ELECTROCHIMICA ACTA
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2018
·
IF 5.116
Zhengyi Qian,Baoyu Sun,Lei Du,Shuaifeng Lou,Chunyu Du,Pengjian Zuo,Yulin Ma,Xinqun Cheng,YunZhi Gao,Geping Yin
Since electrode surfaces primarily house the sites of oxygen reduction/evolution reactions, surface chemistry is pivotal for both charge and discharge processes of Li–O 2 batteries . Herein, we introduce oxygen-containing functional groups associated with defects on the carbon fiber papers (functionalization) via acid treatment and investigate their effects on the rechargeable nonaqueous Li–O 2 batteries. The discharge platform increases from 2.68 V to 2.79 V, meanwhile the decreased charge overpotential (a drop of 0.84 V) is also observed after functionalization. It is found that the discharge products formed on pristine carbon fiber exhibit a huge toroidal-like structure, in contrast to the porous flake clusters with much smaller size on the functionalized carbon fiber. On the other hand, the smaller product clusters are found to be much easier to be oxidized, leading to remarkably reduced charge overpotential. In this regard, the decomposition of electrolyte and corrosion of carbon cathode are dramatically alleviated, thus leading to greatly promoted cycling performance. All the experimental facts suggest that the oxygen functional groups associated with defects could provide tremendous active sites for the nucleation of discharge products and result in remarkably decreased overpotential for both the oxygen reduction and the oxygen evolution reaction in our cases.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2017
·
IF 3.359
Cheng Tan,Lei Li,Kongzhai Li,Dapeng Zhong
A novel method to separate As from high As-Sb dust using Fe 2 O 3 as a fixative under an O 2 -N 2 atmosphere is proposed. Here, Sb is oxidised and converted to Sb 2 O 4 and FeSbO 4 that remain in the roasted residue, and As is volatilized in the form of As 4 O 6 . The Sb 2 O 3 can be selectively oxidised from the dust by using 21 vol% O 2 , but the formation of amorphous substance (As-Sb-O) hinders the effective separation of As and Sb. Adding Fe 2 O 3 hinders the amorphous substance formation and destroys the structure of the solid solution ((Sb, As) 2 O 3 ) in the raw material by converting the Sb component in it to FeSbO 4 . Therefore, the volatilization rates of As and Sb can reach up to 90.53% and only 13.20%, respectively at a roasting temperature of 723 K, roasting time of 90 min, an Fe 2 O 3 dosage of 15 mass%, and O 2 content of 21 vol%.
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CHEMICAL ENGINEERING JOURNAL
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2017
·
IF 6.216
Ruxin Peng,Jihai Shao,Yuanlin Xie,Anwei Chen,Liang Peng,Qingru Zeng,Si Luo
Being that the influence of organic ligands on contaminant removal by nanoscale zero valent iron (nZVI) has been explored in quite a few studies, there is little information on reaction mechanisms of the ZVI-ligand system under different aeration conditions. The degradation of nitrobenzene (NB) by nZVI-oxalic acids (OA) was investigated under N 2 , O 2 and without aeration conditions. From the findings, it was evident that OA dramatically improved NB degradation by nZVI with all of the aeration conditions. Approximately 100% of NB was degraded by nZVI-OA+N 2 system after 60 min of reaction, followed in effectiveness by nZVI-OA+ without aeration (95%) as well as nZVI-OA+O 2 (85%). Operation parameters including OA concentration and pH had significant effect on the removal of NB in the nZVI-OA system. 3 mM OA concentration and pH 3.0 were found to be favourable. The Fe 2+ , total dissolved iron concentrations, pH and ORP values in the nZVI-OA systems had also been monitored. Intermediates and trapping experiments showed that reduction played a fundamental role in the NB degradation by nZVI-OA under N 2 or without aeration conditions. The formation of Fe(OA) 0 and Fe(OA) 2 2− complexes had lower standard ORP, which could improve the strength of reductant in the systems, and thus resulting in an increased degradation efficiency of NB by nZVI-OA+N 2 . Under O 2 aeration condition, the NB degradation process could be regarded as an oxidation . In the meantime, OA promoted the production of reactive oxidants species by speeding up the oxidation rates of Fe 2+ by O 2 and H 2 O 2 . Summarily, the improved reactivity of nZVI was largely as a result of the strong complexation ability of OA.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2017
·Vol. 164
·期 13
·G112
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IF 3.259
Yuchen Hui,Xiaoyan Ma,Fengjin Qu,Fang Chen,Ying Chen
A practical strategy is developed to fabricate stable glucose/O2 biofuel cells with high power density assembled by enzymatic bio-electrodes based on three-dimensional nickel foam. The porous three-dimensional nickel foam is used as a substrate to enhance the enzyme loading, while the reduced graphene oxide and gold nanoparticles decorating on the nickel foam are employed as the direct electron transfer system for bio-anodes and bio-cathodes. The ferrocenecarboxylic acid serves for the mediated electron transfer to further increase electron transfer rate for glucose oxidase electrodes. Covalent bond is employed to immobilize the mediator and enzymes for improving the stability of bio-electrodes and biofuel cells. As the results, the surface glucose oxidase loading reaches to 4.03 × 10−7 mol cm−2 with good enzymatic activity. Additionally, the obtained glucose/O2 biofuel cells exhibit an outstanding maximum power density of 2.84 ± 0.09 mW cm−2, with a remarkable long-term operational stability for retaining 85.5% of its performance after 70 days. In human blood, the biofuel cell shows a favorable output performance of 0.39 ± 0.04 mW cm−2, implying the appropriateness for practical applications.
