Small
·
2024
·
IF 13
Nan Wang,Tingxue Fang,Tinghui An,Yuhao Wang,Jiaqi Li,Shuming Yu,Honghai Sun,Dong Xiang,Xiangjie Bo,Kedi Cai
Li-O 2 batteries urgently needs high discharge capacity and stable cycling performance, requiring effective and reliable bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, Hovenia acerba Lindl -like heterostructure composed of cobalt sulfide and tin dioxide supported on carbon substrate (CoS/SnO 2 @C) is prepared via CO 2 laser irradiation technology. The half-wave potential of CoS/SnO 2 @C for the ORR is 0.88 V, while the overpotential of the OER at 10 mA cm −2 is as low as 270 mV. The Li-O 2 batteries employing the bifunctional CoS/SnO 2 @C catalyst displays a high discharge specific capacity of 3332.25 mAh g −1 and long cycling life of 226 cycles. Additionally, theory calculations demonstrate that the construction of heterostructure decreases energy barrier of the rate-determining step (RDS) for both ORR and OER. Notably, SnO 2 behaves as the electronic promoter to optimize the electronic structure of heterostructure interface and triggers charge redistribution of CoS, which weakens the adsorption strength of the * O-intermediates and allows to break the linear scaling relationship, thus further enhancing the catalytic performance of CoS/SnO 2 @C. This research furnishes directions for the design of heterogeneous catalysts, highlighting its great potential for application in rechargeable Li-O 2 batteries.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Dan Li,Changyan Zhu,Min Zhang,Ying Wang,Ziye Kang,Yulong Liu,Jun Liu,Jia Liu,Haiming Xie
How to develop a homogeneous redox mediator (RM) towards both ORR and OER and how to prevent the shuttle effect are two main issues for Li-O 2 batteries thus far. Here, we firstly report 1,2-dimethyl-3-propylimidazolium iodide (DMPII), which serves multiple functions as a RM for discharge capacity promotion, a RM for charge potential reduction, and a Li anode protector for shuttling suppression by in situ generating a “self-defensed” SEI layer. Benefiting from these advantages, a cell with DMPII displays a stable cyclability with a low terminal charge potential of ~3.6 V till the cell death, a considerable rate performance, and a good reversibility associated with Li 2 O 2 formation and degradation. Based on the experimental and density functional theory (DFT) calculation results, a working mechanism for a cell operation is also proposed. These results represent a promising progress in the development of multiple-functional RM for Li-O 2 batteries. Moreover, we expect that this work gives an insight into the in situ protection of Li metal anode for board applications ( e.g., Li-S batteries, all-solid-state Li-ion batteries, etc. ).
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BIOSENSORS & BIOELECTRONICS
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2013
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IF 5.437
Lin Liu,Feng Zhao,Fengji Ma,Liping Zhang,Suling Yang,Ning Xia
β-Amyloid (Aβ) peptides are believed to be important for the diagnosis and prognosis of Alzheimer's disease (AD) serving as reliable molecular biomarkers. In this work, we reported a simple and sensitive electrochemical strategy for the detection of total Aβ peptides using gold nanoparticles modified with Aβ(1–16)-heme (denoted as Aβ(1–16)-heme-AuNPs). Monoclonal antibody (mAb) specific to the common N-terminus of Aβ was immobilized onto gold electrode for the capture of Aβ(1–16)-heme-AuNPs. The anchored Aβ(1–16)-heme-AuNPs showed strong electrocatalytic O 2 reduction. Pre-incubation of the mAb-covered electrode with native Aβ decreased the amount of Aβ(1–16)-heme-AuNPs immobilized onto the electrode, resulting in the decrease of the reduction current of O 2 to H 2 O 2 . The competitive assay is sensitive and selective to Aβ peptides. The voltammetric responses were found to be proportional to the concentrations of Aβ ranging from 0.02 to 1.50 nM, and a detection limit of 10 pM was achieved. To demonstrate the viability of the method for the analysis of Aβ in real sample, artificial cerebrospinal fluid (aCSF) containing Aβ(1–40), Aβ(1–42) and Aβ(1–16) was tested. We believe that the method would offer a useful means for quantifying Aβ in a biological matrix, and be valuable in the design of new types of electrochemical biosensors for the detection of peptides and proteins.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yuanhong Xie,Chenrui Liu,Dejian Li,Yun Liu
Herein, a novel composite of MIL-101(Fe) loaded with nitrogen doped carbon quantum dots (NCQDs/MIL-101(Fe), denoted as NQML), which can construct dual effect of photocatalysis and photo-Fenton for organic pollutants removal, was prepared by solvent impregnation method. Characterization methods proved that NQML had been synthesized successfully. Additionally, the adding volume of NCQDs could effectively influence the photocatalytic activities of NQML-x composites (x represents the adding volume of NCQDs) for tetracycline (TC) degradation, and NQML-8 exhibited the optimum photocatalytic performance among the studied catalysts upon visible light illumination under natural pH, which can completely degrade TC within 180 min. By comparison, the TC degradation kinetic constant in the system with NQML-8 was as 15.85 and 8.24 folds of that in the NCQDs and MIL-101(Fe) systems, respectively. The mechanism study proved that the enhanced photocatalytic performance of NQML was resulted from the visible light up-conversion property, electron-hole separation and transfer capacity of NCQDs. Meanwhile, NQML could not only produce h + but also lead to in-situ generation of O 2 - and H 2 O 2 by activation of O 2 under visible light. The generated H 2 O 2 could react with Fe(II) in MIL-101(Fe) to produce OH so as to construct a dual effect of photocatalysis and photo-Fenton in TC removal.
