FUEL
·
2023
·
IF 7.4
Yang Shen,Chunjiang Liu,Cunhao Cui,Hairong Ren,Mingming Gu,Haoran Liu,Zhongyue Zhou,Fei Qi
Lignin catalytic pyrolysis presents a promising and sustainable approach to producing aromatic molecules. Herein, we investigated the effect of modified zeolite with copper (Cu/HZSM-5) catalyst on efficiently pyrolyzed kraft lignin into aromatic hydrocarbons (AHs) production, especially mononuclear aromatic hydrocarbons (MAHs). Time-of-flight mass spectrometry (TOF-MS) was employed to compare the volatile product profiles of lignin during catalytic pyrolysis. The highest yield of MAHs reached 70.59 mg/g based on dry lignin at 550 °C, accounting for 70.23% among lignin pyrolysis products, compared to the pristine HZSM-5 zeolite catalytic system with MAHs yield of only 54.31 mg/g and of 40.34% in products. At 550 °C and 60 s residence time, the 5% Cu/HZSM-5 catalyst demonstrated the best performance compared to all other catalysts in terms of selectively producing MAHs. The results are ascribed to the enhancement of decarboxylation and aromatization processes by the doping of copper. This work demonstrates a cost-effective pathway that potentially converts kraft lignin into aromatic hydrocarbon production at a phenomenally high selectivity, providing a concept for industrial application toward biomass utilization and high value-added production.
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Ming Zhan,Yue Wang,Huai Liu,Rui Zhang,Lincai Peng,Junhua Zhang
Visible-light-driven upgrading of biomass and its derivatives into value-added chemicals under mild reaction conditions is an economical and sustainable strategy for biomass valorization. In this contribution, industrially-accessible anthraquinone and its derivatives (AQs) have been developed as efficient metal-free photocatalysts for the photo-oxidation of 5-hydroxymethylfurfural (HMF). Especially, a quantitative furans selectivity containing 86.0 % of 2,5-diformylfuran (DFF) and 13.6 % of 5-formyl-2-furancarboxylic acid (FFCA) was implemented at HMF conversion of 88.8 % over 2,6-dibromoanthraquinone (2,6-DB-AQ) catalyst under visible light illumination. In addition, the homogeneous 2,6-DB-AQ catalyst can be readily separated and recycled from the reaction mixture by a “water-assisted” precipitate method. Photophysical characterizations indicated that the introduction of bromine substituents on AQ enhances its visible light absorption ability, decrease its band gap energy and enables the catalyst with a more stable photoexcitation state. It has also been demonstrated that the lower photoexcitation energy of O 2 over 2,6-DB-AQ endowed the catalyst with better capacity for the activation of O 2 than that of AQ. These contributions should be in charge of the excellent catalytic activity of 2,6-DB-AQ for the photo-oxidation of HMF. This work demonstrates an efficient and recyclable organo-photocatalyst for the visible-light-mediated valorization of biomass-derived alcohols and aldehydes to value-added chemicals.
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 4
·1170-1179
·
IF 2.936
Luo Mingsheng,Li Hong,Song Huanqiao,Shao Changke,Wang Aimei
The alkylation of phenol with methanol was studied in vapor phase over 5 wt% cerium supported on HZSM-5 catalyst prepared by three different methods, such as impregnation, ball mixing and solid-state ion-exchange. The catalytic activities are tested in a fixed-bed reactor, and the physicochemical properties of the catalyst are characterized with X-ray powder diffraction, scanning electron microscope, nitrogen physical sorption, Fourier Transform Infrared Spectrometer, Infrared spectra of pyridine adsorption, X-ray photoelectron spectroscopy and temperature-programmed desorption of ammonia. It was found that the dispersion form of cerium was greatly affected by the preparation method, and difference in acidity affects catalytic performance in the alkylation reaction of phenol and methanol. Ball milling method generated greater amount of strong Brønsted acidic sites and lower specific surface area than other catalysts, which led to higher carbon deposition rate and lower catalyst activity. The catalyst prepared by impregnation method yields higher Lewis acid concentration (2.09 μmol/g) and more chemisorbed oxygen due to the increased Ce 3+ concentration in the lattice, resulted in an improved o-cresol selectivity of 48%. Furthermore, the catalyst prepared by solid-phase ion-exchange method produces a catalyst with appropriate B/L ratio of 60.6 and large specific surface area of 389.0 m 2 /g, which yields the highest phenol conversion of 23%. Graphical Abstract
✓ 已验证
