JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Zongping Jia,Chengying Du,Lulu Zhu,Zhonglai Wang
An alumina porous layer open-tubular (Al 2 O 3 PLOT) column coated with γ–alumina nanoparticles (20 nm) for highly volatile hydrocarbons (C1 to C5) separation was described. Relative to the coating of bulk alumina, this column was easily coated with dynamic method under 0.4 or 0.6 MPa for 0.53 mm or 0.32 mm capillary, respectively. And the thickness of coating layer could be tuned by repeating the coating process after column was dried and activated at 300 °C for 3 h. The effect of deactivation agents on the physicochemical properties of nano γ–alumina was characterized by X–ray diffraction (XRD) measurement and nitrogen adsorption–desorption isotherms. The influences of deactivation agents, film thickness, conditioning and column dimensions on the inertness, polarity, selectivity and elution order of C1 to C5 separation were investigated in detail. The crystallite structure and size of nano alumina were not affected by the deactivation agents and remained constant during the column making processes, whereas specific surface area, pore volume and average half pore width altered significantly. The specific surface area decreased to 125.4 m 2 g –1 or 174.0 m 2 g –1 and the average half pore size distributions decreased to 1.6–8.4 nm or 2.4–14.3 nm when it was deactivated with potassium chloride or sodium sulfate solution, respectively. The deactivation agents and its concentrations impacted significantly on the retention performance of column. The column deactivated with sodium sulfate solution exhibited stronger polarity and lower selectivity than which deactivated with potassium chloride solution although both columns showed good inertness. The length, internal diameter and film thickness of the column had less influence on the selectivity and resolution for C1 to C5 hydrocarbons separation, whereas the conditioning temperature and time had an obvious influence. The column had distinguished polarity and selectivity which was different from either bulk or commercial alumina columns. Typically, the hydrocarbons were baseline separated with resolutions ranging from 1.65 to 15.33 within 9 min under programmed temperature below 100 °C, and the tailing factors ranging from 1.02 to 1.07.
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高影响因子
CHEMISTRY OF MATERIALS
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2022
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IF 10.508
Ningdi Xu,Baolong Wang,Ziqiang An,Yingying Liu,Li Liu,Zhen Hu,Yudong Huang
γ-Radiation derived from clean energy has emerged as a promising technology for disposal of waste plastics. However, due to radical-mediated uncontrolled recombination, a foremost challenge remains in radiation-triggered complete degradation for thermoset plastics. Herein, the radiation-sensitive epoxy thermoset (EP-DESN) containing phenyl imine-conjugated N–N bonds (PINN bonds) and S–S bonds was designed to initiate rapid degradation at a dose of 10 kGy. The phenyl imine-conjugated linkages can stabilize the radiation-induced broken N–N bonds, overcoming radical-mediated uncontrolled recombination and cross-linking. Moreover, the phenyl-iminyl-conjugated radicals generated by PINN bond scission can cleave the active S–S bonds to promote subsequent spontaneous degradation for maximum degradation efficiency. Meanwhile, EP-DESN exhibited superior thermal robustness and chemical resistance comparable to some conventional high-performance epoxy thermosets. Using EP-DESN as a binder, we prepared recyclable carbon fiber-reinforced composites, and nondestructive recycling of value-added carbon fiber (CF) is achieved, thus facilitating the concept of a circular CF economy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Jin Liu,Hongyu Chen,Chaosheng Zhu,Songfang Han,Jun Li,Sijia She,Xiaoyong Wu
Advanced oxidation processes (AOPs) based on photo-Fenton reaction has been widely used in refractory organic wastewater treatment . However, the mineralization rate and H 2 O 2 utilization in AOPs is relatively low. Herein, a photothermal-assisted photocatalytic-Fenton-like process with CuO x /γ-Al 2 O 3 catalyst was designed to solve the above issues. The utilization rate of H 2 O 2 and mineralization rate of tetracycline hydrochloride (TC) in the 3%-CuO x /γ-Al 2 O 3 /H 2 O 2 /full spectrum light system were significantly increased to 72.0% and 74.3%, respectively, which were ascribed to the synergy of photothermal effect and photocatalytic-Fenton-like reaction. During the simultaneous removal of TC and Cr(VI), the reaction efficiency of 3%-CuO x /γ-Al 2 O 3 /H 2 O 2 /light system was much higher than that of 3%-CuO x /γ-Al 2 O 3 /H 2 O 2 system. In addition, the 3%-CuO x /γ-Al 2 O 3 /H 2 O 2 /light system was not only active in wider pH range (3–9), but also effective in various organic pollutants and Cr(VI) coexisted solutions as well as different water conditions. More importantly, a possible photothermal-assisted photocatalytic-Fenton-like reaction mechanism for the simultaneous removal of TC and Cr(VI) in the CuO x /γ-Al 2 O 3 /H 2 O 2 /light system was proposed. This work may pave a new way for efficient simultaneous removal of refractory organic pollutants and heavy metals in wastewater.