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Journal of Materials Chemistry A · 2019 ·Vol. 8 ·期 1 ·259-267 · IF 10.733

Novel MoSi2 catalysts featuring surface activation as highly efficient cathode materials for long-life Li–O2 batteries

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.

CAS / MDL: 18868-43-4
研究领域: 材料科学 · 电化学 · 能源存储
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Visible-light-driven H2O2 production from O2 reduction with nitrogen vacancy-rich and porous graphitic carbon nitride

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.

CAS / MDL: 3317-61-1
研究领域: 材料科学 · 环境科学 · 光催化
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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.

研究领域: 材料科学 · 生物医学工程 · 微生物学
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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.

研究领域: 材料科学 · 电化学 · 环境工程
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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.

研究领域: 环境科学 · 电化学工程 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

PIM-1 mixed matrix membranes incorporated with magnetic responsive cobalt-based ionic liquid for O2/N2 separation

Hongyong Zhao,Ting Song,Xiaoli Ding,Ruyi Cai,Xiaoyao Tan,Yuzhong Zhang

Membrane technology for O 2 /N 2 separation is a mature industrial unit. Membranes with excellent permeation-separation performance are still one of the critical requirements. The cobalt-based compounds have been well known for their good affinity for O 2 , which can facilitate O 2 transfer and improve the O 2 /N 2 selectivity in membranes. The cobalt-based compounds, moreover, have a magnetic responsive effect, which can lead to a further improvement in O 2 /N 2 separation under a magnetic field. A class of PIM-1 mixed matrix membranes (MMMs), containing cobalt-based ionic liquid (CILs)@polyarylate (aromatic polyester) (PAR) (core-shell) composite nanospheres (CILs@PAR (c-s) CNPs), were prepared. Chemical compositions of CILs@PAR (core-shell) CNPs were determined by Fourier transform infrared spectroscopy (FTIR). Morphologies and structures of CILs@PAR (core-shell) CNPs were observed by transmission electron microscopy (TEM). Gas adsorption properties of CILs@PAR (core-shell) CNPs were tested. Thermal properties of the (CILs@PAR (c-s) CNPs)/PIM MMMs were investigated by simultaneous thermal analysis (TGA-DSC). Gas permeation-separation performances of the (CILs@PAR (c-s) CNPs)/PIM MMMs were also reported. Compared with the original PIM-1 membrane, the (CILs@PAR (c-s) CNPs)/PIM MMMs display higher O 2 /N 2 selectivity because of cobalt-based ionic liquid as O 2 carrier, coupled with a reduction in O 2 permeability. With increasing the content of the CILs@PAR (c-s) CNPs, the O 2 /N 2 selectivity increases, and the O 2 permeability decreases. It is also found that, as a magnetic field on the MMMs, the O 2 /N 2 selectivity further increases; and it increases more, as a higher content of CILs@PAR (c-s) CNPs. Therefore, the (CILs@PAR (c-s) CNPs)/PIM MMMs exhibit excellent O 2 /N 2 selectivity of ∼5 coupled with good O 2 permeability of ∼140 Barrer under a 180 mT magnetic field and show great potential for air separation.

CAS / MDL: 554-95-0
研究领域: 材料科学 · 化学工程 · 分离技术
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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
研究领域: 化学催化 · 燃料电池材料 · 纳米材料
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2023 · IF 4.5

Co nanoparticles embedded into leaf-like porous carbon as a promising cathode catalyst for Li-O2 batteries

Chaoyang Sun,Fenglong Xiao,Di Wu,Gang Lian,Deliang Cui,Qilong Wang,Haohai Yu

Rechargeable Li-O 2 batteries show great potential due to their superior high energy density. However, the practical application is still limited by the sluggish kinetics, resulting in poor cycling performance and high overpotentials. Herein, highly dispersed Co nanoparticles embedded into porous N -doped carbon matrix (DCo-NC) with carbon nanotubes is explored through the pyrolysis of a bimetallic leaf-shaped ZnCo-ZIFs. The evaporation of Zn species and porous carbon matrix derived from ZIFs prevents the Co nanoparticles aggregation, exposes more Co-N active sites and provides abundant pores. They facilitate Li + and electron transfer, prevent Co nanoparticles from deactivation and provide enough space for Li 2 O 2 , thereby accelerating oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) kinetics. Accordingly, the Li-O 2 batteries with DCo-NC cathode exhibit reduced overpotential, high discharge capacity (10,490 mA h g −1 at 100 mA g −1 current density) and improved cycling performance (258 cycles at 500 mA g −1 with a limited capacity of 500 mA h g −1 , 103 cycles at 500 mA g −1 with a limited capacity of 1000 mA h g −1 ).

CAS / MDL: 10026-22-9 693-98-1
研究领域: 材料科学 · 能源存储与转换
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

α-Fe2O3 nanospindles as an efficient catalyst for optical and magnetic fields co-assisted Li-O2 cells

Daming Yang,Guiru Sun,Xinru Wang,Fengyang Li,Ze Gao,Pingli Zhang,Wei Lu,Ming Feng

The photo-assisted lithium-oxygen (Li-O 2 ) cell is widely concerned due to its low overpotential. However, rapid recombination rate of photogenerated electrons and holes remains a fundamental challenge for photo-assisted Li-O 2 cells. Herein, we design an optical and magnetic fields co-assisted Li-O 2 cell based on α-Fe 2 O 3 nanospindles. We employed PL spectrum and I-t curve confirm that under the magnetic field, the photogenerated electrons and holes are driven via the opposite Lorentz forces in photo-assisted Li-O 2 cells, which is beneficial to accelerating the formation and decomposition of Li 2 O 2 . The optical and magnetic fields co-assisted Li-O 2 cell based on α-Fe 2 O 3 nanospindles achieves an ultra-high discharge platform of 3.47 V and a low charge platform of 3.57 V, as well as a surprising energy efficiency of 97.2%. In addition, the optical and magnetic fields co-assisted Li-O 2 cell can stably cycle for over 25 cycles. This study offers a reference for improving the electrochemical kinetics of photo-assisted Li-O 2 cell by introducing magnetic field, which opens up a new avenue for the development of high-performance Li-O 2 cells.