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2026
·
IF 13.5
Yafei Jiang,Shixing Xu,Qingze Ma,Jiaxuan Zhang,Weishuo Wang,Yanzhao Yang,Hao Tian
Converting glucose into value-added cyclic carbonates is a promising route for carbon utilization, and strongly influenced by the acidic properties and mass transport characteristics of solid acid catalysts. In this study, H-ZSM-5 nanosheets with varied Si/Al ratios were synthesized to investigate the effects of framework composition and b -axis length on glucose conversion. Increasing the Si/Al ratio decreased the density of acid sites but simultaneously reduced the b -axis length, enriched aluminum species near the external surface, and increased the relative abundance of Lewis acid sites, thereby enhancing the accessibility and utilization of active site. Consequently, H-ZSM-5_100 exhibited the highest site time yield, the lowest apparent activation energy, and the highest selectivity toward fructose and 5-hydroxymethylfurfural (5-HMF). Under optimized reaction conditions, H-ZSM-5_100 achieved a glucose conversion of 56.3% with a 5-HMF formation rate of 42.8 mmol h −1 g −1 . These results demonstrate that the catalytic performance of H-ZSM-5 nanosheets is governed by the synergistic effects of framework composition, the distribution of acid site, and crystal morphology, providing guidance for the rational design of zeolite catalysts for biomass conversion. Rational regulation of zeolite acidity and diffusion properties is crucial for efficient biomass conversion. This work presents H-ZSM-5 nanosheets with tunable Si/Al ratios are developed to reveal the synergistic effects of acid site distribution and b -axis length on glucose conversion, enabling enhanced production of fructose and 5-hydroxymethylfurfural through optimized active-site accessibility. Download: Download high-res image (175KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2023
·Vol. 13
·期 49
·34660-34669
·
IF 3.9
Yu Huang,Yanqin Rong,Wenjia Zhang,Zibin Zhang,Xiaoyuan Zhang,Wenting Liang,Cheng Yang
A carboxylatopillar[5]arene-embellished (CP5) magnetic graphene oxide nanocomposite (MGO@CP5) was smoothly constructed via a mild layer-by-layer method. The morphology, structure, and surface characteristics of this nanocomposite was investigated by field-emission scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, Raman spectroscopy, zeta potential, and other techniques. Benefiting from a high capture ability for small molecules of CP5 as a supramolecular host molecule, along with a negative surface charge and large surface area of MGO@CP5, this nanocomposite exhibits an ultrafast, efficient adsorption property for representative cationic dyes: methylene blue (MB) and basic fuchsin (BF). The removal efficiency of MB and BF can reach nearly 99% within 3 min, while the maximum adsorption capacity of the two dyes reaches 240 mg g−1 for MB and 132 mg g−1 for BF. Furthermore, owing to excellent magnetic responsiveness from the tight loading of Fe3O4 nanoparticles on graphene oxide, MGO@CP5 could be easily and magnetically separated, regenerated, and reused four times without an evident reduction in the removal efficiency (>95%). Impressively, the adsorption property of MGO@CP5 reveals a strong tolerance to pH changes and ionic strength interference, which renders it a promising adsorbent in the field of water treatment.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Yaping Liu,Chao Pan,Xiaomin Qiu,Xianjie Li,Hengjun Gai,Meng Xiao,Tingting Huang,Quanhong Zhu,Hongbing Song
Although fossil fuels bring convenience to the production and life of people, they also cause numerous environmental problems. As a result of overexploitation, fossil fuels are gradually being depleted as a nonrenewable resource. Biomass is a green and renewable resource and has attracted people’s attention. As a platform compound derived from renewable biomass, 5-hydroxymethylfurfural (HMF) is important for in-depth research. The oxidative esterification process from HMF to dimethyl furan-2,5-dicarboxylate (FDMC) was achieved using a gold (Au) nanoparticle (NP) catalyst supported on poly(ionic liquid)s (PILs). The comprehensive characterization of the synthesized catalyst showed that the Au NPs were successfully loaded on PILs, and a strong interaction occurred between the catalyst support and the metal. In this work, 10 %Au/PILs-Cl-1 was used as the best catalyst. The conversion of HMF ( C HMF ) and the selectivity to FDMC ( S FDMC ) reached 95.08 % and 96.82 %, respectively, under the conditions of 120 °C, 1.5 MPa, 12 h, and 0.5 equiv. CH 3 ONa. In addition, cycling experiments indicated the stability and successfully recycling of 10 %Au/PILs-Cl-1 catalyst.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Yu Chen,Haoquan Guo,Junye Yang,Kaiyang Xu,Xinyu Lu,Yue Yang,Hongqiao Lin,Lizhi Wu,Li Tan,Guohui Yang,Noritatsu Tsubaki,Xiaoli Gu,Yu Tang
