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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
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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
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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
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FUEL · 2023 · IF 7.4

“On-off”controlled H2 evolution and O2 evolution upon NH3BH3 hydrolysis resp·H2O2 decomposition on Pt/ZIF-67

Qi Rong,Wenkai Huang,Fuhua Xu,Yanlan Wang,Changlong Wang,Xiang Liu

In spite of significant developments are accomplished in the exploration of H 2 and O 2 evolution upon water electrolysis/photolysis, this remains a challenge to design and develop ideal catalytic systems for this reaction and to isolate H 2 from H 2 -O 2 mixture with membranes. Herein, a series of ZIF-67-supported transition metal nanoparticles (TMNPs/ZIF-67), including Pt, Ir, Pd, Rh, Au and Ag, via immobilization of ultrafine TMNPs at the surface of ZIF-67, have been designed and developed for the selective H 2 generation from NH 3 BH 3 hydrolysis and O 2 evolution upon H 2 O 2 decomposition. In particular, the optimized nanocatalyst Pt/ZIF-67 presents the super-high catalytic property in the both H 2 evolution upon NH 3 BH 3 hydrolysis (689 mol(H 2 )·mol Pt -1 ·min −1 ) and O 2 evolution upon H 2 O 2 decomposition (979 mol(O 2 )·mol Pt -1 ·min −1) at 30 °C. Importantly, the selective “on–off” control for demand-based H 2 generation from NH 3 BH 3 hydrolysis was successfully realized by Zn 2+ /EDTA-2Na system. This highly efficient Pt/ZIF-67 proposed a new method for the promising potential application of ammonia borane and hydrogen peroxide as an economic and safe H 2 resp. O 2 carrier for fuel cell.

CAS / MDL: 13774-81-7 13454-96-1
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2023 · IF 5.8

Multifunctional barrier membranes promote bone regeneration by scavenging H2O2, generating O2, eliminating inflammation, and regulating immune response

Shuo Liu,Huiqi Yang,Liguo Zhang,Alberto Bianco,Baojin Ma,Shaohua Ge

The injured bone microenvironment is typically characterized by high-level reactive oxygen species (ROS, mainly H 2 O 2 ) and low content of oxygen. The former can cause cell apoptosis, induce immune imbalance and inflammation, inhibit osteogenic differentiation, and delay bone repair . In this work, barrier membranes made of a combination of hydroxyapatite nanowires (HAp NWs) and polylactic acid (PLA) loaded with manganese dioxide nanosheets (NSs) ( [email protected] ) were prepared to guide bone regeneration (GBR). Due to the catalytic function of MnO 2 , [email protected] membranes are able to effectively decompose H 2 O 2 to generate O 2 . In vitro experiments demonstrated [email protected] membranes inhibited the apoptotic process caused by high level of H 2 O 2 , decreased intracellular oxidative stress , suppressed inflammation-related gene/protein expression, and inhibited macrophage M1 polarization. The nanostructured HAp stimulated osteogenic differentiation, and the loading of MnO 2 NSs played a synergistic effect. In addition, the barrier function of PLA could hamper the epithelium overgrowth, providing the development space for periodontal regeneration. By scavenging H 2 O 2 , generating O 2 , eliminating inflammation, and regulating immune response, [email protected] membranes efficiently promoted bone regeneration. Our results confirmed that composite membranes have great potential for application in GBR, and provide a reference for future design of bone repair materials.

CAS / MDL: 7722-64-7
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Oxygen-rich hierarchical activated coke-based gas diffusion electrode enables highly efficient H2O2 synthesis via O2 electroreduction

Wei Zhou,Liang Xie,Yan Wang,Yani Ding,Xiaoxiao Meng,Fei Sun,Jihui Gao,Guangbo Zhao

Large-scale application of H 2 O 2 production through 2-electron oxygen reduction reaction (2eORR) greatly depends on the cost of electrode materials and configuration. In this work, engineered coal-derived oxygen-rich hierarchical activated coke (AC), which is low-cost and highly tunable in porosity and surface chemistry, was used as catalyst to fabricate gas diffusion electrodes (GDEs) for efficient H 2 O 2 production. Results showed that Fenton’s reagents treatment could significantly increase the contents of C O and –COOH on AC, leading to an increased hydrophilicity. However, the higher O contents do not necessarily enhance the selectivity of AC towards 2eORR (i.e., F-5-AC, F-10-AC), especially that F-20-AC exhibited a complete 4e pathway. GDEs were then fabricated with AC and oxidized AC as catalyst, key fabrication parameters including the PTFE binder and AC particle size, and operating parameters such as current intensity, electrolyte pH, and O 2 flow rate were optimized. Up to 747 mg/L H 2 O 2 were generated within 90 min. Results showed that oxidized AC exhibited a decreased H 2 O 2 yield, due to the flooding of GDEs caused by super-hydrophilicity property. Finally, DFT calculations were employed to reveal the synergistic effect of different O groups considering the fact of high O contents on AC.

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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.

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Small · 2022 ·Vol. 18 ·期 23 ·2200548 · IF 15.153

Au3+-Functionalized UiO-67 Metal-Organic Framework Nanoparticles: O2•− and •OH Generating Nanozymes and Their Antibacterial Functions

Meng-Meng Pan,Yu Ouyang,Yong-Li Song,Lu-Qin Si,Ming Jiang,Xu Yu,Li Xu,Itamar Willner

The synthesis and characterization of Au 3+ -modified UiO-67 metal-organic framework nanoparticles, Au 3+ -NMOFs, are described. The Au 3+ -NMOFs reveal dual oxidase-like and peroxidase-like activities and act as an active catalyst for the catalyzed generation of O 2 •− under aerobic conditions or •OH in the presence of H 2 O 2 . The two reactive oxygen species (ROS) agents O 2 •− and •OH are cooperatively formed by Au 3+ -NMOFs under aerobic conditions, and in the presence of H 2 O 2. The Au 3+ -NMOFs are applied as an effective catalyst for the generation ROS agents for antibacterial and wound healing applications. Effective antibacterial cell death and inhibition of cell proliferation of Staphylococcus aureus ( S. aureus ) and Escherichia coli ( E . coli ) bacterial colonies are demonstrated in the presence of the Au 3+ -NMOFs. In addition, in vivo experiments demonstrate effective wound healing of mice wounds infected by S. aureus , treated by the Au 3+ -NMOFs.

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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.

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CHEMOSPHERE · 2021 · IF 7.086

Janus graphite felt cathode dramatically enhance the H2O2 yield from O2 electroreduction by the hydrophilicity-hydrophobicity regulation

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

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
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Pd–O2 interaction and singlet oxygen formation in a novel reactive electrochemical membrane for ultrafast sulfamethoxazole oxidation

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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