CHEMOSPHERE
·
2021
·
IF 7.086
Wei Zhou,Xiaoxiao Meng,Jihui Gao,Fei Sun,Guangbo Zhao
s Hydrogen peroxide (H 2 O 2 ) electrosynthesis from 2-electron O 2 reduction reaction (2eORR) is widely regarded as a promising alternative to the current industry-dominant anthraquinone process. Design and fabrication of effective, low-cost carbon-based electrodes is one of the priorities. Many previous work well confirmed that hydrophilic carbon-based electrodes are preferable for 2eORR. Here, we proposed a strategy of hydrophilicity-hydrophobicity regulation. By using commercially available graphite felt (GF) as electrodes, we showed that both hydrophilic GF, hydrophobic GF, and Janus GF yielded significantly higher H 2 O 2 production, which is 7.3 times, 7.6 times, and 7.7 times higher than the original GF, respectively. Results showed that currents and stirring rates affect the H 2 O 2 yields. The enhancement of hydrophilic GF is due to the incorporation of oxygen-containing functional groups, while the hydrophobic and Janus GF comes from the locally confined O 2 bubbles, which built a gas-liquid-solid interface inside GF and thus enhance the H 2 O 2 formation kinetics. Finally, the effectiveness of the hydrophilicity-hydrophobicity regulation concept was tested in Electro-Fenton process by removing typical dyes and antibiotics. This work supply an effective but facile strategy to enhance the performance of carbon-based electrodes towards 2eORR by regulating the micro-environment of electrodes.
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ACS Omega
·
2021
·
IF 3.512
Shuangping Xu,Wenqiang Ma,Hailiang Zhou,Yushu Zhang,Hongge Jia,Jingyu Xu,Pengfei Jiang,Xintian Wang,Wenwen Zhao
The synthesis of poly(methyhydrosiloxane) (PMHS) and N,N′-bis(3-allyl)pyromellitic diimide was optimized for O2/N2 separation. The membrane exhibits excellent mechanical and thermal properties and shows an O2/N2 selectivity of up to 4.44 with an O2 permeability of 31.0 Barrer; compared with polydimethylsiloxane (PDMS) and pure polyimide (PI) membranes, the separation selectivity shows a 107% increase for PDMS, and the permeation shows a 660% increase for pure PI. The obtained results were well above the ones reported on the literature for similar conditions opening the door for the preparation of a stable polysiloxane (PMHS-I) gas separation membrane with extraordinary O2/N2 separation performance.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Lehui Ren,Mei Chen,Jinxing Ma,Yang Li,Zhiwei Wang
In this study, a novel reactive electrochemical membrane (REM) made of Pd-loaded porous Ti was prepared to achieve ultrafast and efficient oxidation of trace antibiotics sulfamethoxazole (SMX) under anodic polarization. At a current density of 0.5 mA/cm 2 , the percentage removal of SMX by the REM was 96.3% in flow-through mode, with the energy cost ( i.e. , the electrical energy per order of removal, 1.34 Wh/m 3 ) being much lower than the flow-by mode (125.76 Wh/m 3 ) under the same operating condition. Quenching experiments and electron spin resonance spectra demonstrated that singlet oxygen ( 1 O 2 ) was the main reactive oxygen species in the REM system, playing a vital role in SMX degradation. Results of this study indicated that 1 O 2 was mainly generated on the anode via Pd–O 2 interaction that directly activated oxygen, rather than the evolution of 1 O 2 precursors ( e.g ., O 2 − and H 2 O 2 ). The constantly high electrochemical removal of SMX (88.5–91.9%) from actual surface water demonstrated that the matrix effect on the process performance was minimal in realistic applications, highlighting this novel REM to be a viable way to remove trace organic contaminants from surface water.
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ACS Catalysis
·
2020
·
IF 12.35
Mo Zhang,Zheng Li,Xing Xin,Junhao Zhang,Yeqin Feng,Hongjin Lv
Selective production of value-added platform chemicals from renewable biomass feedstocks and their derivatives has attracted tremendous attention with high potential in addressing global problems of energy and sustainability. In this work, a lead-halide perovskite (MAPbBr3, MA = methylammonium) is utilized as a photocatalyst for selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) using atmospheric O2 upon visible-light irradiation. Under minimally optimized conditions, the photocatalytic conversion of HMF in acetonitrile solvent reaches 100% with a DFF selectivity of over 90%, achieving an overall furanic carbon yield of over 96%. A detailed catalytic mechanism was proposed based on various spectroscopic and experimental results, revealing that the atmospheric O2, photogenerated electrons (e–), holes (h+), •O2–, and 1O2 species together play crucial roles in the effective and selective photo-oxidation of HMF to DFF. In addition, our present photocatalytic system is also applicable for photo-oxidation of benzyl alcohol with approximately 100% conversion and benzaldehyde selectivity, providing insights for future exploration of the present catalytic system.