Dimethylfuran is a promising liquid fuel that can be derived from sustainable biomass sources. Obtaining dimethylfuran from biomass through an efficient catalytic hydrodeoxygenation process is an effective way to achieve carbon neutrality. Herein, we report a catalytic system employing a highly dispersed Pd-Co bimetallic catalyst supported on molybdenum carbide for the conversion of 5-hydroxymethylfurfural to dimethylfuran. Bimetallic catalysts with varying Co loading were prepared via co-precipitation and temperature-programmed carburization, followed by a series of hydrodeoxygenation performance evaluation. The results reveal that, at 180 °C and 2 MPa hydrogen pressure, the 0.5Pd10Co/MoC x catalyst achieves a remarkable 5-hydroxymethylfurfural conversion of 99.9 % with a dimethylfuran selectivity exceeding 97 %. Comprehensive characterizations confirm the role of bimetallic active sites and suggest the reaction mechanism. Pd doping enhances the surface area and promotes hydrogen dissociation, and consequently lowering the reduction temperature of catalyst. The unique electronic structure of Mo in the carbide support promotes charge transfer from the support to the Pd-Co bimetallic site, thereby promoting the generation of more Co δ+ and Co 2+ . The presence of a high oxygen vacancy content facilitates the cleavage of C-O bonds, while the synergy effect of bimetallic sites changes the reaction path and promotes the hydrogenation of the aldehyde group, thus greatly improving the reaction efficiency.
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 5
·2058-2068
·
IF 10.182
Changqu Lin,Chaoqun Chai,Yuanzhang Li,Jiao Chen,Yanyu Lu,Hongli Wu,Lili Zhao,Fei Cao,Kequan Chen,Ping Wei,Pingkai Ouyang
Alkaline earth metal salts are environmentally friendly and economical. They have attracted much attention in the process of biomass conversion, especially for isomerization and dehydration. However, the lack of understanding of the alkaline earth metal-mediated catalytic mechanism prevents the achievement of high HMF yields from glucose or fructose. Herein, we performed experimental and theoretical studies on CaCl2-catalyzed glucose-to-fructose isomerization and fructose-to-HMF dehydration. In CaCl2 solution, the highest fructose yield (33.6%) from glucose can be achieved at 80 °C. Meanwhile, the presence of CaCl2 in fructose-to-HMF dehydration notably improved fructose conversion. A “one-pot” isomerization–dehydration of glucose to prepare HMF was designed and 100% conversion and 52.1% HMF yield were obtained. The CaCl2 solution can be reused for five runs while maintaining catalytic activity without regeneration. Through 1H NMR, 13C NMR, DOSY-NMR and DFT calculations, we concluded that the coordination between the C1/C2 sites of the β-glucopyranose tautomer and CaCl2 promoted the 1,2-intramolecular hydride shift of glucose, thus rapidly converting glucose into fructose. Similarly, Ca2+ can complex with the C2/C6-OH of β-D-fructofuranose and stabilize this tautomer, which easily forms HMF. This is the main reason that CaCl2 can promote the preparation of HMF from fructose.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ruixia Yang,Qiaohong Peng,Bing Yu,Youqing Shen,Hailin Cong
Yolk-shell Fe 3 O 4 @MOF-5 nanocomposites were synthesized by utilizing a simple solvothermal method. The physicochemical properties of the yolk-shell Fe 3 O 4 @MOF-5 nanocomposites were characterized by transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET) and vibrating sample magnetometer (VSM) methods. The nanocomposites had a catalytic yolk, a hollow cavity and a porous shell. The nanocomposites had relatively high specific surface area of 203 m 2 g −1 and showed superparamagnetic property. The catalytic activities of the yolk-shell Fe 3 O 4 @MOF-5 nanocomposites were evaluated by using methylene blue dye as a model pollutant. It is demonstrated that the yolk-shell Fe 3 O 4 @MOF-5 nanocomposites as a heterogeneous Fenton-like catalyst exhibited excellent catalysis since the internal cavity provided a relatively stable micro-environment for the reaction of the active ·OH radicals and the pollutants on the basis of the confinement effect. Furthermore, the yolk-shell Fe 3 O 4 @MOF-5 nanocomposites could be lightly separated from the pollutant solution by an external magnetic field and maintained good catalytic activity after five recycles, indicating the good stability of the nanocomposites.
