbon support. The percentage of pyridine nitrogen possessed with melamine as a nitrogen–carbon precursor (31.35%) was much higher than that with urea (16.47%) and dicyandiamide (8.20%) as nitrogen–carbon precursors. The presence of pyridine nitrogen could not only serve as the coordination site for even dispersity and stability of Ru nanoparticles but also regulated the electron density of Ru nanoparticles (NPs) and increased the active site Ru0 through electron transfer.
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Foods
·
2023
·Vol. 12
·期 14
·2794
·
IF 5.2
Shushan Gao,Chonghao Zhu,Liangfei Ma,Chenghai Liu,Hongqiong Zhang,Shengming Zhang
To reduce the usage of petroleum-based plastic products, a lignin-based film material named aminated lignin/Fe(III)/PVA was developed. The mixture of 8 g lignin, 12 mL diethylenetriamine, 200 mL NaOH solution (0.4 mol·L−1), and 8 mL formaldehyde was heated at 85 °C for 4 h; after the aminated lignin was impregnated in the Fe(NO3)3solution, a mixture of 3 g aminated lignin/Fe(III), 7 g PVA, and 200 mL NaOH solution (pH 8) was heated at 85 °C for 60 min; after 2 mL of glycerin was added, the mixture was spread on a glass plate to obtain the aminated lignin/Fe(III)/PVA film. This film demonstrated hydrophobicity, an UV-blocking function, and a good slow-release performance. Due to the formation of hydrogen bonds between the hydroxyl groups of lignin and PVA, the tensile strength, the elongation at break, and the fracture resistance of the film were 9.1%, 107.8%, and 21.9% higher than that of pure PVA film, respectively. The iron content of aminated lignin/Fe(III)/PVA was 1.06 wt%, which mainly existed in a trivalent form. The aminated lignin/Fe(III)/PVA film has the potential to be used as a food packaging material with anti-ultraviolet light function and can also be developed as other packaging materials, such as seedling bowls, pots for transplanting, and coating films during transport.Keywords:lignin;polyvinyl alcohol;Fe(III);packaging material;slow-release function
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