RENEWABLE ENERGY
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2022
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IF 8.634
Jun Zhang,Chengyu Li,Sheng Hu,Jing Gu,Haoran Yuan,Yong Chen
In the present study, CuO and Cu 2 O were employed in H-transfer transformation of bio-based furfural (FFR) using methanol as both the solvent and an in-situ hydrogen source , to clearly elucidate the catalytic mechanism of copper oxides (CuO x , x = 0.5, 1) during the reaction. A number of characterization techniques including XPS , H 2 -TPD, in-situ FTIR, etc., were undertaken to track the state of copper species. Owing to the synergistic effect of in-situ generated H 2 , Cu 0 species and CuO x derived Brønsted/Lewis acid sites, FFR could be efficiently hydrogenated into FA and subsequently deoxygenated into MF in methanol. The combined results from in-situ characterizations and experiments show that the FFR-to-FA (FA, furfuryl alcohol) and FFR-to-MF (MF, 2-methylfuran) conversions largely depended on the hydrogen production capability from methanol reforming and FFR adsorption strength over CuO x . Density functional theory (DFT) calculations demonstrated that the CuO(200) surface revealed lower free energy and energy barriers for methanol reforming and FFR transfer hydrogenation. This study provides a promising guidance for reasonably designing copper-based materials in the hydro-upgrading of bio-based unsaturated molecules into value-added chemicals in methanol without external H 2 supply.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Ye Meng,Yumei Jian,Jie Li,Hongguo Wu,Heng Zhang,Shunmugavel Saravanamurugan,Song Yang,Hu Li
The appropriate regulation of photocatalyst band structure by simultaneous introduction of active sites is an effective strategy in constructing efficient photocatalytic systems for biomass valorization. Herein, a renewed host–guest photocatalyst (Ov-WO 3 @CB[5]) prepared by anchoring cucurbit[5]uril on oxygen vacancy-rich WO 3 was efficient for reductive upgrading of biomass derivatives using NH 3 -BH 3 , such as cascade photocatalytic hydrogenation-cyclization of ethyl levulinate to γ-valerolactone (up to 99 % yield) at 25 °C in 1 h, and quantitative production of primary/secondary bio-alcohols or arylamines from various aldehydes/ketones or nitroarenes, respectively. Also, the rate of H 2 production by direct photocatalytic hydrolysis of NH 3 -BH 3 could reach 5.75 mL h −1 g −1 . The inclusion of cucurbit[5]uril effectively adjusted the semiconductor band structure and enhanced migration efficiency of photo-generated carriers, and the hydrophobic cavity of cucurbit[5]uril favored the entrance of NH 3 -BH 3 , as elaborated by theoretical calculations. Properly engineering supramolecular surface-active sites based on interface host–guest chemistry opens new avenues for reductive upgrading of biomass and hydrogen evolution.
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高影响因子
Foods
·
2022
·Vol. 11
·期 17
·2662
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IF 5.561
Xiangying Yu,Xiaochun Chen,Yuting Li,Lin Li
To reflect the volatile differences of dried citrus peel as affected by cultivars and drying methods, the volatile compounds of dried citrus peel of two cultivars (Citrus reticulata“Chachi” andCitrus reticulata“Ponkan”), prepared under three drying methods (sun-drying (SD), hot-air-drying (AD), and freeze-drying (FD)), were analyzed by GC-MS, odor activity values (OAVs), and GC-IMS. GC-MS data indicated that SD was favorable to preserve terpenic alcohols (linalool, α-terpineol and terpinene-4-ol), β-cymene, methyl methanthranilate, and monoterpenes; while AD was favorable to preserve aliphatic aldehydes and sesquiterpenes; and SD was more similar with AD in GC-MS analysis of volatile profile (of higher MW) for both cultivars from the PCA outcome. Furthermore, significant difference in volatile isomeric composition of different samples was also clearly demonstrated through extracted ion chromatogram (EIC) by GC-MS analysis. GC-IMS analysis showed the favorability of FD to preserve ketones, phenols, esters, and aromatic aldehydes; and SD was more similar with FD in GC-IMS analysis of volatile profile (of smaller MW) for both cultivars from the PCA outcome. Moreover, the OAVs indicate that 2-methoxy-4-vinylphenol contributed much to the flavor of dried Ponkan peel, while 2-methoxy-4-vinylphenol, methyl methanthranilate, and methyl anthranilate played an important role in the flavor of dried Chachi peel; and the highest OAVs for monoterpenes were observed at SD for both cultivars. Thus, the combination of GC-MS and GC-IMS analyses with PCA in this paper suggested the superiority of SD to preserve volatiles and characteristic aroma in dried citrus peel, and that SD contributed much to the quality of dried Chachi peel.Keywords:citrus peel;volatile compounds;sun-drying (SD);hot-air-drying (AD);freeze-drying (FD);GC-MS;GC-IMS
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PubMed
高影响因子
ACS Nano
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2022
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IF 18.027
Kuncan Wang,Shangheng Liu,Juntao Zhang,Zhiwei Hu,Qingyu Kong,Yong Xu,Xiaoqing Huang
Carbon nanocages (CNCs) have attracted tremendous interest in heterogeneous catalysis due to their promising properties of porous structure and improved mass transfer. Nevertheless, the controlled synthesis of CNCs remains a great challenge. Herein, we have shown the successful construction of functionalized N-doped CNCs (NCNCs) via a one-stone-two-birds strategy. The selective use of hexacarbonyl molybdenum (Mo(CO)6) can not only protect the profile of the ZIF-8 precursor from collapse during thermal treatment but also be sacrificed for the functionalization of NCNCs after pyrolysis. Detailed mechanism studies reveal that Mo(CO)6 evolves into MoO3 on the surface of ZIF-8 and then facilitates the rapid pyrolysis of ZIF-8, leading to the formation of NCNCs decorated with small-sized MoC nanoparticles (MoC/NCNCs). The versatility of this one-stone-two-birds strategy has been validated by the generations of Cr- and W-decorated NCNCs. Moreover, MoC/NCNCs can serve as a selective and stable catalyst for furfural hydrogenation. This work provides a facile and universal strategy for fabricating and functionalizing CNCs, which attracts research interest in the fields of chemistry, material science, catalysis, and beyond.
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PubMed
高影响因子
FUEL
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2022
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IF 8.035
Lungang Chen,Yong Liu,Xinghua Zhang,Jianguo Liu,Qi Zhang,Longlong Ma
Catalytic conversion of biomass to liquid fuel is one of critical part to ease dependence on fossil fuel. Herein, a route of transformation of biomass-derived furfural and levulinic acid into long-chain hydrocarbon fuels was developed. A C20 oxygenate with 95 % mol yield was firstly synthesized through condensation-polymerization reactions catalyzed by NaOH. Various techniques were employed to verify the chemical structure of the C20 oxygenate. The condensation mixture was then directly subjected to hydrodeoxygenation reaction to prepare long-chain hydrocarbons with a catalytic system of Pd/C and H 3 PO 4 in aqueous phase. A 57.1 % weight yield of liquid fuel was obtained with main products of C12, C14, and C18 hydrocarbons. The mass percent of carbon and hydrogen in fuel was significant improved to 95.91 %, as well as the high heat value was increased to 47.04 MJ/kg.