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ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Mingjie Sun,Shuai Guo,Ziling Wang,Lu Zou,Bo Chi,Jian Pu,Jian Li
It is crucial to design effective cathode catalysts for high performance of Li–O 2 batteries (LOBs). Herein, porous LaCo 0.6 Ni 0.4 O 3 nanofibers decorated with ultrafine Co 3 O 4 nanoparticles (Co 3 O 4 @LCN NFs) are designed and employed as cathode catalyst for LOBs. The X-ray photoelectron spectroscopy measurement results suggested that uniform dispreading of Co 3 O 4 nanoparticles on LCN NFs surface could largely increase the surface chemisorbed oxygen, resulting in enhanced catalytic activity. Furthermore, with the assistance of Co 3 O 4 nanoparticles, Co 3 O 4 @LCN NFs can significantly facilitate O 2 adsorption and diffusion, Li 2 O 2 nucleation/decomposition and the formation of tiny sheet-like Li 2 O 2 , thereby achieving a low charge overpotential. A high specific capacity of 11,288 mA h g −1 , a low charge voltage plateau of 3.72 V at first cycle and excellent cycle stability of 116 cycles at 1000 mA g −1 are obtained for LOBs with Co 3 O 4 @LCN NFs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Yanbin Wang,Di Meng,Xu Zhao
Visible-light-driven H 2 O 2 production from O 2 reduction is an eco-friendly strategy and attracts increasing attentions. In this study, KOH modified graphitic carbon nitrides (CNKx) were constructed through the thermolysis of melamine-cyanuric acid supramolecular-complex in the presence of KOH. The BET specific surface area of CNK 0.2 with porous structure was 92 m 2 g −1 . The photocatalyst was characterized by XPS, ESR and element analysis and the analysis suggested that nitrogen vacancy was created in the framework of g-C 3 N 4 . Photoluminescence (PL) spectra indicated that the recombination of photogenerated electrons and holes was efficiently suppressed. ζ-potential revealed that more negative charge on the surface of CNK 0.2 , which promoted the adsorption of O 2 and accelerated the photocatalytic H 2 O 2 production. ESR experimental and radical quenching results illustrated that superoxide radical (O 2 - ) was the primary intermediate during the O 2 reduction process, suggesting the O 2 reduction pathway by CNK 0.2 was the sequential two-step single-electron reduction.
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Journal of Materials Chemistry A
·
2019
·Vol. 8
·期 1
·259-267
·
IF 10.733
Congcong Dang,Yu Wang,Biao He,Weibin Zhang,Feng Dang,Hongchao Wang,Yong Du
Searching for highly efficient and low cost electrocatalysts is an urgent challenge to provide high capacity and long cycle life Li–O2 batteries (LOBs). In this work, the highly efficient electrocatalytic properties of MoSi2 were first demonstrated using particles prepared by a solid–state reaction method. The surface was activated, playing a dominant role in the electrocatalytic performance. After acid etching to remove SiO2 impurities arising from the surface oxidation, MoSi2 exhibited excellent bifunctional electrocatalytic properties for LOBs. Mo6+ on the surface contributed to the initial low overpotentials of 0.45 V (3.2 V for the OER and 2.75 V for the ORR) and transformed into Mo4+ for a long cycle life. As a consequence, outstanding rate capabilities of 12 708 mA h g−1 at 100 mA g−1 and 10 794 mA h g−1 at 800 mA g−1, and excellent cycle durability of 215 and 90 cycles at a limited capacity of 1000 mA h g−1 at 200 and 500 mA g−1, respectively, were obtained for the MoSi2 cathode.
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Surfaces and Interfaces
·
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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CHEMICAL ENGINEERING JOURNAL
·
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
·
2017
·Vol. 164
·期 13
·G112
·
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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JOURNAL OF MATERIALS ENGINEERING AND PERFORMANCE
·
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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Bioactive Materials
·
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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