APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Huiling Zhang,Xiaomei Zhou,Longxin Liu,Fujun Lan,Teng Zhao,Mo Qiu,Qingxin Guan,Wei Li
Atomically dispersed cluster catalysts own versatile applications in biomass valorization, while the controllable assembly and microenvironmental regulation remain a crucial challenge. Herein, Co clusters assembled via nanosized ZIF-67 sprouted from Co-Al layered double hydroxide nanoflowers were applied for selective hydrogenation of furfural (FAL). The pyrolysis temperature can tune the microstructures and acid properties of the catalyst, which accounts for the hydrogenation of FAL to furfuryl alcohol (FOL), 2-methylfuran (2-MF), and tetrahydrofurfuryl alcohol (THFOL) with yield of 99.1 %, 96.7 %, and 82.3 %, respectively. The Co clusters favor C O bond adsorption via bridging-type adsorption mode while suppressing the furan ring adsorption. Moreover, ultra-dispersed Co clusters facilitate the cleavage of C-OH bonds in FOL intermediate, leading to a high 2-MF yield. As the pyrolysis temperature increase, the formed Co nanoparticles are conducive to the parallel adsorption of FAL, resulting in the production of THFOL. This work affords a multi-functional catalyst in catalytic biomass upgrading.
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CATALYSIS TODAY
·
2023
·
IF 5.3
Zhenyu Li,Enhui Du,Panpan Hao,Liyuan Huai,Yang Zhong,Soliman I. El-Hout,Chunlin Chen,Jian Zhang
The oxidation of biomass-derived 5-hydroxymethyl furfural (HMF) into 2,5-Furandicarboxylic acid (FDCA) is a favorable reaction since FDCA is an ideal alternative to petroleum-based monomer terephthalic acid in bio-based polyester industry. However, producing FDCA with high yield under mild conditions is still challenging, especially at energy-saving near-ambient temperatures. Here, we present a Pd nanoparticles catalyst supported on Vulcan XC-72 carbon (Pd/VC) that can completely convert HMF and achieve an encouraging FDCA yield (92.4%) at 30 ℃. The most important observations include yield declines at pure oxygen bubbling, and the transformation of intermediates becomes stagnant; instead, switching to the diluted oxygen is effectively driving the tandem oxidation as the over-oxidation, and thus, rapid deactivation of the Pd surface could be alleviated. The negative effect of high oxygen concentration also occurs in the dehydrogenation and oxygenation of an extended substrate. Since the decisive influence of oxygen content has often been neglected in past investigations of oxidative transformation over Pd-based catalysts, the current study may offer a critical reminder for other liquid-phase oxidation reactions.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuchao Shao,Zhangrui Luo,Menggang Bao,Weizhong Huo,Rong Ye,Muhammad Ajmal,Wenjing Lu
Acid hydrothermal treatment of biowaste is a beneficial approach for producing hydrochar with high hydrothermal humic acid (HHA) selectivity, along with a by-product hydrothermal solution containing saccharides, furans, and aromatic compounds. Conversely, alkaline hydrothermal conditions are suitable for humification to form HHA. This study explored the recycling of hydrothermal solution as a solvent for hydrochar production, aiming to reduce salt content in wastewater and the need for acid/alkali inputs. The acidity of the recycled hydrothermal solution significantly influenced the quality of the prepared hydrochar in terms of alkaline hydrothermal humification. Insufficient solution acidity resulted in a decrease in hydrochar-derived HHA yield (65.0 wt% to 20.2 wt%). Maintaining sufficient acidity (pH 0) in the recycled hydrothermal solution not only improved the hydrochar yield (29.6 wt% to 33.1 wt%) via polymerization or condensation reactions but also maintained ab high level of hydrochar-derived HHA yield (68.2 wt% to 71.2 wt%). This can be attributed to adequate hydrolysis of biowaste and polymerization of soluble chemicals into the hydrochar. Furthermore, the total yields of hydrochar-derived and solution-derived humic substances were higher compared to values obtained without hydrothermal solution recycling. This study presents an innovative hydrothermal process for HHA production, offering cost savings and environmental benefits.
