Molecular Catalysis
·
2022
·
IF 5.089
Wenpeng Han,Shujuan Wang,Yajie Liu,Chaoqun Li,Ningning Yuan,Ligong Zhou,Mingxing Tang,Hui Ge
The transformation of biomass to liquid fuels and chemicals is of great interests. Herein, a series of reduced NiZn-CT (CT represents calcination temperature) catalysts with flower-like morphology and uniform particle sizes were prepared by co-precipitation method and used for hydrogenolysis of 5-hydroxymethylfural (HMF) to 2,5-dimethyfuran (DMF). The characterizations evidenced the formation of NiZn alloy phase in the catalysts through the strong metal-support interaction (SMSI), which had high C-O hydrogenolysis ability. The synergy of hydrogenation and C-O hydrogenolysis is essential for HMF to DMF, and we surprisingly found that this synergistic effect can be achieved just by controlling calcination temperature to regulated SMSI between Ni and ZnO. By this way, 99% DMF yield was gained at 180 °C for 4 h under 2 MPa H 2 over reduced NiZn-450 catalyst. More importantly, the active centers of this Ni/ZnO catalyst exhibited outstanding stability. There was no significant decrease in activity after reusing 9 times. The current research provided an easy-made catalytic system for HMF hydrogenolysis.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 101
·期 6
·3234-3245
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IF 2.5
Luxin Zhang,Meng Hu,Ruijun Sun,Xu Xing
The production of 5-ethoxymethylfurfural (EMF) from cheap and abundant glucose feedstock has attracted a great deal of attention because of its potential applications. Herein, three porous tetra-component metal oxide solid acid catalysts (SO 4 2− /ZFSA-A, SO 4 2− /ZFSA-F-10, SO 4 2− /ZFSA-F-20) containing both Brønsted and Lewis acid sites have been successfully synthesized and can efficiently catalyze the synthesis of EMF from glucose. Particularly, the SO 4 2− /ZFSA-A, SO 4 2− /ZFSA-F-10, and SO 4 2− /ZFSA-F-20 catalysts were prepared under the template of sodium alginate, 10% F127, and 20% F127, respectively. The prepared catalysts were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), N 2 -adsorption–desorption isotherm, X-ray photoelectron spectroscopy (XPS), thermogravimetry (TG), temperature-programmed desorption of ammonia (NH 3 -TPD), and pyridine infrared spectra (Py-FTIR). The characterization results indicated that all three catalysts have a porous structure. The pore distribution of the SO 4 2− /ZFSA-A catalyst is mainly macroporous and mesoporous, while the SO 4 2− /ZFSA-F-10 and SO 4 2− /ZFSA-F-20 catalysts are mainly mesoporous. The SO 4 2− /ZFSA-F-20 catalyst exhibited the highest catalytic performance due to its large specific surface area, desirable mesoporous structure, high total acidity (especially strong and super strong acidity), and appropriate Lewis/Brønsted acid ratio. By applying SO 4 2− /ZFSA-F-20, the formation of EMF from glucose was successfully catalyzed and EMF was obtained at a yield of 34.56% after 12 h at 160°C. This yield is much higher compared with most other results achieved by solid acids catalysis. In addition, the reaction parameters such as reaction temperature, reaction time, glucose amount, and catalyst dosage were shown to have a significant effect on the catalytic performance. Notably, the SO 4 2− /ZFSA-F-20 catalyst exhibited good reusability, as its activity did not significantly diminish after four rounds of repeated experiments and was successfully reactivated after calcination.
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GREEN CHEMISTRY
·
2021
·Vol. 24
·期 2
·877-884
·
IF 10.182
Baolong Zhang,Hui Fu,Tiancheng Mu
Electrochemical oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) has drawn wide attention recently. Rational interface engineering can modulate the electronic structure, tune the adsorption energy and endow the hybrid material with more active sites for HMF electrochemical oxidation. Herein, we propose a strategy for the synthesis of metal sulfide/metal phosphide (MSx/MPy, M = Co, Fe, Ni…) nanotube arrays with abundant interfaces by the sequential electrodeposition interface engineering method. Since Ni-based electrocatalysts show high efficiency for the electrochemical oxidation of HMF, we designed and synthesized interface-rich heterogeneous NiSx/Ni2P nanotube arrays. The abundant interfaces promote electron transfer between NiSx and Ni2P, which synergistically improves the oxidation state of the Ni species and further enhances the electrocatalytic performance of HMF oxidation. The NiSx/Ni2P electrocatalyst shows superb HMF oxidation activities with a low onset potential of 1.25 V vs. RHE. A current density of 20 mA cm−2 can be reached at 1.346 V vs. RHE, which is reduced by 204 mV compared with that with water oxidation. Chronoamperometry electrolysis reveals that HMF conversion is nearly 100% and FDCA selectivity can reach 98.5%.
