Biomass Conversion and Biorefinery
·
2020
·Vol. 11
·期 5
·1931-1941
·
IF 2.602
Tian Xiatian,Qi Benkun,Zhang Shaofeng,Luo Jianquan,Wan Yinhua
5-Hydroxymethylfurfural (HMF) is a promising platform chemical for production of value-added chemicals and fuels. Conversion of abundantly available and cheap sucrose for HMF synthesis was systematically investigated in the present study. Results showed that Lewis acid AlCl 3 is effective in catalytic transformation of sucrose. Combining AlCl 3 with different Brønsted acids, no matter whether they were inorganic acids (HCl, H 2 SO 4 , and H 3 PO 4 ) or organic acids (malic acid, succinic acid, and oxalic acid), or variation of ratio of Lewis acid/Brønsted acid represented by AlCl 3 /HCl, did not change the obtained maximum HMF yields compared with AlCl 3 alone, but shortened the time required to reach the maximum HMF yield. Sucrose conversion in a green reaction media of aqueous γ-valerolactone (GVL) solvent resulted into comparable HMF yields with dimethyl sulfoxide (DSMO)-water system. Addition of monovalent salt NaCl and divalent salt Na 2 SO 4 produced opposite effect with Cl − promoting while SO 4 2− inhibiting HMF production. Furthermore, HMF synthesis from constituent monosaccharides of sucrose and molasses, a by-product from sugar manufacturing process, was also carried out and it was found that an equivmole mixture of glucose and fructose gave rise to almost identical HMF yield to the same mole of sucrose. Molasses, even after chemical pretreatment for removal of certain amount of inorganic salts and color substances, was significantly inferior to synthetic molasses in terms of HMF formation, indicating the complexity and difficulty in chemical valorization of molasses for production of platform molecules.
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CATALYSIS LETTERS
·
2020
·Vol. 151
·期 2
·538-547
·
IF 2.482
Chen Han,Xu Qiong,Li Hui,Liu Jian,Liu Xianxiang,Huang Geng,Yin Dulin
Nickel supported on equilibrium fluid-catalytic-cracking catalysts (Ni/E-cats) were prepared by a simple grinding-pyrolysis method and employed for the transfer hydrogenation of ethyl levulinate (EL) to γ-valerolactone (GVL). 96.2% selectivity of GVL and 90.3% conversion of EL were obtained at 180 °C for 6 h over 30-Ni/E-cat. Through XRD, N 2 adsorption–desorption, NH 3 -TPD and SEM analysis, the high activity of the 30-Ni/E-cat catalyst was attributed to its dispersed Ni metal active centers and available acidic sites. Catalytic probe test revealed that metal and acid sites of Ni/E-cat played a synergistic catalytic role in the synthesis of GVL in 2-propanol, where Ni metal sites contribute to the hydrogenation of ketone group in EL, and acid sites of E-cat promoted the lactonization of intermediate ethyl- or isopropyl 4-hydroxyvalerate. Two reaction pathways and synergistic mechanism were proposed in this catalytic system. Moreover, Ni/E-cat catalyst exhibited good stability up to four cycles without obvious loss of catalytic activity. Graphic Abstract
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ACS Applied Bio Materials
·
2020
·
IF 0
Xuebin Ma,Xin Liu,Penghui Wang,Xiaoxue Wang,Rong Yang,Shuai Liu,Zhiwen Ye,Bo Chi
Reversibly cross-linked adaptable hydrogels show great advantages in tissue engineering. The dynamic adaptable networks can overcome three-dimensional (3D) physical restrictions to enable normal cellular functions without hydrogel degradation. However, because of the dynamic reversibility, adaptable hydrogels typically exhibit weak mechanical properties and rapid erosion behaviors. Herein, we develop a facile strategy to prepare stable adaptable hydrogels using dynamic covalent chemistry, stable covalent chemistry, and the interpenetrating polymeric network (IPN) strategy. The developed IPN HA/γ-PGA adaptable hydrogels have stable structures, good mechanical properties, enzymatic degradability, and injectability. Compression test indicates that although containing 95% water, the IPN HA/γ-PGA adaptable hydrogels can suffer more than 85% compressive strain and show a fast shape recovery capacity and good antifatigue ability. Benefitting from the good cytocompatibility of functionalized HA and γ-PGA and the mild preparation process of IPN HA/γ-PGA adaptable hydrogels, NIH 3T3 cells can tolerate the 3D encapsulation process and show high cell viability. Therefore, owing to their desirable properties, the developed HA/γ-PGA adaptable hydrogels have great potential applications for load-bearing tissue engineering.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Wenlin Li,Feng Li,Junwen Chen,Luis E. Betancourt,Chunyan Tu,Mingjie Liao,Xing Ning,Jiajun Zheng,Ruifeng Li
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is an essential reaction step to produce value-added renewable chemicals and fuels. In this study, it is demonstrated that the dispersed state of metal and the acid properties of the support can be tuned directly in the synthesized stage for the Ru/MCM-49 catalysts. The average metal particle size of Ru was found at ∼2.0 nm, and strong metal–support interaction was observed for the Ru/MCM-49(DP) catalyst. Mesopores presented can enhance the conversion rate for LA to GVL. The presence of a higher amount of Lewis acid sites can promote the ring closure esterification of the intermediate 4-HPA. High catalytic activity with a TOF value of >3000 h–1, as well as excellent reusability, were achieved by Ru/MCM-49(DP). The agglomeration of Ru particles and the coke formation were thought to be responsible for the deactivation of the catalyst.
