Journal of Cleaner Production
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2025
·
IF 10
Hongguang Zhang,Zi Yu,Yongxin Liang,Tao Gan,Zuqiang Huang,Huayu Hu,Yanjuan Zhang
The utilization of organic molecules as in-situ hydrogen donors for producing γ-valerolactone (GVL) biofuel from biomass-derived levulinic acid (LA) represents one of the promising sustainable approaches. However, this process still faces challenges, including the difficult activation of the hydrogen source and the transport limitations of active hydrogen species. Herein, a Co-MnO/spontaneously polarized ceramic-carbon (Co-MnO/SPCE-C) composite catalyst, featuring a unique spontaneous polarization effect, was developed for catalytic transfer hydrogenation (CTH) of LA to GVL in the isopropanol/H 2 O (volume ratio = 1/19) cosolvent system. Co-MnO/SPCE-C contributed to an outstanding LA conversion of 99.9% and a favorable GVL yield of 93.5%, surpassing the performance achieved by comparative catalysts. Various characterization techniques demonstrate that SPCE with far-infrared emission and surface electric field increased the oxygen vacancies, thereby promoting hydrogen spillover and enhancing the properties of CoO x –MnO acidic sites. The 17 O NMR spectra reveal that SPCE activated water clusters by weakening the hydrogen bonding network. Moreover, D 2 O experiments show that SPCE facilitated the participation of water in the reaction. This work provides valuable insights into the development of an efficient strategy for producing GVL from LA. Before the catalyst can be considered for commercial applications, the focus in the future should be on a comprehensive computational analysis, long-term evaluation of catalyst stability, and additional industrial-scale testing.
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高影响因子
Journal of Materials Chemistry C
·
2021
·Vol. 9
·期 44
·15918-15926
·
IF 7.393
Zhigang Gao,Luyue Niu,Feifei Zhang,Sikai Wang,Jing Xiao,Jun Chen,Lian Zhang,Jing Ren,Katsuhisa Tanaka
Manipulating the plasmonic properties of metal nanocrystals (NCs) is key to many modern nanophotonic technologies. Here, the strategy of combining Ag+ ↔ Li+ ion exchange and controlled thermal crystallization is proposed as an effective means to prepare transparent nano-glass composites (nano-GCs) embedded with hybrid Ag–metal and γ-Ga2O3:Ni2+ NCs. Only by this method can a large amount of Ag–metal NCs (1.1 mol%) be implanted and well dispersed in the glass matrix without sacrificing their optical transmission properties. The broadband near-infrared (NIR) emission of Ni2+ is enhanced by 100% in the presence of Ag–metal NCs, which is otherwise impossible by raising the Ni2+ concentration due to the limited solubility and intrinsically weak absorption of Ni2+ in nano-GCs. The mechanisms responsible for the enhanced NIR emissions of Ni2+ are comprehensively discussed in the context of both experimental investigations and theoretical simulations. The present study not only provides a promising robust nano-GC-based gain medium for integrated optics but also offers some insights into the plasmonic metal-enhanced photoluminescence for enriched optical functions.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Ming-Jia Guo,Cheng-Cheng Xiang,Yi-Yang Hu,Li Deng,Si-Yu Pan,Chao Lv,Shou-Xiao Chen,Hao-Tian Deng,Cheng-Dong Sun,Jun-Tao Li,Yao Zhou,Shi-Gang Sun
Silicon (Si) is considered to be one of the most suitable anode materials for high energy density lithium-ion batteries due to its high theoretical specific capacity. However, the practical application of Si anode is limited by its huge volume change, leading to the rupture of electrode during cycling. In this study, a natural polymer of poly-glutamic acid ( γ -PGA) is derived from nattomycin gum and poly-acrylic acid (PAA) through thermal cross-linking method and served as a dual force cross-linked binder. The two polymers are firmly bonded by dehydration to form the cross-linked γ -PGA-PAA binder with stable ester bonds, which readily creates hydrogen bonding forces with the hydroxyl groups on Si surface. The γ -PGA-PAA exhibits robust mechanical properties to achieve excellent electrochemical performance of Si-based electrode. When the γ -PGA-PAA is used as binder of Si nanoparticle anodes, the capacity retention of Si/ γ -PGA-PAA electrode can reach 63.1% after 300 cycles at charge/discharge current density of 420 mA g −1 with a mass loading of about 0.7 mg cm −2 . As a comparison, the capacity retentions of the Si/PAA and Si/ γ -PGA electrodes are respectively 8.7 and 17.9% under the same conditions. At higher current density of 2940 mA g −1 , the capacity retention of Si/PAA electrode has dropped dramatically to 23.3%, and the Si/ γ -PGA-PAA electrode keeps still high-capacity retention of 72.5% after 400 cycles, while the Si/ γ -PGA electrode can only last 40 cycles. When the three binders are applied to SiO electrode with 1 mg cm −2 loading, the γ-PGA-PAA binder yields also the highest capacity retention of 87.3% after 100 cycles at 160 mA g −1 , while those corresponding to PAA and γ-PGA binders are 81.3% and 74.9%, respectively. XPS characterization results indicate that the γ -PGA-PAA binder has a strong adhesion to Si particles. This cross-linked binder network of γ -PGA-PAA effectively enhances the cycling performance and maintains the structural integrity of Si and SiO electrodes.