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2023
·
IF 8.7
Jie Liu,Dawei Xu,Qian liu,Shuirong Li,Dechao Wang,Zhifeng Zheng
Functional groups on carbon substrates help to anchor conductive polymers through electrostatic interactions, but excessive groups are usually contradictory to the improvement of graphitization, which is closely relevant to the conductivity of electrodes. Herein, the balance between graphitization and oxygen-containing functional groups of carbon substrates was analyzed via adjusting the carbonization temperature ( T c ) of carbon foams (CFs) and fabricating polypyrrole (PPy)/CFs free-standing electrodes. The graphitization of CFs is accompanied by the dissociation, migration and rearrangement of O atoms, resulting in structural changes of CFs at different T c , which affects the morphology of PPy, as well as the adsorption and electron transfer between CFs and PPy. Besides, the increase of T c improves the conductivity and rate capability of composite electrodes due to the graphitization enhancement of CFs. However, the accompanied reduction of functional groups results in the densification of PPy coatings, which causes the attenuation of specific capacitance and cycling stability of composite electrodes. In addition, PPy/CFs can show much better electrochemical performances than that of the pure PPy film, with a specific capacitance of 545.5F g −1 (1 A/g) and a 100% capacitance retention after 10,000 GCD cycles.
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高影响因子
NATURE
·
2023
·Vol. 621
·期 7979
·511-515
·
IF 64.8
Yang Guangxu,Gong Zhenggang,Luo Xiaolin,Chen Lihui,Shuai Li
Plywood is widely used in construction, such as for flooring and interior walls, as well as in the manufacture of household items such as furniture and cabinets. Such items are made of wood veneers that are bonded together with adhesives such as urea–formaldehyde and phenol–formaldehyde resins 1 , 2 . Researchers in academia and industry have long aimed to synthesize lignin–phenol–formaldehyde resin adhesives using biomass-derived lignin, a phenolic polymer that can be used to substitute the petroleum-derived phenol 3 , 4 , 5 , 6 . However, lignin–phenol–formaldehyde resin adhesives are less attractive to plywood manufacturers than urea–formaldehyde and phenol–formaldehyde resins owing to their appearance and cost. Here we report a simple and practical strategy for preparing lignin-based wood adhesives from lignocellulosic biomass. Our strategy involves separation of uncondensed or slightly condensed lignins from biomass followed by direct application of a suspension of the lignin and water as an adhesive on wood veneers. Plywood products with superior performances could be prepared with such lignin adhesives at a wide range of hot-pressing temperatures, enabling the use of these adhesives as promising alternatives to traditional wood adhesives in different market segments. Mechanistic studies indicate that the adhesion mechanism of such lignin adhesives may involve softening of lignin by water, filling of vessels with softened lignin and crosslinking of lignins in adhesives with those in the cell wall.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xian Shi,Xinyi Xing,Mengya Ruan,Qichun Wei,Ying Guan,Hui Gao,Siquan Xu
Efficient and green catalysis of cellulose to 5-hydroxymethylfurfural (HMF) is currently a challenge that needs a breakthrough. In this study, a series of inexpensive (x)SO 4 2- /HfO 2 heterogeneous catalysts were prepared and exhibited superior catalytic performance for conversion of cellulose into HMF in the green water-tetrahydrofuran monophasic system (H 2 O-THF). An optimal HMF yield of 54% was acquired through detailed evaluation of reaction conditions. Various analyzes including ICP-OES, XRD, SEM, TEM, FTIR, N 2 adsorption–desorption isotherm, XPS, TG, NH 3 -TPD and Py-FTIR were applied to inspected the physicochemical characteristics of the (x)SO 4 2- /HfO 2 catalysts. Meanwhile, the recyclability of the catalyst and the by-products generated during the reaction process were studied and captured, respectively. The results presented herein show that the catalytic system of (30%)SO 4 2- /HfO 2 catalyst combined with H 2 O-THF monophasic solvent is advanced, and it can be both green and efficient without the presence of other additives and promoters, and has great potential in the future.