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Bioactive Materials
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2024
·
IF 18
Changjiang Liu,Kun Liu,Dong Zhang,Yuting Liu,Yifeng Yu,Haifei Kang,Xianzhen Dong,Honglian Dai,Aixi Yu
Diabetic wounds present multiple functional impairments, including neurovascular dysregulation, oxidative imbalance, and immune dysfunction, making wound healing particularly challenging, while traditional therapeutical strategies fail to address these complex issues effectively. Herein, we propose a strategy utilizing dual-layer microneedles to deliver therapeutic gases by modulating neurovascular coupling and immune functions for diabetic wound treatment. The microneedle can respond to reactive oxygen species (ROS) in the diabetic microenvironment and subsequently generate oxygen (O 2 ) and nitric oxide (NO). These gases comprehensively promote neuro-vascular regeneration, reduce oxidative stress levels, and attenuate inflammation. In vivo studies demonstrate that the microneedle can accelerate diabetic wound healing by modulating neurovascular regeneration and inflammatory processes. Transcriptomic analyses further validate the involvement of related advantageous signaling pathways. The potential mechanism involves the activation of the PI3K-AKT-mTOR pathway to facilitate autophagy, ultimately accelerating the healing process. Thus, our multifunctional dual-layer microneedles provide an effective strategy for treating diabetic wounds.
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PubMed
高影响因子
JOURNAL OF MATERIALS ENGINEERING AND PERFORMANCE
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2025
·
IF 2
Zhang Dongbo,Tang Xinyue,Wang Ning,Xiao Mingwei,Yan Jiangrong,Zhang Yongsheng
High-entropy oxides used as thermal barrier coating materials have attracted considerable attention from scientific communities owing to their unique properties, such as low thermal conductivity and good stability at high temperatures. In this study, a new (La 0.2 Gd 0.2 Zr 0.2 Ce 0.2 Ho 0.2 )O 2-δ ((LGZCH)O) fluorite-structured high-entropy oxide was successfully synthesized through a solid-state reaction at 1400 °C. The resulting material demonstrated good phase stability after sintering at high temperatures. The microstructure, microscopic morphology, ionic valence, compositional distribution, optical properties, thermal conductivity, thermal expansion properties, and mechanical properties of (LGZCH)O were investigated. X-ray diffraction results showed that the (LGZCH)O fluorite-structured high-entropy oxide exhibited good stability during sintering at different temperatures with an optimum sintering temperature of 1580 °C. Ce 4+ converted to Ce 3+ at high temperatures. Scanning electron microscopy results showed that the material had a high porosity of approximately 28.9% after sintering at 1580 °C. (LGZCH)O had a higher infrared radiation emissivity of 82.2%-87.6% in the range of 2.5-6.0 μm indicating that it had better thermal radiation shielding performance. After porosity modification, the thermal conductivity ranged from 1.27 to 1.00 W m −1 K −1 from room temperature to 1000 °C, which is considerably lower than that of yttria-stabilized zirconia. Additionally, (LGZCH)O exhibited low coefficients of thermal expansion measuring 9.65 × 10 −6 K −1 and 10.13 × 10 −6 K −1 at 1000 and 1200 °C, respectively. The hardness and Young’s modulus of the bulk (LGZCH)O measured via nanoindentation tests were 8.86 GPa and 153.98 GPa, respectively, which are marginally inferior to those of YSZ. Therefore, (LGZCH)O can be considered a promising candidate material for thermal barrier coatings.