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ANALYTICAL CHEMISTRY
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2014
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IF 5.825
Chuantao Hou,Dapeng Yang,Bo Liang,Aihua Liu
The power output and stability of enzyme-based biofuel cells (BFCs) is greatly dependent on the properties of both the biocathode and bioanode, which may be adapted for portable power production. In this paper, a novel highly uniform three-dimensional (3D) macroporous gold (MP-Au) film was prepared by heating the gold “supraspheres”, which were synthesized by a bottom-up protein templating approach, and followed by modification of laccase on the MP-Au film by covalent immobilization. The as-prepared laccase/MP-Au biocathode exihibited an onset potential of 0.62 V versus saturated calomel electrode (SCE, or 0.86 V vs NHE, normal hydrogen electrode) toward O2 reduction and a high catalytic current of 0.61 mAcm–2. On the other hand, mutated glucose dehydrogenase (GDH) surface displayed bacteria (GDH-bacteria) were used to improve the stability of the glucose oxidation at the bioanode. The as-assembled membraneless glucose/O2 fuel cell showed a high power output of 55.8 ± 2.0 μW cm–2 and open circuit potential of 0.80 V, contributing to the improved electrocatalysis toward O2 reduction at the laccase/MP-Au biocathode. Moreover, the BFC retained 84% of its maximal power density even after continuous operation for 55 h because of the high stability of the bacterial surface displayed GDH mutant toward glucose oxidation. Our findings may be promising for the development of more efficient glucose BFC for portable battery or self-powered device applications.
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Advanced Energy Materials
·
2024
·Vol. 14
·期 36
·2401509
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IF 24.4
Han Yu,Guoliang Zhang,Dongmei Zhang,Ruonan Yang,Xia Li,Xiuqi Zhang,Gang Lian,Hua Hou,Zhanhu Guo,Chuanxin Hou,Xiaoyang Yang,Feng Dang
Although lithium–oxygen batteries (LOBs) hold great promise as future energy storage systems, they are impeded by insulated discharge product Li 2 O 2 and sluggish oxygen reduction reaction/oxygen evolution revolution (ORR/OER) kinetics. The application of a highly efficient cathode catalyst determines the LOBs performance. The d-band modulation and catalytic kinetics promotion are important concept guidelines for the performance enhancement of cathode catalysts. In this work, the homogeneous in-plane distortion-derived synergistic catalytic capability of an Ag 2 Mo 2 O 7 catalyst with modulated d-band centers and promoted ORR/OER kinetics is demontrated. The uniform elongation of Ag─O bonds and compression of Mo─O bonds in (020) plane leads to d-band splitting and d-band center optimization and delivers improved adsorption behavior for high ORR/OER capability. Furthermore, the spatial and energy overlap of Ag d xz and O 2 anti-bonding π * orbitals facilitate electron injection during ORR process and reduce the energy barrier for charge transfer and O 2 desorption during OER process, accelerating the ORR/OER kinetics. As a result, the (020) plane-exposed Ag 2 Mo 2 O 7 cathode exhibits ultralong cycle stability of 817 cycles at 500 mA g −1 and large specific discharge/charge capacities of 15898/15180 mAh g −1 . This work provides facile concept guidance for optimizing catalytic capability through controlled lattice distortion in cathode catalysts for LOBs.