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高影响因子
Journal of Cleaner Production
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2022
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IF 11.072
Dong Feng,Ao Xia,Shuai Wu,Yun Huang,Xianqing Zhu,Xun Zhu,Balakrishnan Deepanraj,Pau-Loke Show,Qiang Liao
Conductive materials may boost the anaerobic digestion of thermal pretreated biomass by overcoming the inhibition effect from by-products generated during the thermochemical pretreatments . The purpose of this study was to explore the influence of magnetite on the anaerobic digestion of furfural, which is found in most biomass hydrolysates . When adding 10 g/l magnetite , the methane yield was enhanced by 125% in comparison to the control. Cyclic voltammetry analysis suggested that the electroactive aggregates were formed after magnetite was added. The microbial community results showed that the Sedimentibacter was significantly enriched (0.2%–18.8%) in the magnetite addition trails; meanwhile, the relative abundance of Methanosaeta was increased by 22.9% compared with the control. Magnetite-amended group of 10 g/l had the lowest hydrogenotrophic methanogens abundance (5.6%) but the highest electrotrophic methanogens abundance (85.3%) than other groups. The energy production efficiency in 10 g/l magnetite addition was 2.3 times higher than that of the control. These evidences indicated that the direct interspecies electron transfer pathway in furfural digestion may be established between Sedimentibacter and Methanosaeta in the presence of magnetite.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2022
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IF 6.437
Linlin Yi,Hong Yao,Xian Li,Zhenzhong Hu,Liu Shi,Yangwei Wu
The catalytic pyrolysis is a promising method for obtaining value-added aromatics, especially benzene, toluene and xylene (BTX). For different biomass-based materials, the dual catalyst system composed of CaO-based and ZSM-5-based catalysts showed an obvious selectivity for the BTX production. This study chose CaO derived from organic calcium precursors (Org-CaO) and nano-sized ZSM-5 (NZSM-5), and comprehensively investigated the effects mechanism of biomass components on the formation pathways of BTX via Py-GC/MS. Under the catalysis of NZSM-5, the BTX yields were only 7.8–30%. The BTX yields on Org-CaO/NZSM-5 were as follows: lipid (63.1%) > hemicellulose (55.4%) > cellulose (40.2%) > lignin (21.7%). Typical pyrolysis intermediates were employed to quantitatively reveal the intermediate reactions. Pyrolysis intermediates exhibited low BTX-forming reactivity over NZSM-5. The pre-catalysis of Org-CaO selectively converted part undesired intermediates (fatty acids and furans) into BTX precursors (short-chain olefins and ketones), facilitating the remarkable increase of BTX yield in the subsequent NZSM-5 catalysis process. However, the pre-catalysis of Org-CaO can hardly make the ring opening reaction of lignin-derived phenolic compounds that have very low reactivity on NZSM-5, and thence high-lignin biomass obtained low BTX production during catalytic pyrolysis by Org-CaO/NZSM-5. These findings afforded a new route for increasing the BTX yields by directionally forming BTX precursors or controlling biomass components.
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高影响因子
FUEL
·
2022
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IF 8.035
Yueqing Wang,Hongxing Wang,Junbo Zhang,Hongyan Zheng,Long Huang,Yulei Zhu
Selectively converting fructose into furfural by H-beta catalyst is a very interesting catalytic process. However, it is a challenging task to clearly elucidate the roles of framework Al for selective scission of C C and C O bond. Herein, selective elimination of framework Al atoms is realized. Several detailed investigations showed that the framework Al species located in different sites play important role in furfural formation. The framework Al atoms of pristine H-beta mainly occupied at T1, T2, T5, T6 and T7 sites. These Al species at pore mouth can be removed by citric acid, while the treatment of nitric acid mainly eliminated the framework Al atoms from T2 and T7 sites. As for oxalic acid, the Al atoms occupied at T2, T5, T6 and T7 was primarily leached. Upon citric acid and nitric acid treatment afforded the similar yield of furfural, indicating that the formation of furfural could not be governed by these Al species at pore mouth, T2 and T7 sites. However, in the case of oxalic acid treatment, complete removal of the Al species on T2, T5, T6 and T7 sites decreased the yield of furfural. Thus, it is reasonably inferred that these Al atoms populated at T1 sites and intersecting channels is more encouraging for the splitting of C C bond, while the Al species occupied at T5, T6 sites and the larger straight channels is probably more favorable to scission of C O bond.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2022
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IF 5.723