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Journal of Materials Chemistry C
·
2023
·
IF 6.4
Tianqi Zhao,Renagul Abdurahman,Qianting Yang,Ruxiangul Aiwaili,Xue-Bo Yin
Herein, we designed and prepared the persistent luminescence nanoparticles (PLNPs) of γ-Ga2O3:Cr,Ba rationally with Cr ions to achieve the near-infrared (NIR) emission at 700 nm and Ba ions to improve the emission intensity by inducing trap distribution. Energy transfer between γ-Ga2O3 and Cr ions occurs as the emission at 508 nm decreases and that at 700 nm increases along with the increased content of Cr ions. In combination with the trap depth, band gap of the host, and energy levels of Cr ions, an emission mechanism was proposed. Thus, NIR emission (700 nm), high brightness, large Stokes shift (446 nm), and long afterglow time (90 min) were achieved with the optimal γ-Ga2O3:0.0025Cr,0.0012Ba (γGCB) under excitation at 254 nm. The emission intensity of γGCB is temperature-dependent for non-contact ratiometric temperature sensing, and temperature linearity ranging from 300 to 420 K was achieved with an absolute sensitivity of 3.4% K−1. γGCB and γ-G2O3 are white under sunlight but exhibit red and green emissions under single excitation at 254 nm. Thus, Morse and binary codes are adapted to achieve encryption information transfer with the combination of γGCB and γ-G2O3. This work provides ideas for selecting a host, emission center, and trap for PLNPs with desirable properties and thus achieves extensive applications, as validated with ratiometric temperature sensing and encryption information transfer.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Shutong Hao,Xiaolin Liu,Qianli Li,Mu Gu,Shuai Cheng,Jingtai Zhao
The demand for scintillators with ultrafast decay times, high spatial resolutions, and high stabilities is increasing due to the development of ultrafast hard X-ray detection, hard X-ray imaging, and high-energy physics facilities. γ-CuI single crystals, which exhibit ultrafast luminescence and high stopping power for hard X-rays, hold great promise for such applications. However, slow luminescence and poor stability caused by surface iodine deficiencies hinder the practical use of γ-CuI. Herein, we treated a γ-CuI single crystal by iodine annealing and SiO2 coating and investigated its crystal structure and luminescence properties in detail. Iodine annealing significantly enhanced the near-band-edge emission of the γ-CuI crystal with an ultrafast decay time of less than 1 ns, while completely suppressing the slow luminescence. Moreover, the SiO2 film effectively prevented the oxidation and decomposition of surface iodine, leading to substantial improvement in luminescence stability. The γ-CuI crystal demonstrated an ultrahigh spatial resolution of 1.5 μm in X-ray imaging, highlighting its potential for ultrafast hard X-ray imaging applications. This study provides insight into the growth, optimization, and application of γ-CuI crystals, advancing the field of scintillator materials.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Qiangqiang Wu,Hanke Li,Guangxing Yang,Yonghai Cao,Hongjuan Wang,Feng Peng,Hao Yu
A variety of adsorbed intermediates have been extensively assigned during CO 2 hydrogenation on Pt/γ-Al 2 O 3 . However, the surface sites where the surface species reside have not been well resolved, which are extremely important to depict the reaction pathways of CO 2 hydrogenation. In the current work, surface species adsorbed on three regions were distinguished by in situ diffuse-reflectance infrared Fourier transform spectroscopy, i.e., contiguous Pt region of Pt nanoparticle, interfacial Pt int -O-Al int region between Pt nanoparticle and γ-Al 2 O 3 , and surface region of γ-Al 2 O 3 away from Pt nanoparticle. The dynamics of adsorbed H species, carbonyl species, bicarbonates, formate species, and adsorbed CO 2 , were identified at different sites, proving that the reaction occurs at the Pt/γ-Al 2 O 3 interface. We found that only the C-containing species at the Pt perimeter are directly active intermediates for the reaction. Such spatial analysis bridges the gap between the hydrogen activation and CO 2 activation, providing a deep understanding of CO 2 hydrogenation. In addition, the interface structure with oxygen vacancy is important for CO 2 activation, driving the reaction through carboxylate (*HOCO) pathway to form CO at the interface rather than formate (*HCOO) pathway and then be hydrogenated at the Pt surface.
