ACS Omega
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2021
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IF 3.512
Lei Hu,Jiayi Zheng,Qing Li,Shunhui Tao,Xiaojie Zheng,Xiaodong Zhang,Yao Liu,Xiaoqing Lin
5-hydroxymethylfurfural (5-HMF) is a promising high value-added platform chemical, which can be produced from glucose, fructose, or lignocellulosic biomass via catalysis technology. However, the effective separation of 5-HMF from aqueous solution and actual biomass hydrolysate is still challenging because 5-HMF can be further rehydrated into levulinic acid (LA) and formic acid (FA) under acidic conditions. Herein, the adsorption behavior of glucose and 5-HMF and its follow-up products (LA and FA) from aqueous solutions onto polymeric adsorbents modified with various functional groups (XAD-4, XAD7HP, and XAD761 resins) was systematically investigated. The results showed that XAD761 resin exhibited the highest adsorption selectivity (α5-HMF/glucose = 42.42 ± 5.84, α5-HMF/FA = 18.41 ± 0.50, and α5-HMF/LA = 3.01 ± 0.10) and capacity for 5-HMF (106 mg g–1 wet resin). The adsorption equilibrium was better fitted by the Freundlich isotherm model at the studied range of 5-HMF concentrations. The thermodynamic study and activation energy also revealed that the adsorption process of XAD761 resin for 5-HMF was spontaneous, exothermic, and physical. The kinetic regression results revealed that the kinetic data of 5-HMF was accurately followed by the pseudo-second-order kinetic model. In conclusion, the present study revealed that the potential of phenol formaldehyde resin with hydroxyl groups could be used as an adsorbent for aldehyde organic compounds.
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FOOD RESEARCH INTERNATIONAL
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2021
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IF 6.475
Jing-Xuan Gao,Yu-Ying Zhang,Xu-Hui Huang,Rong Liu,Xiu-Ping Dong,Bei-Wei Zhu,Lei Qin
As an important aquaculture shellfish, the superior taste and high nutritional value of oyster ( Crassostrea gigas Thunberg) have drawn extensive attention. In this study, twenty-one free amino acids (FAAs) and six 5′-nucleotides were evaluated through stable isotope labeling-liquid chromatography coupled with tandem mass spectrometry (SIL-LC-MS/MS), and the lipid profile was explored using ultrahigh performance liquid chromatography-Q Exactive HF mass spectrometry (UHPLC-QE/MS). The adductor muscle of the oyster possessed a high level of sweetness-related amino acids (Arg, Gly and Hyp) and 5′-nucleotides. A total of 149 lipid species were detected in different tissues of oysters, including 17 triacylglycerols (TAGs), 6 diacylglycerols (DAGs), 61 phosphatidylcholines (PCs), 29 phosphatidylethanolamines (PEs), 11 lysophosphatidylcholines (LPCs), 8 lysophosphatidylethanolamines (LPEs), and 1 lysophosphatidylinositol (LPI). FAAs, 5′-nucleotides and lipid profile in the digestive gland of oysters can be divided into three stages, from November to April, May to July, and August to October. The highest proportion of umami-taste amino acids and 5′-nucleotides appeared from March to May. The highest percentage of high unsaturation degree glyceride and phospholipids appeared in August and April, respectively. Thus, the results reported in this study are important for product development and sustainable exploitation in the future.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Yi Yang,Huiqi Zhu,Xuhui Xu,Lulu Bao,Yinuo Wang,Haowen Lin,Chenyang Zheng
Eutrophication caused by excessive phosphate has become a global environmental issue that urgently needs to be solved due to its destructive effect on the ecosystem and adverse effect on human health. In this study, a novel lanthanum carbonate-grafted ZSM-5 zeolite (LC-ZSM-5) was developed to effectively achieve highly selective phosphate removal from wastewater. The LC-ZSM-5 adsorbent shows high adsorption capacity (highest at over 45 mg-PO 4 3- /g) in the pH range of 3–6 with a fast adsorption rate (reaching 80% of the maximum adsorption capacity within 150 min and equilibrium at 350 min). High stability can be observed with less than 0.3 mg/L La leakage during the adsorption process . Four kinetic models are used to describe the adsorption process. The pseudo second order model and the Elovich model are found to fit the data best with a high correlation coefficient (r 2 = 0.99), showing that the adsorption process is influenced simultaneously by the phosphate concentration and interaction between adsorbent and adsorbate. The change of curve slope from 4.0 to 0.89 and intercept from 0.76 to 27.6 in intra-particle model indicates that the adsorption process is controlled by a combination of intra-particle diffusion and film surface diffusion . The maximum phosphate adsorption capacity calculated from the Langmuir model is 47.7 mg-PO 4 3- /g, and the adsorption isotherm data are fitted well by the Freundlich model (r 2 = 0.95) and the Koble-Corrigan model (r 2 = 0.95), suggesting that the phosphate adsorption process is dominated by nonregular multilayer adsorption with the coexistence of monolayer adsorption. The ionic strength and co-existing anions have little impact on the adsorption capacity of LC-ZSM-5, proving the adsorption selectivity of phosphate onto LC-ZSM-5. Characterization results show that spindle-like lanthanum carbonate particles are fabricated on ZSM-5. Combining the adsorption process and the characterization, it can be derived that phosphate is adsorbed by LC-ZSM-5 mainly through electric attraction and ligand exchange. Our study demonstrates the great potential application value of LC-ZSM-5 in commonly seen phosphate-containing wastewater.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Mengmeng Zhang,Jiaying Lou,Rui Xu,Peng Li,Yunfei Sha,Hui Zhang,Yu Jia,Zhenxia Chen,Da Wu,Yun Ling,Yaming Zhou
Metal-organic frameworks (MOFs) featuring a fcu-type net based on 12-connected [Zr 6 (μ 3 -O) 4 (μ 3 -OH) 4 ] cluster have received considerable interest for the fundamental investigation of structure-property relationships in a wide range of catalytic reactions . In this work, the bipyridine (bpy) chelate group was introduced into the fcu-type framework of UiO-67, giving UiO-67bpy as the catalyst support. Then, FeCl 3 was post-synthetically anchored to the bpy group, resulting into the isolation of FeCl 3 /UiO-67bpy. Catalyzed hydrolysis of 5-hydroxylmethoxyfurfural (HMF) into levulinic acid (LA) was then explored and revealed that it can efficiently and selectively catalytic convert HMF into LA, which is superior to that of FeCl 3 /UiO-67 where FeCl 3 is encapsulated in the cage of UiO-67 and dispersed on the pore surface. The recyclability studies further confirmed the importance of anchored FeCl 3 where there is no significant decrease in catalytic activity as compared with that of FeCl 3 /UiO-67. Taking the detailed textural porosity and catalytic results of isomorphous structures in consideration, our studies revealed that narrowing the pore size with anchored FeCl 3 on the skeleton of the fcu-type Zr-MOF rather than encapsulating FeCl 3 inside the cage is more favored for the rehydration reaction of HMF to LA.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Lifang Gao,Zhenbang Liu,Jinling Ma,Lijie Zhong,Zhongqian Song,Jianan Xu,Shiyu Gan,Dongxue Han,Li Niu
A key challenge for the conversion of 5-hydroxymethylfurfural (HMF) into value-added 2,5-furandicarboxylic acid (FDCA) is improving the sluggish kinetics of selective oxidation alcohol groups. Electrocatalysis has been proved to be a green and efficient strategy for heterogeneous synthetic chemistry. Herein, we report an electrocatalyst of NiSe@NiO x core-shell nanowires for efficiently upgrading HMF into FDCA. The NiSe@NiO x features conductive NiSe nanowires as a core and active NiO x as a shell, showing a smaller Tafel slope of 23 mV dec −1 accompanying with a near-quantitative yield of FDCA and 99% Faradaic efficiency (FE). X-ray photoelectron spectroscopy unveils the high valence of Ni species in the NiO x shell may be the active sites. Further integrated electrolyzer can produce FDCA and hydrogen simultaneously, showing a 100% FE even after six successive cycles, disclosing robust stability. All these results demonstrate NiSe@NiO x core-shell nanowires as a promising robust non-precious electrocatalyst for highly efficient biomass transformation.