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高影响因子
CELLULOSE
·
2020
·Vol. 27
·期 7
·3581-3590
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IF 4.21
Yang Xue,Song Yanliang,Ma Sen,Zhang Xu,Tan Tianwei
A method for isolating components of lignocellulose in hybrid poplar by using an organic solvent (γ-valerolactone) in combination with a solid organic acid ( p -toluenesulfonic acid) is studied here. The combined hydrolysis factor (CHF) was used to measure the severity of the pretreatment conditions and to find the optimal reaction conditions (CHF = 54.99) by judging enzymatic saccharification and characterization of lignin residual. At this pretreatment strength, 91.67% hemicellulose and 86.14% lignin in lignocellulose were effectively removed, and the enzymatic hydrolysis of cellulose residue reached 84.84%. Hemicellulose was hydrolyzed to 4.39 g L −1 of xylose, and a portion was converted to 2.95 g L −1 of furfural and 3.59 g L −1 of acetic acid. The molecular weight, polydispersities and phenolic hydroxyl groups content of the isolated lignin were 1587 g mol −1 , 1.04 and 3.64 mmol g −1 respectively, which indicated that the lignin had the potential to be a phenolic resin material and wood polyurethane foam. In summary, this method effectively separated three components of lignocellulose and obtained high purity cellulose and lignin.
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FOOD CHEMISTRY
·
2025
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IF 9.8
Quanyu Zhang,Youling Feng,Hanyu Liu,Hao Zhang,Zhixun Ma,Xin Du,Xiufang Xia
Black soybean seed coat anthocyanins (BBSACN) have garnered considerable attention for their strong antioxidant and health-promoting properties, yet their inherent instability severely hinders practical applications. Cyclodextrin metal-organic frameworks (CD-MOFs) are commonly utilized for safeguarding and delivering active compounds. However, their susceptibility to damage in aqueous environments restricts the efficient loading of hydrophilic active ingredients. This study aimed to create a cross-linked CD-MOF (CLCD-MOF) system to enhance the stability of BBSACN under diverse conditions. Diphenyl carbonate was used as the crosslinker to generate a CLCD-MOF that maintained structural stability in water for 7 days. Thorough physicochemical characterization, including SEM, FTIR, XRD, and TGA, and molecular dynamics simulations verified the successful encapsulation of anthocyanins. The findings indicated that non-covalent interactions such as hydrogen bonding and hydrophobic forces notably enhanced the stability of anthocyanins during extended storage, heating, and light exposure. In comparison to free anthocyanins, those encapsulated in CLCD-MOF showed about 35 % higher retention under light exposure and even greater improvements during storage and heating. In conclusion, this study presents promising opportunities for utilizing CD-MOF carriers to tackle the increasingly intricate challenges in the food industry.
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Chen Tai,Huarong Liu,Yuan Hu
Hydrogen is a very promising green energy alternative to fossil fuel owing to both environmental friendliness and high-energy nature; however, improving the hydrogen production efficiency of photocatalysts under visible light has remained a challenge. Herein, CdS/Pt/MIL-125 nanocomposite has been fabricated using γ-ray irradiation, where Pt and CdS nanoparticles with clean surfaces are well dispersed inside and on the surface of MIL-125, respectively, which greatly promotes effective space separation of photogenerated carriers and thus improves the visible-light catalytic activity. The hydrogen generation rate of CdS/Pt/MIL-125 nanocomposite is found up to 6783.5 μmol/(g·h) under visible-light illumination, which is 7.3 times that of CdS/MIL-125 without Pt as electron trap reservoirs and 4.4 times that of Pt/CdS/MIL-125 without effective spatial separation between CdS and Pt. The reason is attributed to the synergy of ternary CdS/Pt/MIL-125 with a unique ordered mesoporous structure that may widen the absorption range of the light, improve the efficiency of light harvesting, facilitate mass transfer, prevent the aggregation of CdS and Pt nanoparticles, suppress the electron–hole (e–h) pair recombination, and provide more active sites. Moreover, the loading amount of Pt or CdS nanoparticles also affects the activity of CdS/Pt/MIL-125 nanocomposite for visible-light catalytic H2 evolution. In view of the extensive use of γ-ray irradiation in industry, this research presents a rational route to the fabrication of novel hybrid photocatalysts for improved visible-light catalytic hydrogen evolution.