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FUEL PROCESSING TECHNOLOGY
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2018
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IF 3.956
Ting Lu,Yucui Hou,Weize Wu,Muge Niu,Wei Li,Shuhang Ren
Carboxylic acids are considered as an important group of chemicals. Direct conversion of cellulose to formic acid (FA) by vanadium(V(V))-contained catalyst is of significant conceptual and practical interest. A second metal (from Mg(II), Ca(II), Al(III), Cr(III), Mo(VI), Mn(II), Cu(II), or Fe(III)) incorporated into V(V)-contained catalyst system was screened to further improve the oxidation of cellulose by O 2 to yield FA. Fe(III) exhibited the best performance and effects of reaction parameters on the conversion of cellulose in NaVO 3 -FeCl 3 -H 2 SO 4 aqueous solution were investigated. Cellulose could be rapidly converted, and the yield of FA (66.8%) was higher than that obtained by the single use of FeCl 3 (48.4%) or NaVO 3 (57.6%). The conversion of cellulose in another V(V)-contained catalyst system (H 5 PV 2 Mo 10 O 40 ) was explored to verify the universal enhancement of FeCl 3 . Influences of the second metal Fe(III) on the V(V)-contained catalyst system and mechanism of cellulose oxidation in the V(V)-Fe(III)-H 2 SO 4 system were studied. Compared with single use of V(V), the employment of Fe(III) alone is not active enough in the oxidative C C bond cleavage . V(V) other than Fe(III) is the main active species for selective oxidation of substrates. The incorporation of Fe(III) and V(V) shows both synergistic and competitive relationships. Both the synergistic and competitive effects are beneficial to increase FA yield, as they promote the oxidation of V(IV) to V(V), increase oxidative ability, and inhibit the overoxidation to by-product CO 2 . The catalyst system was reused four times without decline in activity.
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Polymer Chemistry
·
2018
·Vol. 9
·期 9
·1095-1108
·
IF 4.927
Xiaoqi Zhao,Wentao Wu,Jian Zhang,Wenxue Dai,Youliang Zhao
Multicomponent miktoarm stars with multifunctional Y junctions may provide us with new insights into their physicochemical properties and prospective applications. Considering the unique role of a gas stimulus in smart materials and the promising gradient-type properties induced by combined stimuli, this study aims at the synthesis, thermoresponsive and self-assembly behaviors of an O2-, redox-, thermo-, and pH-responsive 3-miktoarm star quarterpolymer. A robust method involving controlled polymerization, amine–thiol–ene conjugation and hydrolysis was developed to achieve a poly(N-isopropylacrylamide-co-4-(2-(2,2,2-trifluoroethylcarbamoyl)ethylthio)-2-(acrylamido)-N-(2-hydroxyethyl)butanamide)-arm-poly(ε-caprolactone)-arm-poly(acrylic acid) star. Owing to the changes in amphiphilicity, chemical composition and mutual interactions, a single stimulus or various stimuli combinations could lead to switchable LCSTs and morphological transformations. Upon increasing pH, O2 treatment and oxidation, the copolymer solution was liable to exhibit enhanced LCST due to the improved hydrophilicity. The star quarterpolymer could self-assemble into multicompartment vesicles (pH 3.0), vesicles (pH 5.9) and small micelle/vesicle mixtures (pH 10) at ambient temperature. Upon thermo, redox and O2 stimuli, the assemblies formed at different pHs could be further converted into some other morphologies such as compound micelles and nanocapsules with hollow caves. Our research affords a general route to synthesize MMSs with tailored Y junctions, and the combination of the O2 stimulus with other stimuli may potentially expand the scope of multi-triggered properties and applications of star copolymers.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 10
·4485-4493
·
IF 9.931
Lingyou Zeng,Kaian Sun,Zhichao Yang,Shengli Xie,Yanju Chen,Zhi Liu,Yaqing Liu,Jinchong Zhao,Yunqi Liu,Chenguang Liu
Three-dimensional (3D) nanomaterials have received significant attention for large-scale functional applications due to their large specific surface areas as well as desired electrical, physicochemical, and catalytic properties. Herein, we present a facile and effective synthetic route for in situ grown 3D hierarchical Ni3S2 superstructures (rod-like arrays and nanoforest patterns) on nickel foam. This handy strategy endows the Ni3S2 superstructures with large surface active areas, porosity, and macro-/mesoporous structures. We have shown that these materials can serve as highly active, binder-free, bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Moreover, these materials were found to provide a ∼100% faradaic yield towards both HER and OER and exhibit remarkable catalytic stability (for >50 h).
