AICHE JOURNAL
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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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高影响因子
DIAMOND AND RELATED MATERIALS
·
2022
·
IF 3.806
Bujun Huang,Juncheng Jiang
New energy utilization devices have attracted great research interest as a sustainable route for clean energy production. However, the disadvantage of this process is the need to use high-cost precious metal catalysts. Hereby, N-doped carbon nanosheets (LNZ@GC) was prepared by ball milling-carbonization two step strategy using alkali lignin as carbon source and the gas-phase exfoliation with NH 4 Cl and ZnCl 2 as pore-forming agents. We investigative the properties of LNZ@GC series and find that LNZ@GC exhibit the most excellent ORR performances with a half-wave potential up to 0.851 V, outstanding stability and methanol tolerance, which are all superior commercial Pt/C. Furthermore, the rechargeable zinc-air battery assembled by LNZ-800@GC shows excellent performance with a high power density of 841.8 Wh kg −1 , a large specific capacity of 750.3 mA h g −1 . This work not only provides a general strategy for the preparation of porous N-doped catalysts, but also provides technical support for the design and development of inexpensive catalysts using lignin as a carbon source.
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 23
·12679-12691
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IF 14.511
Feiyan Shi,Shuai Zhao,Junyu Yang,Yao Tong,Jiajun Li,Shangru Zhai,Xinyu Zhao,Shenghan Wu,Hongsheng Li,Qingda An,Kai Wang
Transition-metal tungstates (MWO4), which are high-performance electrode materials for supercapacitor use thanks to their intrinsically outstanding electrochemical properties, have recently emerged and drawn great attention. Herein, we synthesized materials consisting of bimetallic Ni4−xCoxWO4 (x = 0.5, 1, 1.5, 2) nanoparticles supported on enzymatic-hydrolysis-lignin-derived three-dimensional hierarchical porous carbon (Ni4−xCoxWO4/HPC) and explored their usage as positive electrode materials for use in asymmetric supercapacitors. The Co/Ni ratio has a significant impact on the specific capacitance of the Ni4−xCoxWO4/HPC electrode, and the Ni3Co1WO4/HPC electrode, which is the best performer among Ni4−xCoxWO4/HPC electrodes to the best of our knowledge, exhibits an optimal specific capacitance of 1084 F g−1 (364.5 C g−1) at a current density of 0.5 A g−1 in 6 M KOH electrolyte solution. This is attributed to the distinctive nanostructure and strong synergistic effects between nickel and cobalt ions. Our density functional theory (DFT) calculations demonstrate that the significant capacitance enhancement seen for Ni4−xCoxWO4/HPC is associated with enhanced conductivity. An assembled asymmetric supercapacitor based on Ni3Co1WO4/HPC can provide a high voltage of 1.6 V and deliver an excellent energy density of 105.6 W h kg−1 at a power density of 400.5 W kg−1, and it has excellent stability, showing 80.74% capacitance retention after 10 000 cycles; this compares favorably with analogous supercapacitors. It is anticipated that the rational design of Ni3Co1WO4/HPC will provide new paths for the synthesis of high-performance bimetallic oxide materials for application in energy-related fields.
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高影响因子
Journal of Cleaner Production
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2022
·
IF 11.072
Bianyang He,Yao Xiao,Yanfang Li,Mingjie Fu,Jianying Yu,Lei Zhu
Bitumen could emerge the degradation of performance under ultraviolet (UV) light easily, then the bituminous pavement would have to be repaired and even reconstructed for safety, causing environmental pollution and energy consumption. Therefore, it is crucial to raise bituminous anti-UV aging property so that the service life of bitumen could be increased memorably, which is beneficial to environmental protection and sustainable development. Lignin grafted layered double hydroxides (LG-g-LDHs) were prepared successfully through covalent bonding with diphenyl-methane-diisocyanate (MDI), and were characterized by Fourier transform infrared (FTIR) spectrometer, scanning electron microscopy (SEM) contact angle tester and ultraviolet and visible (UV–vis) spectroscopy. Then LG-g-LDHs were used for modifying bitumen, the effects on anti-UV aging properties were researched by physical properties, four components analysis, FTIR and dynamic shear rheometer (DSR) test. The results showed that LG-g-LDHs were prepared and represented a stable cross-linked structure, then they had a combined effect of chemically absorbing and physically reflecting UV light owing to the multi-layered and benzene ring structure. Due to the introduction of lignin, the compatibility between LDHs and bitumen could be improved. After aging, the properties including physical properties and rheological behaviors of bitumen decreased and colloidal stability declined. Compared with LDH, LG-g-LDHs represented better inhibitory action in performance deterioration and colloidal stability of bitumen, which indicated that LG-g-LDHs could strengthen bituminous anti-UV aging properties for sustainable service of bitumen.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Weijun Yang,Yanlin Zhu,Yongbin He,Liqiang Xiao,Pengwu Xu,Debora Puglia,Piming Ma
Poly(lactic acid) (PLA) is an ideal biodegradable polymer material, widely applied in some disposable areas, such as packaging, biomedical and health care. However, its inherent brittleness, poor heat resistance and mono-functionality limit its application to a certain extent. In this study, PLLA-PCL-lignin nanocomposites (lignin nanoparticles (LNP) grafted with PLLA and poly(ε-caprolactone) (PCL) copolymer) produced by melt processing, were used as an interfacial compatibilizer. Meanwhile, partial replacement of PLLA by PDLA, in combination with an annealing treatment, were considered to enhance mechanical and heat-resistance of neat matrix. Mechanical thermal,optical properties, and heat resistance of the nanocomposites were comprehensively investigated. Interestingly, the notched impact strength was significantly increased from 2.3 (neat PLLA) to 15.3 and 12.1 kJ/m 2 for L8-C2 and LD8-C2 samples (PLLA, PDLA and PCL shorted as L, D and C, respectively), respectively. The lignin containing nanocomposite films also showed excellent UV-B resistance, due to the presence of LNP. Furthermore, a remarkable improvement of storage modulus up to 355 and 221 MPa at 90 °C was obtained for h-LD9-C1 and h-LD8-C2 (heat treatment shortened as h) via annealing treatment, enhancement ascribed to the transformation from homocrystallites to stereocomplex crystallites . As a consequence, a toughened PLA-PCL-lignin nanocomposite with good heat- and UV-resistance was successfully prepared, enlarging its possible use as multi-functional PLA based engineering plastic.
