Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Putrakumar Balla,Prem Kumar Seelam,Ravi Balaga,Rajendiren Rajesh,Vijayanand Perupogu,Tong Xiang Liang
Sustainable catalysis is the key for the future progress toward biorefinery and bioeconomy. In this work, we designed and developed an inexpensive and eco-friendly Ni@C catalyst for selective hydrogenation of biomass-based platform molecules. A facile synthesized Ni nanoparticles encapsulated in a stabilized carbon support derived from a sacrificial agent copolymer-gel was investigated in the hydrogenation of furfural (FA) to tetrahydrofurfuryl alcohol (THFOL) and levulinic acid (LA) to γ-valeralactone (GVL). The aim is to study the two different reactions over a highly stabilized Ni nanoparticles embedded in the carbon matrix. The Ni@C was found to be active and selective in multi-catalyzed hydrogenation reactions. The Ni nanoparticles with small and ultra-fine sizes are highly dispersed over the carbon matrix. This was concluded through high-resolution micrography images (SEM, TEM) and XRD patterns. In both reactions, a complete conversion of furfural and levulinic acid was achieved with maximum selectivity over the Ni@C catalyst. The effect of reaction temperature, solvent type, reaction time, and H 2 pressure were also studied. Overall, optimized reaction conditions were determined, and the Ni@C is easily reusable and exceptionally durable in the studied reaction cycles. The apparent activation energies for FA hydrogenation to THFOL and LA hydrogenation to GVL are 15.4 kJ/mol and 33.6 kJ/mol, respectively.
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JOURNAL OF RARE EARTHS
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2021
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IF 3.712
Xianghua He,Ben Dai,Yafang Zhang,Dan Zhao,Dihui Zhang,Ruping Liang,Chao Chen
Efficient and applicable catalysts are highly desirable for advanced biomass transformation industry, here, we fabricated a series of Nd-Co-P catalysts for hydrogenation of furfural (FAL) to furfuryl alcohol (FOH). By comprehensive characterizations, it is demonstrated that the prepared Nd-Co-P samples are structured as (NdPO 4 ) m /Co 2 P nanocomposites with molar ratio ( m ) in range of 0.24–1.1; by manipulating m , the outstanding catalytic efficiency comparable with the performance of precious metal catalysts , such as turnover frequency (TOF) up to 0.50 s −1 (being ten-fold higher than Co 2 P) and FOH yield up to 97%, is achieved on the reusable (NdPO 4 ) m /Co 2 P composites. Temperature programmed desorption (TPD), in-situ infrared spectroscopy (IR) and kinetic-mechanism studies further disclose that Co 2 P is decisive for activating FAL, instead, NdPO 4 possesses unique capability of activating hydrogen which readily facilitate the selective hydrogenation of FAL to FOH through a rapid Langmuir–Hinshelwood process over (NdPO 4 ) m /Co 2 P catalyst. These results indicate that rare-earth phosphates like NdPO 4 can act as the promising and reliable catalytic component to activate hydrogen, which can be of interest not only for innovating novel and applicable non-metallic catalysts for sustainable biomass transformation analogous to hydrogenation of FAL, but also for expanding material base for other green mass transformation techniques involving hydrogen.
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GREEN CHEMISTRY
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2019
·Vol. 21
·期 14
·3911-3919
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IF 9.405
Yanlong Qi,Shijun Liu,Long Cui,Quanquan Dai,Jianyun He,Wei Dong,Chenxi Bai
The synthesis of functionalized 1,3-dienes has received increasing attention due to their importance in the practical development of high-performance elastomers. In the present work, furfural and acetone, acting as renewable feedstocks, are first employed to produce a functionalized 1,3-diene containing a furan group (1-(2-furyl)-1,3-butadiene, F-diene). After selective hydrogenation of the CO group, the aldol adduct (4-(2-furanyl)-3-buten-2-ol, FAH) shows a nearly complete conversion, with an excellent selectivity (as high as 92%) towards F-diene over ceria-based catalysts in a fixed bed. BET, TEM, XRD, XPS, Raman, TPD, TPR and TGA were conducted to identify the relationship between the catalytic performance and catalyst structure. A plausible reaction pathway for the dehydration of FAH over ceria-based catalysts was proposed using a radical mechanism, which suggested the importance of the Ce4+–Ce3+ redox cycle for the dehydration of FAH to F-diene. Furthermore, the ceria-based catalysts exhibited a notable carbon resistance.