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Materials Research Express
·
2019
·Vol. 6
·期 11
·115540
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IF 1.449
Yong Liu,Qiong Luo,Hao Lu,Zhao Wang
The factors influencing the hydrothermal synthesis of ZSM-5 have been investigated in detail, such as silicon source, template, pH, reaction temperature, etc The type of template plays a key role. It is difficult to synthesize ZSM-5 without template or using inorganic template under our research conditions. However, the organic template of tetrapropylammonium bromide (TPABr) or n-butylamine (BTA) is beneficial to the synthesis of HZSM-5. The pH range of 10.79–11.14 is favorable for the synthesis of HZSM-5 zeolite. When temperature is greater than or equal to 160 °C, the synthesis of target zeolites is easy. However, if temperature is ≤140 °C, the synthesized product belongs to amorphous solid. Scanning electron microscopy (SEM) shows that the morphology of HZSM-5 crystal is hexagonal columnar. Fourier transform infrared (FTIR) analysis shows the synthesized product has a good ZSM-5 skeleton structure. The synthetic HZSM-5 zeolite has the BET specific surface area of about 387.326 m2 g−1. The adsorption capacities of the synthesized HZSM-5 for phenol, quinoline and indole can reach up to 43.54 mg g−1, 83.10 mg g−1 and 69.51 mg g−1, respectively.
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ACS Applied Bio Materials
·
2019
·
IF 0
Peihong Li,Chunling Zhang,Rui Li,Lijie Qu,Xueyan Dai,Yanlong Sui,Jiazi Hou
Pluronic F127 is a thermosensitive polymer that has been extensively studied and utilized in biomedicine. To improve the gelation properties of F127, α-cyclodextrin was introduced by physical interactions, such as forming inclusion complexes, hydrogen bond self-assembly, and hydrophobic interactions, to prepare F127−α-CD hydrogels. This study explored the temperature-dependent sol–gel transition behavior, gelation mechanism, interior morphology, and controlled release of the anticancer drug 5-fluorouracil. Results showed that hydrogel could be obtained at 1.0%–8.0% weight content of F127. The cross-linking points in this system were PEO−α-CD microcrystalline region and micelle with poly(propylene oxide) as the core. The network inside F127−α-CD hydrogels made it stable and conducive for controlled release. Therefore, this hydrogel is a promising drug release system.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2019
·Vol. 220
·期 4
·1800464
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IF 2.622
Lefan Li,Qiao Wang,Zongjin Li,Siyao Guo,Guoxing Sun
A gel material that can be applied to industry needs to fulfill two requirements: excellent mechanical properties and high temperature resistance. Previous research developed a hydrogel enhanced by sub-5 nm particles, with excellent mechanical properties. While its application in the open environment is still limited by the volatilization of inner moisture, in this research, a non-volatile gel (NV gel) enhanced by 5-nm spherulites is manufactured. The NV gel remains stable after staying at 90 °C for 24 h. Meanwhile, being enhanced by sub-5 nm nanospherulites, the NV gel shows good mechanical properties: with 200 ppm nanoparticle content, the tensile strength reaches 814 kPa and the compressive stress is 173.41 MPa at a recoverable 99% strain. The high temperature resistance is characterized by thermogravimetric analysis (TGA) and mechanical testing after thermal treatment. Transmission electron microscopy, scanning electron microscopy, Fourier transform infrared spectroscopy, time of flight secondary ion mass spectrometry, and thermogravimetric analysis are used to evaluate the microstructure of NV gel. Possessing non-volatile and good mechanical properties at the same time, this NV gel becomes very suitable for fulfilling the application requirement as an engineering material.