Qin Wang,Dan Luo,Jiansu Ran,Jie Zheng,Yuntong Cui,Ruixue Yangcheng,Shuang Luo,Jianjian Wang
It is highly desirable but of challenge to develop an efficient process for lactic acid (LaA) production from xylose performed in water. Herein, a novel catalyst prepared via a facile solvent-free coordination route is developed to efficiently produce LaA from xylose in water. The structural properties of the prepared catalyst and the reaction conditions are systematically investigated. The production rate of LaA at 190 °C in water is up to 1.8 h −1 , outperforming the most recent reports (below 1.1 h −1 ). Detailed experimental and characteristic studies reveal that the presence of Lewis acidic sites and basic sites in the catalyst structure can not only lower the energy barrier of xylose conversion but also boost the efficient conversion of the active reaction intermediates into LaA. The findings of this work will provide a new approach for the efficient production of LaA from carbohydrates.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yuchao Shao,Menggang Bao,Weizhong Huo,Rong Ye,Muhammad Ajmal,Wenjing Lu
Acid hydrothermal treatment of biowaste is favorable for producing hydrochar and corresponding hydrothermal solution containing saccharides, furans and aromatic compounds, while the alkaline hydrothermal condition is beneficial for their humification to form hydrothermal humic acid (HHA). Herein, the humification potential of hydrochar, hydrothermal solution, and their mixture under alkaline hydrothermal conditions was compared to further reveal their contribution to HHA. The result showed the main source of HHA was hydrochar, occupying 70 wt% of total HHA yield from their mixture while hydrothermal solution only contributed 17 wt%. Moreover, the HHA that existed in hydrochar (denoted as HHA acid ) was 32 wt% while the hydrochar-derived HHA obtained after alkaline hydrothermal treatment (denoted as HHA alk ) increased to 65 wt%, close to that from commercial coal or lignite. The hydrochar was further separated into four components, i.e. hydrothermal fulvic acid (HFA), stable HHA acid (S-HHA acid ) non-stable HHA acid ( N -HHA acid ) and remaining substance (RS), aiming to reveal the major pathway of the incremental HHA production under alkaline hydrothermal condition. Reactions of RS + HFA, RS + N -HHA acid and self-synthesizing of RS all contributed to the incremental HHA alk yield with the major contribution (75C%) from the first combination (RS + HFA). The pathways of alkaline hydrothermal humification of hydrochar were revealed after analyzing the molecular level structure of HHA alk by UPLC-MS. This in-depth analysis fills the knowledge gap in the mechanism of hydrothermal humification of biowaste.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Shuibo Wang,Chunzheng Wu,Hongbo Yu,Yuting Chu,Shiwei Wang,Tong Li,Hongfeng Yin
Tailoring the interface between active metals and promoters to improve catalytic performance is a challenging issue for bicomponent catalysts. Herein, we developed a series of silica supported Pt-CoO x hybrid nanocatalysts though in situ oxidation of supported bimetallic PtCo nanoparticles (NPs) with different Pt/Co ratios. Focusing on the hydrogenation of acetophenone to 1-phenylethanol as the model reaction, the obtained Pt-CoO x /SiO 2 catalysts showed superior activity and selectivity compared to Pt/SiO 2 , and the sample with a Co/Pt molar ratio of 1/3 performed the best. Our research showed that the CoO x on Pt not only changed its electronic and geometric properties, but also promoted the adsorption of reactants and the dissociation of H 2 . A further increase of the Co/Pt ratio to 1/1, however, reduced the activity due to blockage of the Pt surface.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yang Peng,Zhanwei Xu,Le Yu,Xucheng Li,Weiran Yang
The direct conversion of furfural (FUR) to 2-methyltetrahydrofuran (2-MTHF) was investigated over a trimetallic CuNiRe/Hβ catalyst. Under optimal reaction conditions at 240 °C under 3 MPa H 2 for 1 h, almost complete conversion of FUR and high-yield of 2-MTHF (81 %) was achieved. This is the highest yield reported for the direct conversion of FUR to 2-MTHF. HR-TEM demonstrated that the growth of Cu nanoparticles (NPs) on the surface of Hβ was inhibited after loading Ni or Re resulted in the smaller Cu particle size and better hydrogenation and hydrodeoxygenation activity. H 2 -TPR characterization exhibited that the reducibility of bimetallic and trimetallic catalysts was higher than that of monometallic catalysts·NH 3 -TPD explained that Hβ acid sites mainly contributed to FUR deoxygenation. The adsorption configurations of FUR, furfuryl alcohol (FOL) and 2-methylfuran (2-MF) on the catalyst were revealed by ATR-IR. Catalyst evaluation and control experiments proved that FUR was first hydrogenated to FOL, followed by hydrodeoxygenation to 2-MF, and finally hydrogenated to 2-MTHF catalyzed by the combination of three metals.
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