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yifan Wang,Zhengjie Peng,Youqing Yang,Zhonnan Li,Yujiao Wen,Meng Liu,Shikai Li,Lezhu Su,Zhi Zhou,Yongfa Zhu,Nan Zhou
The abuse of agrochemicals has caused serious environmental pollution, raising urgently requirement for sensitive controlled release systems. Biochar supported γ-FeOOH nanoarrays (γ-FeOOH@BC) were synthesized in situ through a two-step pyrolyzation-oxidation procedure. The decoration of γ-FeOOH nanoarray structure significantly enhanced the surface positive charge of the composite (pH zpc increased from 2.7 to 7.8), due to which active substances could be electrostatically self-assembled on γ-FeOOH@BC to realize accurate release by changing the environmental pH. The assembled amounts of QNC and PO 4 3- could reach a value of 94 mg·g −1 and 92 mg·g −1 respectively, and the encapsulation efficiency as well as the release concentration were closely related to the pKa of the substance. 45% (QNC) and 63% (PO 4 3- ) could be released at pH = 7.8 and finally both reached to 88% at pH = 11. After 5 rounds of the sensitivity test, QNC/ PO 4 3- could be well assembled or released by pH adjustment, and the encapsulation efficiency remained above 75%. Meanwhile, the assembly structures could also be self-formed in real soil containing QNC/PO 4 3- and had selective herbicidal activity on barnyard grass plants. This work not only provides a feasible material but also a novel method for self-assembly and controlled release of agricultural chemicals.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xiaoyan Yin,Tingting Cai,Chao Liu,Chen Huang,Jia Wang,Jun Hu,Neng Li,Jianchun Jiang,Kui Wang
Efficient depolymerization of lignocellulosic biomass into platform chemicals is of great importance to bring the comprehensive bio-refinery concept into industrial reality. Herein, we reported an environmentally benign pretreatment process for full components utilization of moso bamboo in co-solvent of γ-valerolactone (GVL) and aqueous solution of p -toluenesulfonic acid (TsOH aq). Notably, over 98 wt% of lignin and hemicelluloses could be simultaneously degraded into oligomeric phenols and pentose under the mild condition of 130 °C for 60 min with GVL/TsOH aq volume ratio of 4/1, following with 91.5 wt% of cellulose retained which was then enzymatic hydrolyzed into 773.2 mg/g glucose. All of the obtained platform chemicals could be easily separated and purified, which significantly facilitate the excellent retrieve of the co– solvent. Moreover, the synergistic effect between GVL and TsOH on efficiency and specificity was proposed by control group experiment and verified by molecular dynamics simulation and quantum chemical calculation. This study provides a facile pretreatment and direct conversion strategy for biorefinery process of lignocellulosic biomass in novel GVL/TsOH aq co-solvent.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2021
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IF 6.064
Yafei Li,Xiaocheng Lan,Boyang Liu,Tiefeng Wang
A stable and highly efficient supported Cu-Ni catalysts for the conversion of ethyl levulinate (EL) to γ-valerolactone (GVL) was developed. The catalysts were characterized by XRD, TEM, TPD, TPR, and XPS. The support effect of metal oxides (Al 2 O 3 , SiO 2 , ZrO 2 , and TiO 2 ) revealed that Cu-Ni supported on Al 2 O 3 showed the highest activity for EL hydrogenation to ethyl 4-hydroxypentanoate (EHP) and the subsequent intramolecular esterification of EHP to GVL. EHP intramolecular esterification to GVL in the ethanol solution was a reversible reaction with an equilibrium constant of 24 at 453 K. A simplified reaction kinetic network was established. The solvent had a significant influence on the reaction equilibrium and the catalyst stability. Cu-Ni/Al 2 O 3 in n-hexane solvent gave a higher GVL yield than that in ethanol solvent, and showed better recyclability than that in toluene solvent. With optimizing the conditions, Cu-Ni/Al 2 O 3 gave 99.9% conversion and 98% selectivity to GVL with a space–time yield of 1.13 g GVL g cat -1 h −1 in n-hexane solvent with good recyclability.