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BIORESOURCE TECHNOLOGY
·
2019
·
IF 6.669
Lin Jiang,Yunpu Wang,Leilei Dai,Zhenting Yu,Qi Yang,Sha Yang,Deyu Jiang,Zhiyun Ma,Qiuhao Wu,Bo Zhang,Yuhuan Liu,Roger Ruan
A ZSM-5/SiC composite catalyst was synthesized and characterized by Brunauer–Emmett–Teller analysis, X-ray diffraction, and scanning electron microscopy in this study. The composite catalyst had the characteristics of ZSM-5 and SiC, and the surface of SiC grew evenly with a layer of ZSM-5. The effect of the composite catalyst on the product distribution and chemical composition in a co-pyrolysis downdraft system was investigated. In a down system with a catalytic temperature of 450 °C, a feed-to-catalyst ratio of 2:1, and a soybean-soapstock-to-straw ratio of 1:1, the proportions of alkanes, olefins, aromatics, and phenoxy compounds were 6.82%, 4.5%, 73.56% and 11.11%, respectively. The composite catalyst combined the catalytic performance of ZSM-5 and SiC, increasing the proportion of aromatics and decreasing the proportion of oxygen-containing compound in the bio-oil. Moreover, the composite catalyst maintained its activity after reusing several times.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Bin Hu,Chunyang Li,Zengchen Liu,Xinlei Zhang,Wen Luo,Lin Jin
Two novel asymmetric structure monomers , 3,6-Bis-(2,3-dihydro-thieno[3,4- b][1,4]dioxin-5-yl)-9-[4-(2,5-di-thiophen-2-yl-pyrrol-1-yl)-phenyl]-9H-carbazole (BDTC) and 2,7-Bis-(2,3-dihydro-thieno[3,4-b][1,4]dioxin-5-yl)-9-[4-(2,5-di-thio phen-2-yl-pyrrol-1-yl)-phenyl]-9H-carbazole (BDDC), were designed and synthesized. Both the monomers could be electropolymerized to form the related polymer films. The electrochemical and electrochromic properties of polymer films were different from that of their homopolymers , which could be attributed to the similar copolymerization effect of asymmetric structure. Different linked positions also led to different features, PBDDC film showed more colors (orange, yellow green, green and blue) than that of PBDTC film (yellow, green and purple blue). However, after the introduction of 2, 2′-Bi(3,4-ethoxylene dioxy thiophene)(BIEDOT), the resulting copolymers exhibited similar electrochromic features(red, brown yellow, green and blue) due to the leading effect of EDOT units. Moreover, all the polymer films displayed fast switching time, reasonable optical contrast and good coloration efficiency, which made them have potential application in electrochromic devices.
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CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Jun Zhang,Kaijun Dong,Weimin Luo
A facile and mild method for the catalytic production of 2,5-dimethylfuran (DMF) from 5-hydroxymethylfurfural (HMF) was developed, which utilized commercial PdCl 2 as the catalyst together with the green, non-toxic and low-cost hydride source, polymethylhydrosiloxane (PMHS). A synergistic effect among hydrogen donor, in situ generated metallic Pd 0 species and acid site HCl in the reaction played a key role in DMF formation. Gratifyingly, the desirable yield of hydrodeoxygenation product DMF as high as 89.7% from HMF was attained at room temperature (298 K) in 0.5 h. Meanwhile, biomass derived sugars also could be converted into DMF in relative high efficiency via a one-pot reaction in the present system. A plausible pathway for the hydrodeoxygenation of HMF into DMF in the present system was also proposed. The study thus highlights a new perspective for a simple, green, and efficient hydrodeoxygenation of biomass derivatives under milder conditions, employing a readily available, inexpensive and practical catalytic system of PdCl 2 -PMHS-ethanol, but without any external hydrogen supplies and pre-reduction treatments.
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Xiaoyue Wan,Qi Zhang,Mingming Zhu,Yi Zhao,Yongmei Liu,Chunmei Zhou,Yanhui Yang,Yong Cao
Site-selective deoxygenation of hydroxyl groups represents essential processes to access valuable functionalized bio-based compounds with industrial potential. One of the challenging tasks in this context is to convert biodiesel-derived glycerol in the presence of abundant water directly to 1,3-propanediol (1,3-PDO), a key component of the emerging polymer industry. Herein, a monometallic iridium supported on H-ZSM-5 in the absence of Re oxophilic metal oxides was prepared via grinding-assisted impregnation procedures and attempted as an effective and recyclable catalyst for the aqueous-phase selective hydrogenolysis of glycerol toward 1,3-PDO in the absence of acid additives. The results revealed the necessity to control the Ir domain dispersions, Ir 0 /Ir 3+ ratio and the amounts of overall acid/Brönsted acid sites. Activity depended linearly on the amount of overall and Brönsted acid sites, and 1,3-PDO selectivity increased in the presence of Ir-induced Brönsted acid sites, denoted as Ir-O(H)-H-ZSM-5. We speculate that Ir-O(H)-H-ZSM-5 are generated by the interfacial synergistic interaction between IrO x and H-ZSM-5 through hydrogen spillover and reverse hydrogen spillover according to the reported literatures. The reaction mechanism to elucidate the role of Ir-O(H)-H-ZSM-5 sites in glycerol hydrogenolysis was also postulated based on extensive characterization and catalytic reaction results.
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