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FUEL
·
2021
·
IF 6.609
Mingquan Li,Aqsa Noreen,Yajie Fu,Cederick Cyril Amoo,Yujia Jiang,Xu Sun,Peng Lu,Ruiqin Yang,Chuang Xing,Shurong Wang
Directly synthesizing olefins from syngas using metal-zeolite composite catalysts has engrossed a lot of attention recently. Fe-based catalysts will be the most promising industrial candidates due to cost and availability constraints. In this work, we investigate the characteristics and Fischer-Tropsch activity of a novel Fe@Na-ZSM-5 composite for one-step conversion of syngas to higher olefins (C 5+ ). The in-situ crystallization mechanism induced Na in the ZSM-5 as a Fe-based promoter which realized 52.5 % selectivity for gasoline of which ∼ 70% were olefins. Additionally, the promotion by the Na ions enhanced the formation of Fe 5 C 2 phases which in turn favored C–C coupling, high gasoline and olefins selectivity. Na type zeolite (Na-Zeolite) offers a novel Na electron promoter, which participate immensely in the development of heterogenous catalyst and functional materials.
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JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Qiyuan Wu,Shi Zhang,Xingtao Zuo,Lanxingyu Liu,Juan Xiong,Jiajie He,Yun Zhou,Cong Ma,Zhongbing Chen,Shuili Yu
Nanofiltration with high stable permeance is of great significance for wastewater treatment . Herein, we reported the novel polyamide thin-film composite (PA TFC) nanofiltration membranes prepared for the first time by blending nanometer cerium doped high silica ZSM-5 zeolites (CeO 2 @HSZSM-5, CHZ) in the aqueous phase followed by the classic interfacial polycondensation . The structural morphology of these membranes and their performance had been characterized. SEM and XPS characterizations clearly revealed the presence of inorganic CHZ in the PA layer. The results also showed that the CHZ-integrated inorganic-organic PA TFC membranes with a higher fraction of CHZ had a thinner PA active layer (28.3 ± 3.6 nm) and slightly enlarged pore size with lower crosslinking degree. The optimized membranes exhibited 1.65-folds pure water permeability of the traditional membrane, 20.3 L/(m 2. h . bar) with comparable Na 2 SO 4 and MgSO 4 rejection of 95.8% and 91.1%, respectively. The rejection of dyes stayed stable above 96.0% with boosted permeance, and the membrane almost completely removed CR and RB as well as natural organic matters. The composite membrane also sustained superior stability and excellent antifouling performance. The as-prepared CHZ-integrated PA TFC membranes with regulatable structural morphology and superior separation properties enables the potential practical application in wastewater treatment.
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ChemSusChem
·
2021
·Vol. 15
·期 13
·e202101889
·
IF 8.928
Miao Zuo,Xinyu Wang,Qian Wang,Xianhai Zeng,Lu Lin
Graphical HMF synthesis in NADES : High yield of 5-hydroxymethylfurfural (HMF) is obtained in a cheap and green natural deep eutectic solvent (NADES) system with a low amount of SnCl 4 catalyst from different biomass materials, including glucose, starch, and food wastes. The addition of water obviously improves the reactivity and economy of the NADES mixture. This is a green and efficient method to utilize carbohydrate resources for HMF production in a robust solvent system. 5-Hydroxymethylfurfural (HMF) has been regarded as an essential building block for synthesizing chemicals and biofuels, but the direct conversion of biomass to HMF is still a critical challenge. In this study, a cheap and green aqueous-natural deep eutectic solvent (A-NADES) was used to efficiently produce HMF from various carbohydrates, with a low amount of SnCl 4 as the catalyst. High HMF yields of 64.3, 64.0, 61.3, and 54.5 % were obtained from glucose, starch, rice waste, and bread waste at 130 °C in the A-NADES/MIBK (methyl isobutyl ketone) biphasic system, respectively. Mechanistic study results revealed that the water in A-NADES was the key factor in facilitating the conversion of Sn atom existent forms and promoted the HMF production. The choline chloride in NADES stabilized the HMF product with the cooperation of extraction solvent MIBK and inhibited the side reactions of HMF. This study investigated the multiple interaction functions of A-NADES to feedstocks and proposed a practical application of novel solvents to facilitate biomass and food waste conversion with a green method.