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JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE
·
2023
·Vol. 103
·期 15
·7631-7642
·
IF 4.1
Dongshuang Liang,Haosong Wen,Yaxuan Zhou,Taohong Wang,Guangqun Jia,Zongyan Cui,Adan Li
Background Honey aroma is one of its most important properties and it depends on the qualitative and quantitative composition of the volatile compounds. The volatile profile of honey could reveal its botanical origin to avoid a false characterization. Thus, it is of great significance to honey authentication. This study developed and validated a headspace solid-phase microextraction and gas chromatography–mass spectrometry (HS-SPME-GC–MS) method for simultaneous qualitative and quantitative analyses of 34 volatile components in honey. The developed method was applied to 86 honey samples from six different botanical origins, including linden honey, rape honey, jujube honey, vitex honey, lavender honey and acacia honey. Results The volatile fingerprints and quantitative results were simultaneously obtained by using the full scan and selected ion monitoring (SCAN+SIM) MS scanning mode. The limits of quantification (LOQs) and limits of detection (LODs) of 34 volatile compounds were in the ranges of 1–10 ng/g and 0.3–3 ng/g, respectively. And the spiked recoveries ranged between 70.6% and 126.2%, with the relative standard deviations (RSDs) not higher than 45.4%. A total of 98 volatile compounds were found with relative contents determined, and the 34 volatile compounds were determined with absolute concentrations. Based on the volatile fingerprints and the contents of volatile compounds, honey samples from six botanical origins were well classified by principal component analysis and orthogonal partial least-squares discrimination analysis. Conclusions The HS-SPME-GC–MS method was successfully applied to achieve the volatile fingerprints of six types of honey and to quantitatively analyze 34 volatile compounds with satisfying sensitivity and accuracy. Chemometrics analysis showed significant correlations between honey types and volatiles. These results reveal the characteristics of volatile compounds in six types of unifloral honey and provide some supports for honey authentication. © 2023 Society of Chemical Industry.
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PubMed
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Peiqi Liu,Wanyun Shao,Zhen Yang,Jiuzhong Yang,Liangyuan Jia,Yang Pan,Zhongyue Zhou,Yingquan Chen,Fei Qi
Reactive intermediates are essential for determining the reaction mechanism of biomass pyrolysis. However, these short-life compounds are rarely reported because they are difficult to probe and identify. Here, the catalytic pyrolysis of furanic compounds over HZSM-5 was investigated by combining a low-pressure reactor and an in situ synchrotron vacuum ultraviolet photoionization molecular beam mass spectrometer (SVUV-PI-MBMS). Important reactive intermediates (m/z < 200) can be detected and characterized by this in situ analysis method, which also allows studying the dynamics of volatile formation as a function of catalyst deactivation. Strikingly, formaldehyde and acetaldehyde as reactive intermediates in the upgrading of 5-methylfurfural (5-MFF) are mainly produced from its side-chain cracking on the external surface of the zeolite, while their conversion is highly related to the contribution of the Brønsted acid site inside the zeolite. It is also evidenced that reactive methylcyclopenadienes (MCPDs) are formed from various compounds (alkynes, furans and olefins) and can be further converted to methylbenzenes (MBs) via ring-expansion. Finally, more complete conversion pathways that contain reactive intermediates for zeolite-catalyzed pyrolysis of furanic compounds are proposed. The key roles of some reactive intermediates in promoting the deoxidation and aromatization of furans are also illustrated.
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POLYMER DEGRADATION AND STABILITY
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2023
·
IF 5.9
Yadong Wang,Li Ma,Hua Wang,Chunzu Cheng,Xianze Yin,Zongmin Zhu
Polylactic acid (PLA) has garnered global attention as a potential biomaterial thanks to its biodegradability and renewability. However, the drawbacks of its high flammability impede its broader application. In this work, two different types of all bio-based charring agents (named as CFU, CVA) were prepared in a green and environmentally friendly ethanol solvent by using chitosan derived from corn starch and sugarcane, as well as bio-based vanillin and furfural, as raw materials. The CFU (or CVA) in conjunction with ammonium polyphosphate (APP) were incorporated into PLA to prepare flame-retardant and high-performance composite materials. The addition of 3.75 wt% CFU (or CFA) and 11.25 wt% APP to PLA resulted in the attainment of the UL-94 V-0 rating, a nearly 28% of limiting oxygen index, as well as a decrease of ∼35 and ∼90% in total heat and smoke releases, respectively. Besides, the addition of mixed flame retardants significantly reduced the viscosity of PLA by an order of magnitude, which was greatly beneficial for processing and production. The mechanical performance testing results demonstrated an increase in the elongation at break and impact strength of PLA composites containing CFU (or CVA) and APP. Moreover, the heat resistance and crystallinity of the PLA composites were also improved.