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高影响因子
FUEL
·
2021
·
IF 6.609
Xueying Gao,Xin Yu,Lincai Peng,Liang He,Junhua Zhang
A magnetically-recoverable multifunctional catalyst (Fe 3 O 4 /ZrO 2 @MCM-41) was tailored by the impregnation of ZrO 2 supported on mesoporous MCM-41 coated Fe 3 O 4 nanoparticles, which successfully served as a monolithic catalyst for the cascade conversion of furfural (FAL) giving high yield to γ-valerolactone (GVL), a versatile platform molecule. The ordered hexagonal framework of the parent MCM-41 well reserved after the embedding of Fe 3 O 4 and ZrO 2 . The incorporation of Fe 3 O 4 could not only impart the catalyst with a strong magnetism, but also tune its acidity to promote GVL production. An impressive yield of 85% was accomplished straight from FAL processing with iso -propanol as a hydrogen donor and solvent. The kinetic study demonstrated higher activation energy for levulinate-to-GVL step (86.9 kJ/mol) than FAL transfer hydrogenation (35.0 kJ/mol) and subsequent alcoholysis process (51.0 kJ/mol). The catalyst could be fully recovered by an external magnetic field and showed good reusability. The sustainability of this conversion represents greatly improved by the process intensification based on one-pot reaction, magnetically-recoverable multifunctional catalyst, and mild operating conditions without using gaseous hydrogen.
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高影响因子
LANGMUIR
·
2021
·
IF 3.882
Qi Hao,Yuetong Kang,Jiang-Fei Xu,Xi Zhang
A novel fluorescence “turn-on” enzyme-responsive supra-amphiphile is developed based on the host–guest recognition between γ-cyclodextrin (γ-CD) and an amphiphilic tetraphenylethene-sodium glycyrrhetinate conjugate (TPE-SGA). The covalent amphiphile TPE-SGA displayed strong fluorescence in aqueous solution owing to the aggregation-induced emission. Upon addition of γ-CD, the fluorescence of TPE-SGA was effectively turned off due to the host–guest recognition with γ-CD prohibiting the aggregation of TPE-SGA in aqueous solution. The as-formed nonfluorescent supra-amphiphile (TPE-SGA/γ-CD) inherited the α-amylase-responsive property of γ-CD. In the presence of α-amylase, the fluorescence of the supra-amphiphile was gradually turned on owing to the hydrolysis of γ-CD, and the fluorescence intensity linearly correlated to the activity of α-amylase. This study enriches the field of supra-amphiphile on the basis of cyclodextrin-based host–guest chemistry and provides a novel strategy to construct fluorescence turn-on functioned self-assemblies. It is anticipated that the fluorescence turn-on supra-amphiphile has potential applications in biological analysis and diagnosis of pancreatic diseases.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wanchen Zhu,Zhongyang Luo,Feiting Miao,Longyi Liu,Akira Nakayama
Biomass hydropyrolysis (HP) vapor upgrading (VU) is highly promising for producing sustainable aviation fuel, yet challenges remain. This study focused on PdMo/γ-Al 2 O 3 and Mo/γ-Al 2 O 3 catalyzed HP-VU of biomass in a pressurized continuous fixed-bed and the reaction mechanism. The results demonstrated that the introduction of Pd enhanced the hydrodeoxygenation activity through multiple effects, including the generation of surface acidic sites, the formation of oxygen vacancies, and the effect of hydrogen spillover. Beyond this, the effects of upgrading temperature and pressure on the catalytic performance of PdMo/γ-Al 2 O 3 were also investigated. Under optimal conditions of 400 °C and 1.0 MPa, the organic phase achieved a mass yield of 12.03 wt%, with the selectivity of C4+ aliphatic hydrocarbons and monocyclic aromatic hydrocarbons reaching 77.01 %, leading to an HHV of 42.41 MJ/kg and high mass balance (98.71 %). Density functional theory calculations further provided insights into the role of defect sites in facilitating C–O/C=O bond cleavage and the contribution of Pd sites to C C bond activation. By integrating theoretical calculations with model compound experiments, the study revealed the potential reaction pathways including hydrodeoxygenation, hydrogenation, and C C coupling. This study provides practical and theoretical insights into the bimetallic-catalyzed HP-VU process of biomass.