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Molecular Catalysis
·
2021
·
IF 5.062
Kequan Chen,Chaoqiang Wu,Chengyong Wang,Alei Zhang,Fei Cao,Pingkai Ouyang
In this study, efficient production of the platform chemical 3-acetamido-5-acetylfuran (3A5AF) from chitin resources via a chemo-enzymatic protocol was investigated. Initially, chitinolytic enzyme was used to convert chitin into N -acetyl glucosamine (GlcNAc) using an affinity adsorption–enzymatic reaction integrated approach. Then, the obtained GlcNAc was used to produce 3A5AF using screened ammonium thiocyanate (NH 4 SCN) as the catalyst. The optimal conditions for converting GlcNAc into 3A5AF were determined at a temperature of 180 °C, solvent of DMAc, a molar ratio of GlcNAc to NH 4 SCN of 2:1, addition of CaCl 2 ·2H 2 O, a molar ratio of GlcNAc to CaCl 2 ·2H 2 O of 1:1 and a reaction time of 10 min, resulting in 3A5AF with a molar yield of 56.66%. The NH 4 SCN showed good recyclability within five cycles. Furthermore, upon scaling up of the 3A5AF preparation, a good yield was still maintained. Additionally, 99% pure 3A5AF needle-shaped crystals were obtained with 34 wt% yield by crystallisation purification. This new chemo-enzymatic protocol provides a good option to convert chitin resources into 3A5AF.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Mengke Liu,Peng Li,Haitang Yang,Nan Jiang,Dingzhong Wang,Shihao Sun,Wei Wei
5-hydroxymethylfurfural (HMF) is one of the food contaminants mainly formed by Maillard and caramelization reaction. Here, we developed a simple method to detect HMF based on split-DNAzyme assisted signal amplification via Quartz crystal microbalance . Firstly, two fragments of the split-DNAzyme (ESΙ and ESII) and AuNPs-ssDNA were prepared. In the absence of HMF, the amino group of ESΙ reacted with the aldehyde group of ESΙΙ by Schiff base condensation，which linked ESΙ and ESII as DNAzyme. With the help of Mg 2+ , this DNAzyme cleaved AuNPs-ssDNA, freeing the complementary sequence of capture DNA from the ssDNA. In the presence of the target HMF, the aldehyde group in its molecular structure preferred to react with ESΙ, which prevented the link of ESΙ and ESII. In this case, DNAzyme cannot be formed effectively and the ssDNA modified on AuNPs cannot be cleaved. Secondly, the capture DNA was immobilized on Au chip in the QCM chamber. Then, the intact AuNPs-ssDNA was introduced to hybridize with the capture DNA, resulted in a large frequency change (ΔF) of the QCM biosensor because of the huge increased mass of AuNPs. So, HMF can be detected based on the frequency change (ΔF) of the QCM biosensor. This QCM biosensor is more sensitive than previously reported methods, which provide a new direction for the analytical detection of HMF and other food contaminants.
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FUEL
·
2021
·
IF 6.609
Mingjie Liao,Xin Ning,Junwen Chen,Jiajun Zheng,Wenlin Li,Ruifeng Li
Zeolite is one kind of the solid acid catalysts for the oligomerization process but surfers from rapid deactivation. In this specific study, a series of mesoporous ZSM-5 catalysts have been synthesized and evaluated in the 1-hexene oligomerization. XRD, BET, SEM, TEM, 27 Al MAS NMR, 29 Si MAS NMR, NH 3 -TPD, Py-FTIR and TGA analysis were used to characterize the physicochemical properties of zeolites. The synthesized mesoporous zeolites were found to be more stable in the reaction and the initial activity increase significantly compared with the common ZSM-5 zeolite . Moreover, the catalytic activity of mesoporous ZSM-5 zeolite is found to be closely related to the number and the distribution of acid sites. The mesoporous ZSM-5 zeolites with the lower amount of acid sites, moderate strength of Brønsted acid sites inhibiting the cracking and coke products. High L/B ratio enhanced the dimers formation. The efficiency was further highlighted by a high space–time yield (STY) of 557 mg·g cat −1 h −1 in the average stage at 260 °C. Compared to conventional ZSM-5 catalyst, the synthesized catalyst displayed excellent resistance to coke deposit.