研究领域: 材料科学 · 电化学
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Preparation and properties of (Ce0.2Zr0.2Ti0.2Sn0.2Y0.2-xCax)O2-δ (x=0∼0.2) high-entropy of compositionally-complex ceramics

Siyuan Li,Cuiwei Li,Huaiming Jia,Guangjin Chen,Kepi Chen,Linan An

In this paper, a series of (Ce 0.2 Zr 0.2 Ti 0.2 Sn 0.2 Y 0.2- x Ca x )O 2-δ ( x  = 0∼0.2) high-entropy of compositionally-complex ceramics were prepared using solid-state reaction method. The results showed that the content of Ca 2+ had significant effects on the phase composition, microstructure and properties of the prepared materials. As Ca 2+ content increased, single-phase fluorite was easier to form. When x  ≤ 0.05, materials contained dual-phase of fluorite and pyrochlore structures. When x  ≥ 0.075, the prepared materials showed single-phase fluorite structure, which indicated that high-entropy fluorite ceramics (HEFCs) could be prepared under this condition. When Ca 2+ content increased from 0.075 to 0.2, grain size of HEFCs decreased, and relative density decreased from 95.7 % to 78.6 %. Thermal conductivity of these HEFCs varied from 1.87 W m −1  K −1 to 1.60 W m −1  K −1 , which was lower than 8YSZ. As Ca 2+ content increased, both size disorder and mass disorder increased too leading to low thermal conductivity. The results indicate that the prepared HEFCs are promising for thermal insulation applications.

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RSC Advances · 2018 ·Vol. 8 ·期 56 ·32325-32332 · IF 2.936

Chemical bond parameters, bond energy and the local crystal sites of Eu3+ in Ca5(BO3)3F:1% Eu3+ phosphor

Yuhan Zhu,Yu Pan,Wenjun Wang,Haibing Xu,Liqun Zhou,Xiaoguang Liu,Ling Li

The local crystal sites occupied by Eu3+ in Ca5(BO3)3F:1% Eu3+ phosphor were investigated experimentally and theoretically. Ca5(BO3)3F:1% Eu3+ was synthesized by high-temperature solid-state method in air. The crystal structure and optical properties of the phosphor were studied by X-ray powder diffraction and photoluminescence, respectively. Two different O2− → Eu3+ CT broad bands with the peaks at 266 and 283 nm in Ca5(BO3)3F:1% Eu3+ were detected, indicating the Eu3+ sites occupied Ca2 and Ca1, respectively. The different sharp f–f emission spectra under the excitation of 283 and 266 nm proved that there are two different local lattice environments around Eu3+ existing in Ca5(BO3)3F:1% Eu3+. Environmental factor he, the standard deviation of environmental factor (EFSD) and the bond energy were used to illustrate and explain the site occupancy mechanism of Eu3+ into the host lattice. By comparing the intensity ratios of 5D0 → 7F2 transition to the 5D0 → 7F1 transition, I(5D0/7F2)/I(5D0/7F1) of Eu3+ at Ca2 (7.381) was found to be 2.5 times stronger than that of Eu3+ at Ca1 site (2.933). was calculated to analyze the I(5D0/7F2)/I(5D0/7F1) value. On the basis of the bond valence model, a bond-energy method was used to study the occupancy of the Eu ion, which indicated that the preferential sites of Eu ion occupancy in the Ca5(BO3)3F are the Ca2 and Ca1 sites. All three theoretical calculation results are consistent with each other.

研究领域: 材料科学 · 固体化学 · 光学 · 晶体学
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ENVIRONMENTAL RESEARCH · 2024 · IF 7.7

SbSeI for high-efficient photocatalytic degradation of multiple pollutants

Kang Li,Yue Gao,Zhongxin Dong,Huibo Zhang,Xudong Fan,Lei Xu,Jie Huang,Feng Teng,Haibo Fan,Jiaming Song,Chunmei Zhang,Xuexia He,Peng Hu

Photocatalytic degradation is an effective technology for degrading water pollution that plays a significant role in environmental remediation. Ternary 2D ternary V-VI-VIIA semiconductors are ideal candidates for photocatalytic degradation of pollutants due to effective light absorption and high charge carrier mobility. In this work, high-quality SbSeI crystals were prepared using the chemical vapor transport (CVT) method and their photocatalytic degradation performance for multiple pollutants was studied. SbSeI exhibits excellent photocatalytic performance in the degradation of potassium dichromate (Cr (VI)), rhodamine B (RhB), tetracycline hydrochloride (TC-HCl) and methyl orange (MO). More than 98% of Cr (VI) and RhB can be removed after irradiation with an Xe lamp for 10 min and 40 min, respectively. The capture experiments and electron spin resonance results indicated that · O 2 − plays a major role in reducing Cr (VI), while h + plays a primary role in the degradation of MO, RhB and TC-HCl. Interestingly, the degradation rate of Cr (VI) is 1.3 times higher than that of a single pollutant system, and the degradation rate of RhB is 1.6 times higher, due to the enhanced separation and utilization of holes and electrons. The results demonstrate that SbSeI is a potential photocatalytic degradation material.

研究领域: 环境科学 · 材料科学 · 化学
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