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高影响因子
Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Lina Zhou,Xingwang Zhang,Lecheng Lei
The δ-FeOOH/γ-Al 2 O 3 composite were prepared under mild conditions by the activated alumina absorption of Fe 2+ followed by rapid oxidation by H 2 O 2 . The δ-FeOOH growing on γ-Al 2 O 3 was composed of nanoneedles , forming a 3D flower-like morphology with a diameter of ~10 nm to provide a large number of active sites. The effects of Fenton reaction conditions, such as catalyst dosage, H 2 O 2 concentration, phenol concentration, initial pH value and temperature, on the catalytic activity of δ-FeOOH/γ-Al 2 O 3 were investigated. Under the optimal conditions, about 97.4% of phenol and 81.6% of total organic carbon (TOC) were removed in 5 min and 2 h, respectively. In addition, with γ-Al 2 O 3 as macroscopic size carrier (the diameter of 1–2 mm), the catalyst could be easily reused 10 runs with no significant reduction in catalytic activity. The possible mechanism was discussed, and it revealed that OH· was the main active species for degradation of phenol into intermediates and further into CO 2 and H 2 O. The δ-FeOOH/γ-Al 2 O 3 also showed high catalytic activity and reusability in the treatment of real industrial wastewater , making it a promising catalyst for industrial application.
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高影响因子
FUEL
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2021
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IF 6.609
Rulu Huang,Yao Liu,Junhua Zhang,Junnan Wei,Lincai Peng,Xing Tang
Both value-added utilization of agricultural waste to prepare catalytic materials and selective conversion of biomass-based carbonyl compounds are hot topics. Herein, sugarcane bagasse ( SB ), a main by-product of cane sugar manufacturing industry, was directly assembled with HfCl 4 and methanesulfonic acid (MSA) via a one-step hydrothermal method for scalable preparation of Hf-containing coordination complex (Hf@ SB -MSA). Characterization results revealed that the coordination between Hf 4+ and phenolic hydroxyl, alcohol hydroxyl, carboxyl groups in SB resulting in the formation of Lewis acid (LA) and Lewis base (LB) sites, while sulfonic group in MSA providing Brønsted acid (BA) sites. The cooperative role of LA, BA and LB in Hf@ SB -MSA delivered prominent catalytic performance for catalytic transfer hydrogenation (CTH) of levulinic acid (LvA) to γ-valerolactone (GVL) with isopropanol as solvent and H-donor at mild reaction conditions (GVL yield was up to 99.1%). Heterogeneity and recycling experiments further revealed the good recyclability of Hf@ SB -MSA, which can be easily separated from the reaction mixture by filtration and repetitively used at least five reaction runs without an obvious loss of activity. More gratifyingly, Hf@ SB -MSA also displayed superior universality for the CTH of various carbonyl compounds to their corresponding alcohols with yields up to 90%.
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Xi Cheng,Qingge Feng,Dachao Ma,Hongcheng Chen,Xu Zeng,Feifan Xing,Jiayang Teng
To eco-friendly catalyze glucose to levulinic acid, recyclable acid catalyst has been researched. The synthesis process of propyl sulfonic acid functionalized SBA-15 was improved and the hydrophobic treatment was performed. The structure and functional groups of materials were characterized by X-ray diffraction, transmission electron microscopy , N 2 adsorption–desorption isotherms, elemental analysis, Fourier transform infrared spectroscopy , X-ray photoelectron spectroscopy and simultaneous thermal analysis. The catalytic activity , recyclability and hydrothermal stability of CH 3 -SBA-15-SO 3 H material were researched. The highest yield of levulinic acid at 61.56% was obtained at 180 ℃ for 2.5 h in γ-GVL-water solvent system, and the yield of levulinic acid was only decreased by 2% after 4 times reuse. The high degree of silicon polycondension and hydrophobic surface of CH 3 -SBA-15-SO 3 H were the key to maintain the hydrothermal stability. The CH 3 -SBA-15-SO 3 H solid acid had great potential in development and utilization of biomass resources .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zhihui Yao,Yuting Li,Daisong Chen,Yiwen Zhang,Xinghong Bao,Juan Wang,Qin Zhong
Carbon-based materials have shown promising results in replacing commercial Pt/C as highly efficient oxygen reduction reaction (ORR) catalysts in renewable energy devices. Designing unique structures of carbon matrix and introducing more active sites are essential for their application as electrode materials. Herein, a feasible approach is reported to synthesize dispersive γ -Fe 2 O 3 clusters embedded in 1D porous carbon nanofibers (CNFs) ( γ -Fe 2 O 3 @CNFs-12) through electrospinning, impregnation and pyrolysis processes. The resulted γ -Fe 2 O 3 @CNFs-12 exhibits excellent ORR performance in alkaline electrolyte with a surprising half-wave potential ( E 1/2 ) of 0.905 V and merely 5 mV drop of the potential after 5000 cycles, outperforming that of commercial Pt/C. Meanwhile, it also shows considerable ORR performance in acidic and neutral media. The remarkable ORR catalytic activity and durability are primarily attributable to the well-designed 1D hierarchical porous structure and accessible γ -Fe 2 O 3 clusters that embedded in carbon nanofibers. γ -Fe 2 O 3 @CNFs-12 is also capable to act as an air cathode for Zn-air batteries with an open circuit voltage of 1.428 V. This work provides a new perspective to the novel design and synthesis of carbon-based ORR electrocatalysts.