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ACS Sustainable Chemistry & Engineering
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2018
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IF 6.14
Wanbing Gong,Chun Chen,Haimin Zhang,Guozhong Wang,Huijun Zhao
Herein, we report that highly dispersed copper–cobalt mixed metal/metal oxide nanoparticles embedded into three-dimensional porous carbon were highly catalytic active nanocomposites for transforming bioderived furfural (FAL) to cyclopentanone (CPO) via aqueous-phase hydrogenation/rearrangement. This simple and efficient catalyst was prepared by controlled pyrolysis procedure using glucose as the carbon source at 500 °C under N2 atmosphere. Characterization of the as-prepared CuCo0.8@C-500 catalyst by XRD, STEM, SEM, TEM, and XPS suggested that there was a synergism between copper and cobalt. Under an extremely low H2 pressure (0.5 MPa), 90.2% yield of CPO could be attained at 150 °C. In addition, the sample could be recycled for several times without decrease in catalytic activity. Two critical reaction intermediates of furfuryl alcohol (FOL) and 2-cyclopentenone (2-CPE) were detected in the tandem catalytic process. These results demonstrated that this synthetic strategy represented a simple and effective way for utilization of inexpensive biomass resources to obtain some valuable chemicals.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2014
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IF 2.235
Yimei Wang,Bing Liu,Kecheng Huang,Zehui Zhang
The paper deals with oxidation of the biomass-derived model molecule 5-(hydroxymethyl)furfural (HMF) catalyzed by the trimetallic mixed oxide RuCo(OH)2CeO2. The catalyst RuCo(OH)2CeO2 was prepared through alkali hydrolysis of RuCl3, Co(NO3)2, and Ce(NO3)2 and characterized by X-ray diffraction and transmission electron microscopy techniques. RuCo(OH)2CeO2 showed high catalytic activity for aerobic oxidation of HMF under mild conditions (in the case of atmospheric oxygen pressure). Various reaction parameters such as the reaction temperature, catalyst amount, solvent, and oxidant were explored. Results demonstrated that the oxidant and solvent showed a remarkable effect on the aerobic oxidation of HMF to 2,5-diformylfuran (DFF). Under optimal conditions, DFF was obtained in a high yield of 82.6% with HMF conversion of 96.5% after 12 h at 120 °C. More importantly, the catalyst could be reused several times without significant loss of its catalytic activity.
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GREEN CHEMISTRY
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2015
·Vol. 17
·期 6
·3644-3652
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IF 8.02
Shanshan Li,Ning Li,Guangyi Li,Lin Li,Aiqin Wang,Yu Cong,Xiaodong Wang,Tao Zhang
Protonated phenol-formaldehyde condensation products of sodium lignosulfonate and lignocellulose derived aldehydes were first reported as cost-effective catalysts for the hydroxyalkylation/alkylation (HAA) of 2-methylfuran and furfural. Among them, the LF resin which was prepared with sodium lignosulfonate and formaldehyde exhibited the best performance. With the LF resin, higher activity, catalytic efficiency and stability than those of Amberlyst resins were observed, which can be rationalized by its higher acidic strength. The HAA product of 2-methylfuran and furfural was further converted to diesel and jet fuel range alkanes by the solvent-free hydrodeoxygenation (HDO) over the Ni/H-ZSM-5 catalysts prepared by conventional or complexation impregnation methods. It was found that the presence of complex agents can promote the dispersion of Ni, which leads to the higher HDO activity of Ni/H-ZSM-5 catalysts.
