ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·24056-24063
·
IF 12.732
Yanfang Chen,Xuemei Yan,Jixiang Xu,Lei Wang
H2O2 has a wide range of uses as an oxidant and is also utilized as a high density and environmentally friendly fuel. In this study, crystalline g-C3N4 was modified with K+, Ni and N-doped carbon by thermal-polymerization of Ni2+-anchored and polyvinyl pyrrolidone-encapsulated melamine-cyanuric acid supramolecules, followed by re-calcination in a KCl–LiCl mixture. The obtained strip-like g-C3N4 nanocrystals exhibited high charge separation efficiency and good light absorption capability. Density-functional theory calculations confirmed that the orbital hybridization of Ni–N atoms enabled the formation of charge-transfer channels, which can capture electrons, achieve enhanced oxygen adsorption and reduction via a two-electron pathway. Under the synergistic effects of K+, Ni and N-doped carbon dopants and crystallinity, the obtained sample exhibited high photocatalytic H2O2 yields of 79.6 μM in O2-saturated pure water, which was 10-fold higher than the yield using pristine g-C3N4. This work provides a novel design for production of highly efficient photocatalysts for H2O2 production.
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Nanoscale
·
2021
·Vol. 13
·期 16
·7774-7782
·
IF 7.79
Gangyong Li,Guangming Ren,Wei (Alex) Wang,Zongqian Hu
Carbonaceous materials are promising electrode materials for enzymatic biofuel cells (EBFCs) due to their excellent electrical conductivity, chemical and physical stability and biocompatibility. Design and preparation of carbon materials with a hollow structure and a rough surface are of great significance for immobilization of enzymes both inside and outside the carbon materials for EBFC applications. We report herein the synthesis of novel carbonaceous materials consisting of bamboo-shaped hollow N-doped carbon nanotubes (N-CNTs) and C3N4 nanosheets (denoted as N-CNTs@C3N4) as electrode materials for dual-capture of enzymes in glucose/O2 EBFCs. The combination of one-dimensional N-CNTs with an open structure and two-dimensional C3N4 nanosheets forms a three-dimensional crosslinking network that significantly enhances the immobilization of enzymes, electrode stability, and mass transfer of substrates, thus boosting the EBFC performance. As a result, EBFCs equipped with N-CNTs@C3N4 can generate a high open circuit potential of 0.93 V and output a maximum power density of 0.57 mW cm−2 at 0.47 V. Additionally, the as-fabricated glucose/O2 EBFCs are capable of directly harvesting energy from various soft drinks, which indicates the promising applications of the N-CNTs@C3N4 nanocomposite as an electrode material for EBFCs.
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IET Nanobiotechnology
·
2020
·Vol. 14
·期 5
·347-356
·
IF 1.859
Mei Yang,Qingyuan Gui,Jinlei Ma,Lei Qi,Bijun Bao,Yida Huang
In this study, Gd 2 O 2 S:Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) upconversion nanotubes (UCNTs) were synthesised by using Gd(OH) 3 :Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) nanotubes as the template. The luminescent and biological properties of Gd 2 O 2 S:Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) UCNTs, along with photodynamic therapy (PDT) applications of the Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 (chlorin e6) nanocomposites, were systematically studied. The resultant UCNTs showed excellent biocompatibility with human retinal pigment cells (ARPE-19) even after a prolonged incubation time of 72 h, and could be used as luminescent probes. Microscopic imaging revealed that the UCNTs existed mainly in cytoplasm. PDT studies on the Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 nanocomposites indicate that the growth of the tumour (cell) could be inhibited dramatically when it was injected (incubated) with Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 nanocomposites under the irradiation of 980 nm laser.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Linfeng Peng,Hang Yin,Lu Zou,Faquan Yu
As a promising energy storage technology, Li-CO 2 /O 2 batteries not only deliver ultrahigh discharge capacity but also capture and convert CO 2 into renewable energy. The exploration into the deposition and decomposition kinetics of discharge product (Li 2 CO 3 ) is urgent for the high thermodynamic stability. Herein, the influence of current density on the essential characteristics of Li 2 CO 3 has been explored. The results show that the Li 2 CO 3 with poor crystallinity and elliptical disk morphology can be obtained at medium current density, corresponding to the excellent electrochemical performance including ultrahigh capacity of 5800 mA h/g, lower discharge-charge gap of 1.15 V, and long-term cycle life of 80 cycles. In addition, the morphology and crystallinity of Li 2 CO 3 are tailored by the relative energy barriers for electron migration and O 2 - generation. At a medium current density (500 mA/g), the accelerated electron migration can realize the nucleation rate equivalent to growth one of Li 2 CO 3 . At this time, Li 2 CO 3 will uniformly deposit on the cathode surface, forming elliptical disk morphology with poor crystallinity. Obviously, this work provides new sights for promoting the development of Li-CO 2 /O 2 battery through rational design of catalysts to accelerate the deposition and decomposition processes of Li 2 CO 3 .