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高影响因子
ACS Applied Bio Materials
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2019
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IF 0
Nier Wu,Huilei Yu,Muyang Sun,Zong Li,Fengyuan Zhao,Yingfang Ao,Haifeng Chen
Silk fibroin (SF) is a natural polymer with low immunogenicity and good biocompatibility. However, most silk-based hydrogels formed through chemical or physical cross-linking are brittle, the preparation of which also inevitably introduces cytotoxic cross-linking agents. Herein, a simple strategy is presented for synthesizing SF hydrogels with tunable mechanical properties by combining γ-ray radiation with ethanol treatment. Neither toxic initiators nor chemical agents are utilized during the whole preparation procedure. For “soft” hydrogels, the compressive moduli are less than 29 kPa (SF-S hydrogels), while for “tough” hydrogels, the compressive moduli are between 1.21 and 2.41 MPa (SF-D hydrogels). Specifically, γ-ray radiation makes SF form uniform and stable chemical cross-linking sites within and between molecular chains, resulting in “soft” and highly elastic SF hydrogels. The physical cross-linking via ethanol treatment leads to the self-assembly of fibroin chains, transforming those soft hydrogels to tough hydrogels. These double cross-linked SF hydrogels (SF-D hydrogels) exhibit excellent mechanical strength. Effects of various cross-linking conditions on the secondary structure, pore structure, mechanical properties, gelation degree, swelling, and in vitro degradation properties are explored. A series of cell experiments demonstrate that the SF hydrogels with different mechanical strength can stimulate the expression of specific genes of rat bone marrow mesenchymal stem cells (BMSCs) in various differentiation directions. These results also show the application prospects in tissue engineering by customizing hydrogels for the mechanical strength of different tissues.
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ACS Catalysis
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2023
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IF 12.9
Chao Zhang,Yingqiang Li,Yue Xie,Zhanjiang Yu,Xin Wan,Xinzhi Wang,Jiaan He,Junlang Li,Zhenguo Chen,Xiaoyong Li,Xiaohui Yi,Zhaoli Wang,Guang-Guo Ying,Dionysios D. Dionysiou,Mingzhi Huang
Selective hydrodehalogenation and hydrodearomatization of toxic chlorophenols into value-added chemicals represents a grand challenge for their efficient reutilization. For this purpose, single-atom catalysts (SACs) could be a strategy with relatively high catalytic selectivity and atom utilization but suffer from the catalytic limitation caused by low metal loading densities. Graphdiyne and γ-graphyne are considered promising substrates of SACs with excellent catalytic properties. Additionally, their quantum dots with nanometer size are expected to supply numerous surface anchoring sites and large atom spacing to confine metal cations to synthesize high-loading SACs. Here we report a synthesis approach for high-loading Ru SACs anchored on graphdiyne/γ-graphyne quantum dots (GDQD-Ru/GNQD-Ru), which exhibit remarkably higher turnover frequency (TOF) and selectivity (>99%) of hydrodehalogenation and hydrodearomatization of chlorophenols than graphdiyne/γ-graphyne nanosheet-based Ru SACs and nanoparticles. There is no significant selectivity decrease in chlorophenol transformation by GDQD-Ru/GNQD-Ru observed in 5 catalyst reuse cycles. GDQD-Ru/GNQD-Ru contribute to nearly exclusive hydrodehalogenation and hydrodearomatization without altering any other bonds in chlorophenols. Experimental results and theoretical calculations reveal that GDQD-Ru is more prone to lower energies of rate-limiting steps in H2-driven chlorophenol transformation than GNQD-Ru. The results confirm that graphdiyne/γ-graphyne quantum dots play crucial roles in facilitating the metal atom loading of SACs. Ru loadings are 27.6 and 16.0 wt % in GDQD-Ru/GNQD-Ru, approximately 7-fold and 4-fold higher than reported Ru SACs, respectively. This study provides mechanistic insights toward the roles of high-loading Ru SACs on sp- and sp2-hybridized carbonaceous substrates in selective hydrodehalogenation and hydrodearomatization.
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