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ENZYME AND MICROBIAL TECHNOLOGY
·
2021
·
IF 3.493
Rong Wang,Xinqi Xu,Xuemei Yao,Hengtao Tang,Xin Ju,Liangzhi Li
Ribose-5-phosphate isomerase A (RpiA) is of great importance in biochemistry research, however its application in biotechnology has not been fully explored. In this study the activity of RpiA from Ochrobactrum sp. CSL1 (OsRpiA) towards D-allose was engineered based on sequential and structural analyses. Strategies of alanine scanning, rational design and saturated mutagenesis were employed to create three mutant libraries. A single mutant of K124A showed a 45 % activity improvement towards D-allose. The reaction properties of the mutant were analyzed, and a shift of optimal pH and higher thermal stability at low reaction temperatures were identified. The conversion of D-allose was also improved by 40 % using K124A, and higher activities on major substrates were found in the mutant’s substrate scope, implying its application potential in rare sugar preparation. Kinetics analysis revealed that K m of K124A mutant decreased by 12 % and the catalytic efficiency increased by 65 % towards D-allose. Moreover, molecular dynamics simulation illustrated the binding of substrate and K124A was more stable than that of the wild-type. The shorter distance and more relax bond angle between the catalytic residue of K124A and D-allose explained the activity improvement in detail. This study highlights the potential of OsRpiA as a biocatalyst for rare sugar preparation, and provides distinct evidences for its catalytic mechanism.
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高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 31
·10922-10927
·
IF 4.39
Wei Wang,Fanhao Kong,Zhe Zhang,Lan Yang,Min Wang
Electrochemical oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is an intriguing way of biomass conversion. Herein, a sulfidation of nickel foam (Ni2S3/NF) was attempted via a hydrothermal method, achieving high selectivity and efficiency for HMF oxidation. The optimized Ni2S3/NF electrode exhibits a nearly 100% conversion of HMF, 98% yield of FDCA, and 94% high faradaic efficiency. This material is stable and retains activity after 6 consecutive measurements. This work provides a facile route to design and prepare electrocatalysts for biomass upgrading.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Weiqi Wei,Gaojing Lyu,Weikun Jiang,Zhengyu Chen,Shubin Wu
In this work, a sulfonic acid-functionalized magnetic separable solid acid (Fe 3 O 4 @SiO 2 -SO 3 H) was synthesized, characterized, and tested for fructose conversion to 5-hydroxymethylfurfural (HMF). Results indicated that the prepared catalyst had a good efficacy for fructose dehydration to HMF due to its larger specific surface area, appropriate acid amount and homogeneous acid distribution. The maximum HMF yield of this work was 96.1 mol%. It was obtained at 120 °C for 1.5 h with 100 mol% fructose conversion. More importantly, the produced HMF could be further in-situ oxidized into 2,5-diformylfuran (DFF) after the replacing of the Fe 3 O 4 @SiO 2 -SO 3 H with a ZnFeRuO 4 catalyst, and the highest DFF yield of 90.2 mol% (based on initial fructose) was obtained after reaction another 8.5 h. The production of DFF from fructose through the above two consecutive steps avoids the intermediate HMF separation, which saves time and energy. In addition, both Fe 3 O 4 @SiO 2 -SO 3 H and ZnFeRuO 4 catalysts exhibited satisfied stability in the recycling experiments, which can be reused at least for five times with the HMF and DFF yield loss<5.3% and 3.3%, respectively. Finally, the plausible reaction mechanisms for fructose conversion to HMF or DFF over Fe 3 O 4 @SiO 2 -SO 3 H or/and ZnFeRuO 4 catalysts were also proposed in this work.
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