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Biao Zhu,Yang Qin,Jiawei Du,Fazhi Zhang,Xiaodong Lei
Electrocatalytic biomass valorization with renewable energy input represents a promising way to produce sustainable and non-fossil-based carbon products. The oxidative production of furandicarboxylic acid (FDCA) from bio-based 5-hydroxymethylfurfural (HMF) has attracted one of the most attention. Herein, spinel CuMn2O4 with an urchin-like nanostructure was synthesized by a hydrothermal method and subsequently soaked in ammonia water to create oxygen vacancies. The as-prepared material was used as an efficient electrocatalyst to oxidize HMF to FDCA. It was confirmed that CuMn2O4 etched with ammonia has an excellent electrocatalytic performance: at a current density of 20 mA/cm2, the potential of HMF oxidation was 1.31 V vs RHE in 1.0 M KOH solution with 10 mM HMF prior to the takeoff of the competing reaction, O2 evolution. Long-term chronoamperometry demonstrated that a 100% conversion of HMF and a 96% Faradaic efficiency of yield of FDCA were achieved. Our results indicated that it is feasible to employ the earth-abundant transition metal-based electrocatalyst CuMn2O4 to selectively oxidize biomass with higher energy conversion efficiency than water splitting as well as to produce valuable products in a H-type electrochemical cell.
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2020
·
IF 2.87
Xing Huang,Guangcai Zhang,Lu Zhang,Qinhui Zhang
This work presented the microfluidic preparation of zeolite film in a capillary microchannel with different length-to-diameter ratios. In the quartz capillary with an inner diameter of 0.53 and 0.32 mm, Zeolite Socony Mobil-5 (ZSM-5) film was prepared by a continuous flow hydrothermal method. Considering the chemically inert surface of quartz capillary and the difficulty of preparing uniform and continuous zeolite film by conventional static synthesis, the ZSM-5 seed layer was precoated as active sites to induce film growth. The parameters of length-to-diameter ratio, seed coating, feed flow rate, and synthesis time were investigated. It revealed that the crystallinity of the ZSM-5 film was significantly affected by the capillary length-to-diameter ratio and seed coating in this flow system. The film morphology and thickness could be precisely controlled by adjusting the feed flow rate and synthesis time. This hydrogen form of the ZSM-5 (HZSM-5) film capillary microreactor was applied in the ketalization reaction of glycerol with acetone to produce solketal. The single-pass yield of solketal could reach ∼30% under mild conditions. This work provided a convenient stratagem of preparing zeolite catalytic coating or other support coatings in closed microchannels with a high length-to-diameter ratio and the potential application in valuable transformation of biomass glycerol.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 9
·1624
·
IF 4.324
Haian Xia,Jiahuan An,Weizi Zhang
The metal–support interaction (MSI) has a remarkable effect on the catalytic properties, but how to precisely modulate its degree remains a huge challenge. Herein, polyvinylpyrrolidone (PVP) with three different molecular weights (MWs) (24, 58, and 130 kDa) was used as a capping agent to fabricate Ag nanoparticles (NPs) supported on ZrO2. The physiochemical properties of the catalysts were characterized by X-ray diffraction (XRD), Transmission Electron Microscope (TEM), X-ray Photoelectron Spectroscopy (XPS), and Fourier transform infrared (FT-IR) techniques. The impacts of MSI on the catalytic activity and reaction kinetics for aerobic oxidation of 5-hydroxymethylfurfural (HMF) were investigated. The results showed that the introduction of PVP with various MWs could efficiently tailor the interfacial interactions and charge transfers (CT) among PVP, the support, and Ag NPs, thereby affecting the oxidation activity of HMF. The turnover number (TON) for HMF oxidation decreases in the order of unsupported colloidal Ag clusters > Ag/ZrO2(58,000) > Ag/ZrO2(130,000) > Ag/ZrO2(24,000) > Ag/ZrO2. The reason for this large difference in the catalytic activity for HMF oxidation is that various MWs of PVP result in a change of MSI, thereby facilitating CT from PVP to Ag metal sites. This study offers a new strategy for modulating MSI by varying the MW of capping agents, thereby tuning the catalytic properties in the oxidation of HMF.Keywords:metal–support interaction;molecular weight;capping agent;PVP;HMF oxidation
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）