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ChemCatChem
·
2023
·Vol. 15
·期 7
·e202300194
·
IF 4.5
Tao Li,Mengling Dong,Jiacheng Xu,Tiantian Zhang,Yan Sun,Ning Li,Zuliang Wu,Jing Li,Erhao Gao,Jiali Zhu,Shuiliang Yao,Yong Huang
Graphical CeO 2 /γ-Al 2 O 3 , Pd/CeO 2 , and Pd/CeO 2 /γ-Al 2 O 3 were used for catalyzing low-concentration CH 4 oxidation . γ-Al 2 O 3 can efficiently promote CH 4 oxidation on Pd/CeO 2 and the formation of bicarbonate that is easily gasified to CO 2 . CeO 2 /γ-Al 2 O 3 , Pd/CeO 2 , and Pd/CeO 2 /γ-Al 2 O 3 were used for catalyzing low-concentration CH 4 oxidation. It was found that nano-sized Pd could obviously promote CH 4 oxidation on CeO 2 /γ-Al 2 O 3 . The interaction between Pd and CeO 2 on γ-Al 2 O 3 resulted in higher ratios of Ce 3+ /(Ce 3+ +Ce 4+ ), Pd 2+ /(Pd 2+ +Pd δ+ ), and O ads /(O ads +O latt ), those benefited the formation of more oxygen vacancies and surface reactive oxygen species for CH 4 oxidation. γ-Al 2 O 3 not only supplied a high surface area and enhanced Pd/CeO 2 dispersion on γ-Al 2 O 3 , but also simulated the formation of bicarbonate, where bicarbonate is easier to gasify to CO 2 than bidentate carbonate that formed on Pd/CeO 2 . Operando diffuse reflectance infrared Fourier transform spectroscopy-mass spectrometer analysis results showed that CH 4 oxidation could occur at a temperature as low as 180 °C due to the reaction with surface reactive OH, this reaction was also accompanied by the formation of bicarbonate. The mechanism of CH 4 oxidation promoted by bicarbonate formation on γ-Al 2 O 3 was proposed.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Jiayu Feng,Ping Ning,Kai Li,Xin Sun,Chi Wang,Lijuan Jia,Maohong Fan
The conventional Haber–Bosch NH3 synthesis process requires high temperatures and pressures, resulting in a high carbon footprint and the need to develop alternative NH3 synthesis methods. Accordingly, plasma-based and γ-Al2O3-catalyzed NH3 synthesis from H2O (a hydrogen source) and air/N2 (a nitrogen source) was studied under low temperature and low pressure conditions. The experimental results show that NH3 can be synthesized with air/N2 and H2O, although byproducts such as NO and N2O are also formed. The NH3 formation rate resulting from the use of N2 and H2O is higher than that of air and H2O. Increasing specific energy input (SEI) can increase the NH3 formation rate. Nevertheless, the energy efficiency of NH3 synthesis technology first increases and then decreases with SEI. An NH3 formation rate of 2.92 μmol h–1 g–1 was achieved with an SEI of 11.68 J mL–1 and energy efficiency of 5.10 mg kW–1 h–1 (1.28 mg kWh–1g–1), when wet air at a flow rate of 200 mL min–1 was introduced into the dielectric barrier discharge (DBD) reactor, which was lower than that (4.30 μmol h–1 g–1) attained with N2 + H2O under an SEI of 11.50 J mL–1 and energy efficiency of 7.63 mg kW–1 h–1 (1.91 mg kWh–1g–1). Additionally, the γ-Al2O3 catalyst exhibited good stability. Different results show that plasma-based and γ-Al2O3 catalyzed NH3 synthesis technology is promising.