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MOLECULES
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2024
·Vol. 29
·期 12
·2753
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IF 4.2
Yongzhen Gao,Wenjing Yi,Jingyi Yang,Kai Jiang,Tao Yang,Zhihan Li,Meng Zhang,Zhongyi Liu,Benlai Wu
The selective hydrogenation of the biomass platform molecule furfural (FAL) to produce furfuryl alcohol (FA) is of great significance to alleviate the energy crisis. Cu-based catalysts are the most commonly used catalysts, and their catalytic performance can be optimized by changing the preparation method. This paper emphasized the effect of calcination atmosphere on the performance of a Cu/Al2O3catalyst for the selective hydrogenation of FAL. The precursor of the Cu/Al2O3catalyst prepared by the ammonia evaporation method was treated with different calcination atmospheres (N2and air). On the basis of the combined results from the characterizations using in situ XRD, TEM, N2O titration, H2-TPR and XPS, the Cu/Al2O3catalyst calcined in the N2atmosphere was more favorable for the dispersion and reduction of Cu species and the reduction process could produce more Cu+and Cu0species, which facilitated the selective hydrogenation of FAL to FA. The experimental results showed that the N2calcination atmosphere improved the FAL conversion and FA selectivity, and the FAL conversion was further increased after reduction. Cu/Al2O3-N2-R exhibited the outstanding performance, with a high yield of 99.9% of FA after 2 h at 120 °C and an H2pressure of 1 MPa. This work provides a simple, efficient and economic method to improve the C=O hydrogenation performance of Cu-based catalysts.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
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IF 5.7
Tong Zhou,Meigui Huang,Heping Cui,Pusen Chen,Khizar Hayat,Xiaoming Zhang,Chi-Tang Ho
The involvement of exogenous alanine was observed to inhibit the generation of 2-furfural during the thermal degradation of the Amadori rearrangement product (ARP). To clarify the reason for the reduced yield of 2-furfural triggered by exogenous alanine, the evolution of the precursors of 2-furfural formed in the ARP model and ARP-alanine model was investigated, and a model including ARP and 15N-labeled alanine was used to differentiate the role of endogenous and exogenous alanine in the degradation of ARP. It was found that the condensation between ARP and 3-deoxyxylosone could occur during thermal treatment. Nevertheless, the interaction of ARP with 3-deoxyxylosone exhibited an accelerated pace in the presence of exogenous alanine. In this way, exogenous alanine blocked the recovery of endogenous alanine while simultaneously enhancing the consumption of ARP and 3-deoxyxylosone during the Maillard reaction. Hence, the yield of 2-furfural was diminished with the interference of exogenous alanine. Furthermore, the promotion of the reaction between ARP and deoxyxylosone induced by exogenous alanine blocked their retro-aldolization reaction to short-chain α-dicarbonyls (α-DCs) and consequently resulted in a lack of pyrazine formation during the ARP degradation. The present study provided a feasible method for the controlled formation of 2-furfural during the thermal treatment of ARP derived from alanine.