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CATALYSIS TODAY
·
2022
·
IF 6.562
Jinshu Huang,Yumei Jian,Hu Li,Zhen Fang
Biochar materials have wide applications in soil improvement/remediation, water pollution control, gas storage, and heterogeneous catalysis, while usually suffering from low surface areas and harsh preparation conditions. In this study, a green, environmentally friendly, and low-cost biochar catalyst (PAP-MEPP-C) was prepared by thermochemical treatment of lignin-derived monomers at a low temperature (80 °C), and further developed for high-efficiency production of biodiesel from non-edible Jatropha oil ( J O). The characterization results showed that the structure of the PAP-MEPP-C biochar catalyst was layered and 3D structure, and its acidity could be controlled by changing the monomeric composition. The reaction conditions of preparing biodiesel catalyzed by PAP-MEPP-C were optimized by the response surface method, and the obtained maximum biodiesel yield was 97.2%. The kinetics of the (trans)esterification reaction over the developed biochar catalyst PAP-MEPP-C was studied, and its superior catalytic performance to other tested acid catalysts could be supported by a relatively lower activation energy (36 kJ mol −1 ). In addition, the biochar catalyst was highly stable and could be recycled four times with more than 90% biodiesel yield.
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高影响因子
APPLIED ENERGY
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2022
·
IF 11.446
Xiangchen Kong,Chao Liu,Xing Wang,Yuyang Fan,Weicong Xu,Rui Xiao
Practical, economical, and high-selectivity methods of lignin bio-oil upgrading could greatly increase biorefinery productivity and profitability. Herein, we report the efficient production of oxygen-containing fuel via supercritical methanol hydrodeoxygenation (SCM-HDO) of lignin bio-oil with a well-defined Cu/CuZnAlO x catalyst. The fuel range cyclic alcohols were majorly produced from guaiacol and corncob lignin pyrolysis bio-oil with selectivity of 66.67 and 15.90% at 300 °C in 8 h, respectively, via Cu species induced hydrogenation of aromatics rings and inhibited over-deoxygenation of alcoholic hydroxyl groups. The catalyst activity decreased by 28% after five runs of bio-oil HDO due to the oxidation of Cu species and carbon deposit, where the oxidation of Cu species played the dominant role as the carbon deposit was restrained to as low as 3.64 wt% with the mild catalyst acidity. Meanwhile, the catalyst activity could be easily recovered through a calcination-reduction process to remove the carbon deposit and reactivate the Cu species. The results offered appealing opportunities for tailoring more efficient approaches for the upgrading of lignin bio-oil to alternative biofuels.