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JOURNAL OF PHYSICS D-APPLIED PHYSICS
·
2024
·Vol. 57
·期 43
·435204
·
IF 3.1
Pengyu Zhao,Yikang Jia,Sihong Ma,Rui Zhang,Kaiyu Li,Tianyi Song,Jianbao Zheng,Jingyao Zhang,Li Guo,Dingxin Liu,Xiaohua Wang,Mingzhe Rong
Methicillin-resistant Staphylococcus aureus (MRSA) presents a significant threat due to the multiple resistance to antibiotics, leading to severe and challenging-to-treat infections. Plasma-activated saline (PAS) prepared by plasma gases, could efficiently inactivate various pathogenic bacteria including both sensitive and antibiotic-resistant bacteria. In this study, the PAS was prepared by plasma gases with different ratios of N2 and O2 activated by gliding arc discharge. First, the gaseous reactive species in the plasma gases were compared, revealing that the highest levels of NOx including NO2 and N2O5 were generated in the gases with the N2/O2 ratios of 4:6, 5:5, and 6:4. Subsequently, the PAS prepared by the two plasma-activated gases at the N2/O2 ratios of 5:5 and 6:4 exhibited the strongest inactivation effects on both planktic MRSA and biofilms. Furthermore, the aqueous reactive species in the PAS exhibited varied change trends with the increasing N2/O2 ratios. Additionally, ultraviolet spectroscopy combined with the probe of N, N-diethyl-p-phenylenediamine was applied for the detection of O2NOO− in the PAS, and the levels of O2NOO− in the PAS were positively correlated with the inactivation effects. Moreover, the PAS induced varying levels of nitration modification on the soluble proteins in MRSA cells, which were related to the intensities of O2NOO− in the PAS. This study regulated the reactive species in the PAS through gas composition and explored the inactivation mechanism of the PAS, providing a new strategy to promote the preparation efficiency of plasma-activated solutions for biomedical applications.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Pengken Li,Hui Zhao,Rong Ji,Wenwen Chi,Xinyu Sun,Yuming Dong,Yongfa Zhu
A one-step two-electron oxygen reduction pathway is crucial for the stable and efficient photosynthesis of hydrogen peroxide. However, the lower oxygen adsorption and activation capacity significantly restrict the ability of the one-step two-electron oxygen reduction pathway. In this work, a covalent organic framework containing a diacetylene unit (COF-Tfp-BDDA) as an efficient oxygen reduction active site was designed for the photosynthesis of hydrogen peroxide. This work demonstrates that the introduction of the diacetylene unit efficiently improved the oxygen adsorption and activation capacity of the COF. Additionally, the introduction of a diacetylene unit effectively promoted charge separation. COF-Tfp-BDDA exhibited a superior rate of H2O2 preparation (880 μmol g−1 h−1) under visible light irradiation from pure water and oxygen, better than most COF-based photocatalysts. The catalyst exhibited a stable hydrogen peroxide photosynthesis efficiency above 100 hours in cycling experiments. Based on the experimental and DFT calculation results, the introduction of a diacetylene unit not only enhances the adsorption and activation of oxygen but also alters the reduction pathway of oxygen, leading to effective charge separation. These factors contribute to the efficient photosynthesis of hydrogen peroxide in pure water. This work provides a novel idea regarding the application of COFs in the field of solar energy conversion.
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SOLID STATE IONICS
·
2016
·
IF 2.38
Cheng-Dong Li,Jin Xu,Ji-Sheng Xia,Wei Liu,Xin Xiong,Zhu-An Zheng
The FeF 3 -coated Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 cathode materials were synthesized via a wet chemical process followed by a solid state reaction . The physical properties of the as-prepared samples were conducted using X-ray diffraction, scanning electron microscopy, and transmission electron microscopy . The results indicated that the surface of cathode particles was covered by FeF 3 film (about 5–15 nm thick). Compared with the bare cathode, the FeF 3 -coated Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 one delivered the higher coulombic efficiency, better rate capability, longer cycle life, and better structure stability. A high capacity retention of 95% (190 mAh g − 1 ) after 100 cycles at 0.5 C rate was obtained for the FeF 3 -coated Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 cathode. Besides, the results from cyclic voltammetry and electrochemical impedance spectra revealed that the noteworthy enhanced electrochemical properties of the surface-modified sample were due to the presence of FeF 3 coating layer , which suppressed the side reaction between the Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 particles with electrolyte and further stabilized the Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 structure with cycling.