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Surfaces and Interfaces
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2024
·
IF 5.7
Xinru Wang,Qiuxu Chen,Daming Yang,Ying Li,Dongxu Yin,Baoxin Ni,Wei Lu,Guiru Sun,Ming Feng
Photo-assisted electrochemical strategy has garnered interest for its ability to diminish the large overpotential of lithium-oxygen batteries (LOBs). Nonetheless, creating a sophisticated photocatalyst capable of absorbing a wide spectrum of light and dramatically lowering the recombination rate for electron-hole pairs presents a significant challenge. Herein, we design an Ag-doped ZnO (Ag@ZnO) hollow nanosphere as photocatalysts to boost the reaction dynamics of photo-assisted LOBs. The Ag@ZnO hollow nanospheres, featuring a mesoporous structure, are beneficial for improving O 2 transport and enabling the retention of discharge products. Additionally, the ability to absorb light and the efficiencies of electron-hole separation are enhanced for Ag@ZnO as a result of Ag doping. The electrons generated by photoexcitation facilitate the conversion of O 2 to produce Li 2 O 2 during discharge, whereas during charging, the presence of holes causes the decomposition of Li 2 O 2 . Consequently, a significantly low overpotential of 0.22 V, ultrahigh cycling efficiency of 93.73%, and good reversibility was achieved for the photo-assisted LOBs using Ag@ZnO. We consider that this work can offer a reliable strategy to improve electrochemical kinetics and contribute to the development of efficient photocatalysts for photo-assisted LOBs.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
·
IF 3.8
Yu-Zhen Xu,Yu-Le Wang,Yu-Dong Shan,Song-Hai Wu,Yong Liu,Xu Han
Selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) by O2 under solvent- and initiator-free conditions is a challenge in chemical processes, which is still constrained by its low selectivity (theoretical selectivity of 50.0%). Given the low epoxide selectivity (<20.0%) of single metal catalysts, we propose a relay catalysis strategy on the oxidation of Cy to Cy-ep with high selectivity by the spherical Mg–Mo bimetallic oxide (MMO). Such a relay catalyst exhibits a desirable Cy conversion of 31.0% and a high selectivity of 49.3% toward Cy-ep. Meanwhile, the high stability and reusability of MMO also indicate its potential to be used for industrial scale-ups. A series of characterizations and DFT calculations reveal that the negatively charged lattice oxygen in [MgII–O–II] adsorbs allylic H of Cy to weaken the bond energy of the allylic C–H bond and form Cy•, and then Cy• rapidly traps O2 to give CyOO•, which subsequently abstracts H from allylic C–H of another Cy to form 2-cyclohexene-1-hydroperoxide (Cy-OOH) and Cy•, achieving the propagation cycle. On the other hand, the Mo(VI) site in MMO catalyzes the produced Cy-OOH peroxo, which then oxidizes Cy to Cy-ep and 2-cyclohexene-1-ol. This work provides insight into the relay catalyst for the epoxidation of olefin with O2 with high selectivity under solvent- and initiator-free conditions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
·
IF 3.8
Bingbing He,Qinyuan Wang,Ying Chen,Weifeng Yao
The development of a cost-effective method for synthesizing hydrogen peroxide (H2O2) holds significant importance. Here, we introduce a novel catalyst, a nitrogen-doped carbon-loaded nickel nanoparticle catalyst (Nix NPs@N–C), tailored for efficient H2O2 production via the two-electron oxygen reduction reaction. Benefiting from the synergistic interplay between highly active nickel nanoparticles and nitrogen-doped carbon, the optimal Nix NPs@N–C catalyst demonstrates an outstanding 78% selectivity for H2O2 at 0.5 V vs a reversible hydrogen electrode (RHE), yielding approximately 387 mmol g–1 h–1 in a 0.1 M KOH alkaline solution at 0.3 V vs RHE. With its utilization of cost-effective raw materials, streamlined synthesis method, and exceptional catalytic performance, the Nix NPs@N–C catalyst emerges as a promising candidate for electrocatalytic H2O2 synthesis in practical applications.
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