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Frontiers in Pharmacology
·
2019
·
IF 3.845
Linghu Ke-Gang,Wu Guo-Ping,Fu Ling-Yun,Yang Hong,Li Hai-Zhi,Chen Yan,Yu Hua,Tao Ling,Shen Xiang-Chun
1,8-Cineole (eucalyptol), a monoterpene, has been widely reported for the anti-inflammatory effects. Our previous data confirmed that 1,8-cineole ameliorated the inflammatory phenotype of human umbilical vein endothelial cells (HUVECs) by mediating NF-κB expression in vitro. At present, we investigated the protection effects of 1,8-cineole on vascular endothelium in lipopolysaccharide (LPS)-induced acute inflammatory injury mice and the potential mechanisms involved in the protection in HUVECs. Results from enzyme linked immunosorbent assays revealed that 1,8-cineole suppressed the secretion of interleukin (IL)-6 and IL-8 and increased the expression of IL-10 in the serum of LPS-induced mice. 1,8-Cineole reduced the inflammatory infiltration and the expression of vascular cell adhesion molecular 1 (VCAM-1) in the sections of thoracic aorta in LPS-induced acute inflammatory mice. Western blotting indicated that 1,8-cineole significantly decreased the phosphorylation of NF-κB p65 and increased the expression of PPAR-γ in the thoracic aorta tissue. 1,8-Cineole increased the expression of PPAR-γ in LPS-induced HUVECs. 1,8-Cineole and rosiglitazone reduced the protein and mRNA levels of VCAM-1, E-selectin, IL-6, and IL-8 in LPS-induced HUVECs, which could be reversed by the action of GW9662 (inhibitor of PPAR-γ). 1,8-Cineole and rosiglitazone blocked the LPS-induced IκBα degradation and NF-κB p65 nucleus translocation, which could be reversed by the pretreatment of GW9662 or silence of PPAR-γ gene. In conclusion, 1,8-cineole attenuated LPS-induced vascular endothelial cells injury via PPAR-γ dependent modulation of NF-κB.
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高影响因子
RENEWABLE ENERGY
·
2019
·
IF 5.439
Jian He,Hu Li,Yufei Xu,Song Yang
γ-Valerolactone (GVL) is an interesting bio-based platform molecule that is utilized as green solvent and a versatile building block for the synthesis of bio-fuels and chemicals. Herein, an investigation on the efficient production of GVL from biomass-based carbonyl compounds such as furfural, levulinic acid, and its esters using 2-propanol as H-donor and solvent over stable Zr-incorporated mesoporous silica (KIT-5) catalysts was presented. Both Lewis and Brønsted acid sites were generated by the introduction of Zr into KIT-5, and the acid density of the resulting Zr-KIT-5(Si/Zr) could be controlled by simply adjusting Si/Zr molar ratio . Among these bifunctional catalysts , Zr-KIT-5(10) showed superior catalytic performance in the production of GVL (>91% selectivity) from biomass-derived carboxides (ca. 94% conversion), which was demonstrated to positively correlate with its large amount of acidic sites and facile access of active sites to interconnected pores. Moreover, the spent catalyst held about 90% of its original activity in the sixth run. Due to the presence of Brønsted and Lewis dual acidic sites in Zr-KIT-5, the direct conversion of furfural to GVL was also permitted in a single pot via tandem reactions involving hydrogenation, ring-opening, secondary hydrogenation, and subsequent cyclization.
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ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Chuanhui Huang,Yujie Wang,Qiao Huang,Yu He,Lan Zhang
Microcystins (MCs), which are produced by eruptive cyanobacteria , seriously threaten the health of humans for their poisonousness. Herein, a facile strategy was introduced to synthesize the magnetic γ-cyclodextrin polymer (Fe 3 O 4 @PDA@γ-CDP) composite and set it as a novel adsorbent with excellent properties for the magnetic solid-phase extraction (MSPE) of MCs. The prepared Fe 3 O 4 @PDA@γ-CDP microspheres exhibit good aqueous dispersibility and highly affinity for MCs, thus contribute to an excellent extraction performance for trace MCs in water samples. Combined with HPLC–MS/MS, a handy, sensitive and efficient method was developed for detection of MCs in water samples, which shows good linearity (R 2 ≥ 0.9992) in the range of 1.0–1000 pg mL −1 , low limits of detection (0.8–2.0 pg mL −1 , S/N = 3), satisfactory repeatability with the relative standard deviations (RSDs) lower than 6.2% (n = 5). At last, the proposed method was successfully applied for the extraction and detection of MCs in fresh water and sea water samples, which provides great potential of trace-level MCs determination in lake and sea water.
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