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JOURNAL OF POWER SOURCES
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2024
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IF 8.1
Jia Cheng,Zhiwei Zeng,Xun Huang,Zidong Wei
The electrocatalytic oxidation of furfural (FA) for the production of valuable chemicals, such as 2-furancarboxylic acid (FAC), presents an attractive alternative to the sluggish oxygen evolution reaction during water electrolysis for hydrogen production. However, the activity and stability of the current electrocatalysts still require further enhancement. In this study, NiMoP is fabricated on Ni foam through pulsed electrodeposition to facilitate the electrooxidation of FA for FAC production in an alkaline environment. A low voltage of 1.43 V vs. reversible hydrogen electrode (RHE) is adequate to achieve a current density of 500 mA cm −2 , with FAC selectivity and Faraday efficiency reaching 97.5 % and 95.2 %, respectively. The extended electrolysis of FA using a continuous-flow electrolytic cell under high current density (500 mA cm −2 ) demonstrates consistent stability at a cell voltage around 1.8 V over a 35-h duration.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
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IF 3.7
Antai Kang,Jiangtao Li,Yubin Li,Min Cao,Li Qiu,Bo Qin,Yanze Du,Feng Yu,Sha Li,Ruifeng Li,Xiaoliang Yan
Bimetallic CuCo catalysts with different Cu to Co ratios on N-doped porous carbon materials (N-C) were achieved using impregnation method and applied in the hydrogenation of furfural (FAL) to furfuryl alcohol (FOL). The high hydrogenation activity of FAL over Cu 1 Co 1 /N-C was originated from the synergistic interactions of Cu and Co species, where Co 0 and Cu 0 simultaneously adsorb and activate H 2 , and Cu + served as Lewis acid sites to activate C═O. Meanwhile, electrons transfer from Cu to Co promoted the formation of Cu + . In situ Fourier transform infrared spectroscopy analysis indicated that Cu 1 Co 1 /N-C adsorbed FAL with a tilted η 1 -(O) configuration. The superior Cu 1 Co 1 /N-C showed excellent adsorbed ability towards H 2 and FAL, but weak adsorption for FOL. Therefore, Cu 1 Co 1 /N-C possessed 93.1% FAL conversion and 99.0% FOL selectivity after 5 h reaction, which also exhibited satisfactory reusability in FAL hydrogenation for five cycles.
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TALANTA
·
2024
·
IF 5.6
Hao-Jie Bai,Hong-Wei Li,Yi Li,Zhijiu Huang,Sha Liu,Xin-He Duan,Yuqing Wu
Detecting the furfural concentration in Baijiu can be used to assess the quality of Baijiu , allowing for the optimization of processing techniques and the enhancement of overall quality. In this paper, a fluorescence-enhanced method based on carbon dots ( o -CDs) is developed for the furfural determination in Chinese Baijiu . In an environment full-filled with · SO 4 ‐ and · OH , furfural undergone a direct surface reaction with the ortho -diamino groups at o -CDs. The created furan-based imidazole increased the surface electron density, leading an emission enhancement and color changes from orange to green. Thereby, a linear fluorescence response of o -CDs-TA to furfural is established in water with a detection limit of 30.5 nM. Finally, after ethanol correction it is used to determine furfural in Chinese Baijiu with high precision and reproducibility, providing a new strategy with low-cost and high sensitivity. In particular, the idea of covalently connecting target molecule to the CDs surface via the assistance of free radical opens a new avenue to merge the nanoscale and molecular realms through implementing chemical role into carbon nanostructures.
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CHEMICAL ENGINEERING JOURNAL
·
2017
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IF 6.216
Hao Chen,Houhang Ruan,Xilei Lu,Jie Fu,Timothy Langrish,Xiuyang Lu
In the present study, an economic and environmentally friendly bi-functional catalyst, Zr-SBA-15, has been prepared to develop a single-step process for synthesis of methyl levulinate (MLA) directly from furfural (FAL) in near-critical methanol without added H 2 . The presence of Zr in SBA-15, the structure of the Zr-SBA-15 catalyst, and its physical properties have been determined by X-ray diffraction (XRD), N 2 adsorption and desorption (N 2 -BET) and transmission electron microscopy (TEM). The Zr-SBA-15 catalyst has high activity for the production of MLA and good reusability. A possible reaction pathway containing two possible reaction pathways during this single-step synthesis of MLA has been proposed: the FAL has been transformed to β-Methoxy-2-furanethanol (MFE) and 2-Furfuryl methyl ether first, which then have been converted to MLA, and the conversion of FAL to MFE has been much easier and faster than that to 2-FME, which may be the major reaction pathway. The SBA-15 has given high activity for the conversion of FAL to MFE, and the incorporation of Zr has converted the MFE to MLA efficiently. The reaction of FAL to MFE to MLA has been found to be the dominant reaction. Finally, the catalyst has shown good reusability for at least five times without any reduction in the catalytic activity.
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