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JOURNAL OF POWER SOURCES
·
2012
·
IF 4.951
Jing Lin,Daobin Mu,Ying Jin,Borong Wu,Yunfeng Ma,Feng Wu
Li-rich layered composite Li[Li 0.2 Ni 0.2 Mn 0.6 ]O 2 is prepared by a novel approach in which carbon felt acts as a carrier for synthesis reaction . The as-prepared material is characterized by SEM, ICP and XRD , its electrochemical performance is also examined with galvanostatic charge/discharge and CV measurements. It is showed that the facile process controls effectively the particle growth (in size around 100–200 nm) of the composite and its chemical composition . The as-prepared material shows a high initial discharge capacity about 288 mAh g −1 when charged to 4.8 V, and a retained value of 246.8 mAh g −1 in the 40th cycle. The crystalline structure of the composite is simulated further by Material Studio. It is revealed that the composite has a compatible layer structure merged by Li 2 MnO 3 and LiNi 0.5 Mn 0.5 O 2 , which makes substantial contribution to the cycleability of the electrode. In addition, the lithiation/delithiaion properties including charge transfer resistance and lithium ion diffusion coefficient are studied with electrochemical impedance spectra.
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Environmental Technology & Innovation
·
2024
·
IF 6.7
Yi Chen,Haolan Zhang,Siyu Hu,Jiaxin Zhang,Shiruo Zhang,Qing He,Qingyue Luo,Jinchuan Gu
Iron is the most suitable candidate for activating peroxymonosulfate (PMS) for organic degradation. To realize the effective separation and recycling of iron catalysts, it is urgent to explore a low-cost and excellent supporter. In this study, a zeolite catalyst (CAN) with both supporter and catalyst functions was synthesized in one step using lithium slag (LS, containing iron), and used to degrade tetracycline (TC) wastewater. The results showed that the electron transfer of iron and sulfur in CAN promotes the decomposition of PMS. The CAN/PMS system exhibited great removal efficiency (89.5 %, 0.083 min −1 ) and relatively lower activation energy (15.31 kJ/mol) toward TC. And • O 2 - plays a crucial role in the degradation. The CAN also represented great catalytic stability and reusability. This study revealed a new approach for the synthesis of high efficiency and low-cost catalysts and the tetracycline degradation.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Zhanshuai Li,Jinsheng Li,Huanyu Zhao,Mengwen Zhang,Pengfei Li,Liang Dong,Lei Wu,Haipeng Ji,Xiwei Qi
A new high-entropy oxide, (Ge 0.2 Mn 0.2 Ti 0.2 Sn 0.2 Mo 0.2 )O 2 with rutile structure, was successfully synthesized using solid-state reaction method. The phase structure of the ceramic samples prepared forming a range of binary to quinary phase with increasing entropy were investigated, and the effects of atmosphere-induction and high-entropy synergistic behavior on the dielectric performance were studied. As the type of the cations increases, the temperature required to form a single rutile structure gradually decreases, while the dielectric properties of the ceramics gradually improved. The dielectric constant of the (Ge 0.2 Mn 0.2 Ti 0.2 Sn 0.2 Mo 0.2 )O 2 high-entropy oxide ceramics sintered in the nitrogen atmosphere at 1350°C is nearly 20 times higher of the ceramics sintered in the air. This significant enhancement can be attributed to the occurrence of two rutile structures and the generation of excessive oxygen vacancies as a result of high-entropy synergistic behavior under the nitrogen sintering atmosphere.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Daming Yang,Yingyue Zhang,Jiaqi Sun,Xinyu Zhang,Ze Gao,Qilong Sun,Tong Wu,Wei Lu,Guiru Sun,Ming Feng
The photo-assisted strategy is viewed as a promising method to improve the ORR and OER performance of Li–O 2 batteries. Nevertheless, designing a photocatalyst that ensures wide light absorption and minimizes the recombination of photoinduced electrons and holes is still a notable challenge. In this study, 2D porous Co 3 O 4 nanosheets are synthesized as photocatalysts for photo-assisted Li–O 2 batteries. Their unique structure improves surface area, facilitates O 2 transport, and stores discharge products. Equally, the Co 3 O 4 nanosheets exhibit strong light responsiveness and photocatalytic activity. Upon optical field, photoinduced electrons and holes are successfully separated on Co 3 O 4 nanosheets, which promotes the formation and decomposition of Li 2 O 2 , respectively. Li–O 2 cells using Co 3 O 4 nanosheets display a low overpotential of 0.15 V and good cycling stability under optical field. These findings highlight the potential of Co 3 O 4 nanosheets as photocatalysts for photo-assisted Li–O 2 batteries, providing a foundation for future energy storage advancements.
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