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CHEMICAL PAPERS
·
2023
·Vol. 77
·期 10
·5999-6006
·
IF 2.2
Yuan Yifan,He Fuduo,Li Xue,Xu Dehua,Yan Zhengjuan,Wang Xinlong
Corncob has a high yield and contains a large number of cellulose substances. Wet phosphoric acid hydrolysis of corncob is of great significance to the utilization of organic waste, and provides theoretical support for the development of sugar-containing synergistic phosphorus fertilizers. In this study, the kinetics of hydrolysis of corncob by wet process phosphoric acid was investigated. The time evolution of total sugar, xylose and furfural formation during a 12-h hydrolysis was simulated by Saeman and biphasic models within differential acid concentrations and temperatures. The formations of both total sugar and furfural coincide a first-order irreversible reaction, which was not applicable to the Saeman model nor the biphasic model. Meanwhile, xylose formation was more suitable for the Saeman model. The optimal conditions for xylose are: a temperature of 100 °C, a reaction time of 720 min, an acid concentration of 55.6% (w/w). The xylose yield of corncobs was 0.15 g/g in the optimal conditions. Graphical abstract
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xinxin Li,Linchuan Cong,Yupeng Wu,Nan Lin,Fangbing Liu,Deyuan Xin,Fuyu Han,Jin Yang,Weitong Chen,Haibo Lin
Electrochemical methods for catalytic furfural conversion have drawn significant interest in both academic and industrial research communities. Paired electrocatalytic conversion has been identified as a promising strategy for reducing energy consumption and promoting carbon neutrality. To optimize product distribution and conversion efficiency, we have developed a divergent paired electrochemical upgrading approach for furfural in acidic environments, with a focus on prioritizing strong gas evolution reactions and product transformations. The high electrocatalytic activity of CuSn/CuF@Cu prepared by electrodeposition can effectively inhibit the hydrogen evolution. The performance of the electrocatalysts and the pathways of electrocatalytic hydrogenation (ECH) of furfural to 2-methylfuran (MF) were investigated by combination of experiments and the density functional theory (DFT) calculations. A stable Ti/PbO 2 electrode with high oxygen evolution overpotential was prepared for anodic electrocatalytic oxidation (ECO) and the product transformation route was described. The conversion of furfural to maleic acid (MA) and MF in acidic environment was successfully achieved. In the paired electrosynthesis system, the electrons generated from anodic ECO of furfural are utilized in valuable and controllable cathodic ECH. It significantly and continuously reduces the power cost associated with renewable energy sources and further promotes the development of biomass electrochemical conversion.
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高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Yiwei Tang,Xiaoning Liu,Ran Xi,Le Liu,Xinhua Qi
As one of the important chemical feedstocks and biofuels, ethyl levulinate (EL) can be produced from biomass-derived furfural by consecutive hydrogenation, etherification and ring-opening reactions. However, this process normally requires two separate steps in different reaction systems, which is complex and energy consumption. Herein, Nb–Ni bifunctional ordered mesoporous carbons (Nb/ [email protected] ) were synthesized by a two-step process where [email protected] was firstly synthesized by a solvent evaporation induced self-assembly (EISA) process using F127 as a template agent, polyphenol gallic acid as carbon precursor and Ni 2+ as cross-linker, following with the supporting of Nb species in the [email protected] by an incipient wetness impregnation method. The as-synthesized Nb/ [email protected] samples were applied for the one-pot catalytic transformation of furfural to EL, and exhibited good activity with the highest EL yield of 83% under an optimized condition. Two possible pathways for the one-pot production of EL were proposed according to two intermediates: (1) hydrogenation of furfural to form furfuryl alcohol (FFA) that is then etherified with ethanol to form 2-(ethoxymethyl)furan (2-EMF); and (2) acetalization and etherification of furfural with ethanol to produce 2-(diethoxymethyl)furan (2-DMF). Then both 2-DMF and 2-EMF are converted to EL through acid catalyzed ring opening reaction. The dominant reaction pathway varied with the properties of the catalyst and the applied reaction conditions.
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危险品化学品经营许可证（带存储）