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高影响因子
FOOD CHEMISTRY
·
2025
·
IF 9.8
Quanyu Zhang,Xin Du,Ruiping Liu,Hao Zhang,Xinjiang Lou,Yingchun Zhu,Xiufang Xia
Clove essential oil (CEO) possesses potent antioxidant and antimicrobial properties but suffers from high volatility and instability, limiting its application in food systems. A green, ethanol-mediated ultrasonic method was developed to synthesize biocompatible γ-cyclodextrin metal-organic frameworks (γ-CD-MOFs) with tunable particle size. Compared to conventional hydrothermal synthesis (3–5 μm), the ultrasonic approach yielded smaller, more uniform γ-CD-MOFs crystals (1–2 μm), which enhanced CEO loading (121 mg/g, +26 %) and improved structural stability. CEO encapsulation stabilized the framework through hydrogen bonding, van der Waals forces, and pore confinement, enabling sustained release at 4 °C and 25 °C. A clear size-dependent effect was observed, with smaller frameworks exhibiting superior loading efficiency and controlled release behavior. Molecular dynamics simulations elucidated the binding mechanism between CEO and the framework. CEO-loaded composites effectively inhibited microbial growth, extended pork shelf life, and exhibited good biocompatibility, offering a promising strategy for food preservation and controlled delivery of volatile bioactives.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 27
·13047-13053
·
IF 3.925
Feng Xu,Chao Liu,Jia-Xin Li,Cai-Zhen Zhan,Qi-Ning Xun,Wen-Shen Zhang,Wen-Fang Xing,Gang-Gang Chang
γ-Valerolactone (GVL) is an important lignocellulosic platform molecule with huge potential for various industrial and chemical applications, which is usually produced using levulinic acid (LA) or its esters as raw materials. However, a two-step reaction process in which hydrogenation of the carbonyl groups on metal sites and subsequent lactonization catalyzed by acidic sites over multiple catalysts has generally been needed to realize this synthesis. In this work, a hierarchically multifunctional single catalyst of Ru/phosphotungstic acid/hierarchically porous UiO-66 (Ru/HPW/HP-UiO-66), simultaneously integrated with acidic and metal sites, has been fabricated via a simple strategy and successfully applied in the one-pot synthesis of GVL using methyl levulinate (ML) as the raw material. The hierarchically porous and nanosized (∼15 nm) HP-UiO-66 can not only provide sufficient space for the mass transfer of substrates but also favors the loading of bulk HPW molecules, which can effectively mediate the catalytic activities and stability of Ru NPs using the confined pore effect of UiO-66 and the strong interaction between HPW and Ru. When applied in the one-pot synthesis of GVL, the hierarchical Ru/HPW/HP-UiO-66 catalyst showed excellent catalytic activity (>97% yield) and stability (maintained after 7 successive cycles) for GVL. More importantly, the hierarchical catalyst also exhibited an extraordinary performance in the hydrogenation of different unsaturated hydrocarbons in aqueous solution. It is expected that our study offers a novel route to biomass upgrades involving metal/acid bifunctional synergistic catalysts.
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高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2025
·
IF 5.2
Zi-Quan Wang,Ya-Peng Du,Xiao-Ping Zheng,Yu Chai,Yu-Cang Zhang,Yan-Zhen Zheng
The direct conversion of raw lignocellulosic waste into specialty chemicals such as levulinic acid (LA) has the potential to significantly enhance biorefinery profitability. Here, we demonstrated that incorporating γ-valerolactone (GVL) as a co-solvent during the SO 3 H-functionalized ionic liquid-catalyzed conversion of bagasse in water markedly enhanced reaction rates and catalytic activity, achieving a LA yield as high as 76.1 % with a 1:1 vol ratio of GVL to water. This catalytic system also effectively converted other lignocellulosic waste to LA. Reaction constants and activation energies for the bagasse dehydration process to LA were obtained. Comprehensive characterization via Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and X-ray diffraction (XRD) elucidated significant changes in functional groups, surface morphology, and crystallinity index of solid residues over extended reaction times. Notably, hemicellulose and cellulose were converted within 4 h, with lignin remaining in the solid residues and forming by-products after prolonged reaction times. This efficient one-pot conversion method showed promise as a sustainable approach to transform agricultural waste into LA, offering new opportunities for eco-friendly resource utilization.
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