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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 10 ·4485-4493 · IF 9.931

Tunable 3D hierarchical Ni3S2 superstructures as efficient and stable bifunctional electrocatalysts for both H2 and O2 generation

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).

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 电化学
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Polymer Chemistry · 2018 ·Vol. 9 ·期 9 ·1095-1108 · IF 4.927

Thermoresponse and self-assembly of an ABC star quarterpolymer with O2 and redox dual-responsive Y junctions

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.

CAS / MDL: 814-68-6 6038-19-3
研究领域: 高分子化学 · 材料科学
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RSC Advances · 2019 ·Vol. 9 ·期 29 ·16288-16295 · IF 3.049

Metal–organic framework derived hollow porous CuO–CuCo2O4 dodecahedrons as a cathode catalyst for Li–O2 batteries

Shu-ying Zhen,Hai-tao Wu,Yan Wang,Na Li,Hao-sen Chen,Wei-li Song,Zhen-hua Wang,Wang Sun,Ke-ning Sun

Herein, hollow porous CuO–CuCo2O4 dodecahedrons are synthesized by using a simple self-sacrificial metal–organic framework (MOF) template, which resulted in dodecahedron morphology with hierarchically porous architecture. When evaluated as a cathodic electrocatalyst in lithium–oxygen batteries, the CuO–CuCo2O4 composite exhibits a significantly enhanced electrochemical performance, delivering an initial capacity of 6844 mA h g−1 with a remarkably decreased discharge/charge overpotential to 1.15 V (vs. Li/Li+) at a current density of 100 mA g−1 and showing excellent cyclic stability up to 111 charge/discharge cycles under a cut-off capacity of 1000 mA h g−1 at 400 mA g−1. The outstanding electrochemical performance of CuO–CuCo2O4 composite can be owing to the intrinsic catalytic activity, unique porous structure and the presence of substantial electrocatalytic sites. The ex situ XRD and SEM are also carried out to reveal the charge/discharge behavior and demonstrate the excellent reversibility of the CuO–CuCo2O4 based electrode.

研究领域: 材料科学 · 电化学
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ACS Omega · 2021 · IF 3.512

A Novel Imide-Bridged Polysiloxane Membrane Was Prepared via One-Pot Hydrosilylation Reaction for O2/N2 Separation

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.

CAS / MDL: 89-32-7 30551-89-4
研究领域: 材料科学 · 化学工程 · 膜技术 · 气体分离
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

Novel and highly efficient catalyst for Li–O2 battery: Porous LaCo0.6Ni0.4O3 nanofibers decorated with ultrafine Co3O4 nanoparticles

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.

研究领域: 材料科学 · 电化学
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ACS Catalysis · 2020 · IF 12.35

Selective Valorization of 5-Hydroxymethylfurfural to 2,5-Diformylfuran Using Atmospheric O2 and MAPbBr3 Perovskite under Visible Light

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.

研究领域: 化学工程 · 可再生能源 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Multifunctional hydrogel platform for biofilm scavenging and O2 generating with photothermal effect on diabetic chronic wound healing

Qian Wang,Weiwang Qiu,Mengna Li,Na Li,Xiaoran Li,Xiaohong Qin,Xueli Wang,Jianyong Yu,Faxue Li,Liqian Huang,Dequn Wu

Diabetic wound treatment remains a major challenge due to the difficulties of eliminating bacterial biofilm and relieving wound hypoxia . To address these issues simultaneously, a multifunctional Dex-SA-AEMA/MnO 2 /PDA (DSAMP) hydrogel platform was developed with excellent biocompatibility and porous structure. The hydrogel could absorb the exudate, maintain humidity and permeate oxygen, which was prepared by encapsulating polydopamine (PDA) and manganese dioxide (MnO 2 ) into Dex-SA-AEMA (DSA) hydrogel by UV irradiation . With the addition of PDA , the DSAMP hydrogel was proved to eliminate the biofilm after NIR photodynamic therapy (PTT, 808 nm) irradiation at 54 °C. Furthermore, in order to mitigate hypoxia wound microenvironment, MnO 2 nanoparticles were added to convert the endogenous hydrogen peroxide (H 2 O 2 ) into oxygen (O 2 , 16 mg L −1 ). The diabetic wound in vivo treated by DSAMP hydrogel was completely healed on 14 days. It was revealed that the DSAMP hydrogel possessed a great potential as dressing for diabetic chronic wound healing.

研究领域: 生物医学工程 · 伤口愈合研究 · 纳米医学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Oxalate-enhanced reactivity of nanoscale zero-valent iron under different conditions of O2, N2 or without aeration

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.

研究领域: 环境科学 · 化学
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Insights into the role of oxygen functional groups and defects in the rechargeable nonaqueous Li–O2 batteries

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.

CAS / MDL: 90076-65-6 67-68-5
研究领域: 材料科学 · 电化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2017 ·Vol. 164 ·期 13 ·G112 · IF 3.259

Three-Dimensional Nickel Foam Based Enzymatic Electrode and Its Glucose/O2 Biofuel Cell with High Power Density

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.

研究领域: 生物化学 · 材料科学 · 能源技术
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SEPARATION AND PURIFICATION TECHNOLOGY · 2017 · IF 3.359

Separation of As from high As-Sb dust using Fe2O3 as a fixative under O2-N2 atmosphere

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%.

CAS / MDL: 1309-37-1 20344-49-4
研究领域: 冶金学 · 环境科学
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BIOELECTROCHEMISTRY · 2022 · IF 5.76

Involvement of O2·− release in zearalenone-induced hormesis of intestinal porcine enterocytes: An electrochemical sensor-based analysis

Yanjing Yun,Zhisong Lu,Xiaodan Jiao,Peng Xue,Wei Sun,Yan Qiao,Yang Liu

Relationship between mycotoxin-induced hormesis and reactive oxygen species (ROS) has not been systematically investigated due to the lack of an effective analysis method. To monitor cellular release and intracellular level of O 2 ·− , carboxymethyl cellulose-Mn 3 (PO 4 ) 2 nanocomposite was synthesized to fabricate an electrochemical biosensor, which selectively detects O 2 ·− over the range of 57.50 nM ∼ 2.95 μM (R 2  = 0.99) with the sensitivity of 78.67 μA μM −1 cm −2 and the detection limit of 8.47 nM. Transient exposure to zearalenone (ZEA) induces the enhancement on cell viability, immediate O 2 ·− release from cells, and reduction of intracellular O 2 ·− level. After post-treatment culture, intracellular O 2 ·− initially increases to a high level and then decreases to the normal level. Concurrently, the ZEA-induced hormesis disappears. Based on the findings, we propose a mechanism, involving the ROS release, increase of succinate dehydrogenase activity and recovery of intracellular ROS, to explain the occurrence and disappearance of hormesis in intestinal porcine enterocytes.

研究领域: 毒理学 · 分析化学 · 细胞生物学
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