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CATALYSIS TODAY
·
2022
·
IF 6.562
Yiming Ma,Yushuai Sang,Kai Wu,Qingfeng Liu,Hong Chen,Yongdan Li
Low selectivity and complex product distribution are the main challenges for the utilization of lignin. Herein, the selective production of 2-(tert-butyl)-3-methylphenol (TBC), an antioxidant in the polymer industry, from depolymerization of enzymatic hydrolysis lignin (EHL) on a hydrothermally synthesized MoS 2 catalyst is studied. The total aromatic monomer yield is 124.1 mg/g EHL and the selectivity of TBC is up to 40.3 wt% in methanol at 280 °C under 2 MPa H 2 for 6 h. The FT-IR analysis of products reveals that MoS 2 has a high activity for demethylation, dehydroxylation and alkylation, and the dimer conversions reveal that C-O and C-C bonds in EHL are broken with MoS 2 . The guaiacol and its derivants are identified as the intermediate for formation of TBC in EHL depolymerization according to the effect of time on product distribution and monomer conversion.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qingqi Zheng,Dequan Zhang,Peng Fu,Aixia Wang,Yongmei Sun,Zhiyu Li,Qingwen Fan
Unraveling the role of volatile evolving and char structural evolution, as well as the pyrolysis reaction pathway, is crucial for lignin effective valorization by a pyrolysis-based biorefinery approach. The fast pyrolysis of lignin at 200–800 °C was conducted to explore volatile release characteristics and their link with char structure evolution. The release of simple substituted aryl compounds below 350 °C was aided by the cleavage of β-O-4 and α-O-4. The C-O, C–C, and carboxyl groups of the depolymerized free radical fragments were cleaved further, providing stable mono-phenol (350 °C → 500 °C). Secondary reactions and pyrolytic macromolecular compounds resulted in the synthesis of polycyclic aromatic hydrocarbons (>700 °C). A cubic polynomial was developed to correlate the aromaticity with the atom ratio of H/C. The ring condensation degree and H/C demonstrated an excellent positive linear correlation. Additionally, the aromatization started at 350 °C, and small aromatic rings were changed into more ordered rings (≥6 rings). The fused-ring structures of char had progressed in the following order: 1 × 2, 2 × 3, 4 × 4, and 4 × 5, corresponding to 350 °C, 500 °C, 600 °C, and 800 °C, respectively. High temperatures contributed to the formation of aromatic monomers. Lignin pyrolysis pathway was established based on the correlation between volatile release characteristics and char structural evolution.
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RENEWABLE ENERGY
·
2022
·
IF 8.634
Junxian Xie,Zheng Cheng,Shiyun Zhu,Jun Xu
In order to improve the pretreatment behavior of neutral deep eutectic solvent (DES), a novel method was proposed by using three types of Lewis base (sodium carbonate, sodium sulfite and sodium acetate as catalysts to pretreat corn straw at 120 °C for 3 h. As compared to DES, DES with Na 2 SO 3 , DES with NaAC and DES with Na 2 CO 3 , all can remove most of hemicellulose and lignin in pretreated corn straw. Meanwhile, the 94.5% of glucose yield was obtained treated by DES with Na 2 CO 3 and was approximately five-fold higher than that of the untreated substrate at an enzyme loading of 15 FPU/g material. The regenerated lignin displayed well-preserved structures, and possessed a high purity (more than 84%), narrow molecular weight distribution (PDI <2.4), excellent thermal stability. Overall, this work provided detailed analysis for efficient deconstruction of corn straw for future industrialized application.
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高影响因子
FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Zhongwei Wang,Xiangqian Chen,Xinlin Xie,Shuangxia Yang,Laizhi Sun,Tianjin Li,Lei Chen,Dongliang Hua
The utilization of lignin to produce high value-added chemicals remains a significant challenge, this study reports the synthesis of highly active nitrogen-doped carbon nanotubes to support nickel-based catalysts via a two-stage pyrolysis process using a mixture of melamine and nickel acetate. The catalyst morphology is controlled through the use of melamine, the doped pyridinic nitrogen serves as an anchoring site for Ni metal, facilitating the dispersion of Ni metal and the formed Ni-Nx bond enhanced the stability of the catalyst. Additionally, the electron transfer between Ni and N atoms promoting the activation of hydrogen on the metallic nickel surface, which together with the aforementioned factors, contributes to the cleavage of the C-O bond in lignin, with 23.1% monomer yield under mild conditions. The density functional theory (DFT) calculations reveal that doped nitrogen atoms can provide electrons to carbon atoms, resulting in an electron-rich state that facilitated the adsorption of hydrogen.
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ChemSusChem
·
2023
·Vol. 16
·期 17
·e202300357
·
IF 8.4
Yinan Tang,Lu Lu,Xiaoxian Zang,Buhuan Wang,Xiangrong Ye
Graphical Cellulose and lignin blend as carbonaceous precursor paves a feasible way to break through the restriction by intrinsic proportion of cellulose and lignin in natural biomass, allowing for tailoring and optimizing composition, structure and porosity of resultant activated carbon (AC) materials to promote power density, energy density and rate performance of supercapacitors. KOH-activated carbon materials prepared from biomass-derived carbon source, cellulose and lignin, were compared. Mixtures of different ratios of cellulose and lignin were used to partially mimic biomass as carbon source. This allows tailoring and optimizing of the KOH activated carbon materials by getting rid of the restriction of the intrinsic proportion of cellulose and lignin in specific biomass. The results indicate that cellulose use results in a more porous structure, whereas lignin use leads to more partially activated graphite structure. The activated carbon material (CL1) prepared from blend of cellulose with lignin in mass ratio of 1 : 1 exhibits a high specific surface area of 2000.39 m 2 g −1 , and in TEABF 4 /ACN (tetraethylammonium tetrafluoroborate dissolved in acetonitrile) electrolyte it showed a maximum specific capacitance of 136.10 F g −1 , a maximum energy density of 18.11 Wh kg −1 , and a capacitance retention of 85.04 % under current density as high as 15 A g −1 .
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PubMed
高影响因子
危险品化学品经营许可证（带存储）