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CERAMICS INTERNATIONAL
·
2025
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IF 5.6
Taoyi Lu,Xingmin Feng,Zhiqin Wen,Li Tang,Suzhen Kang,Jiyuan Huang,Gaoxiang Wei,Siyi Huang,Defeng Long,Sheng Wang
In this study, (Ce 0.2 Zr 0.2 La 0.2 Yb 0.2 Ln 0.2 )O 2- δ (Ln = Er, Y, Sm; labelled as H-Er, H-Y, H-Sm) high-entropy fluorite oxides (HEFOs) are designed by standard deviation and first-principles calculation. These HEFOs are subsequently synthesized via solid-phase reaction method, and the phase formation, microstructure, mechanical and thermal properties of the three samples have been systematically investigated. The results show that the three samples, exhibiting a single-phase fluorite structure, are successfully prepared after sintering at 1600 °C, and all the elements are uniformly distributed with no elemental segregation and agglomeration. The calculated δ of H-Er, H-Y and H-Sm are 0.3399, 0.3668 and 0.3458, respectively, so the chemical formula of three HEFOs are (Ce 0.2 Zr 0.2 La 0.2 Yb 0.2 Er 0.2 )O 1.6601 , (Ce 0.2 Zr 0.2 La 0.2 Yb 0.2 Y 0.2 )O 1.6332 and (Ce 0.2 Zr 0.2 La 0.2 Yb 0.2 Sm 0.2 )O 1.6542 , respectively. Additionally, the effects of rare earth ions (Er, Y and Sm) on the hardness, Young's modulus and thermal conductivity of HEFOs are analyzed. H-Y exhibits the highest hardness value and largest Young's modulus among the three HEFOs, primarily due to the largest mean acoustic velocity and cohesion energy in absolute value, smallest AGS and average bond lengths. The thermal conductivities ( κ ) of the three samples are only 1.465–1.598 W m −1 K −1 at 1000 °C. Furthermore, the thermal conductivities of the three samples are significantly lower than that of 8YSZ within the temperature range from 25 °C to 1000 °C, and H-Sm exhibits the lowest thermal conductivity in this temperature range. Consequently, they are anticipated to have promising applications in the field of thermal barrier coatings (TBCs).
研究领域:
材料科学
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固体力学
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计算材料学
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Jiadong Hou,Yufeng Liu,Chufei Cheng,Fuhao Cheng,Pengfei Qin,Yang Miao,Weihua Ji,Xiaomin Wang
The limited efficiency of traditional trial-and-error experiments has impeded the development and application of high-entropy fluorite oxides in thermal insulation coatings. To solve this problem, a novel entropy descriptor based on first principles is presented to help select candidate components for synthesizing high-entropy fluorite structure oxides. Results show that the compatibilities of 10 single-phase high-entropy fluorite oxides can be accurately predicted based on entropy formation ability. In the studied (Zr, Hf, Pr, La, X) O 2-δ system, a correlation between thermal characteristics and size/mass differences was established by designing the size and mass of X. Specifically, we found that the thermal conductivity is more strongly correlated with the difference in atomic mass, while the coefficient of thermal expansion is strongly correlated with the difference in atomic size. X-ray photoelectron spectroscopy (XPS) analysis shows that the concentration of oxygen vacancy can effectively reduce the thermal conductivity of high-entropy fluorite oxides. In addition, the values of hardness, elastic modulus and thermal conductivity of five single-phase fluorite oxides are successfully predicted by first principles calculation , and the differences between these values and the experimental results are small, which provides a prospective significance for the performance prediction of high-entropy fluorite oxides. Our findings provide a strategy for customizing high-entropy fluorite single-phase oxides with suitable properties to meet the performance requirements of thermal barrier coatings (TBCs).
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FOOD CHEMISTRY
·
2026
·
IF 10.4
Qiuya Ji,Kai Ye,Ran Meng,Sijie Wu,Ran Feng,Bao Zhang
To address the conflicting challenges of fat reduction, texture fidelity, and co-delivery of hydrophilic and hydrophobic bioactive compounds, this study explored an innovative O 1 /W/O 2 -microstructured bigel system, WGB(O 1 /W/O 2 ). The system was stabilized through whey protein aggregates rapidly adsorbing at dual interfaces as an amphiphilic mediator, along with hydrogen bonding formation with guar gum in hydrogel matrix. The extended multilayered structure enabled WGB(O 1 /W/O 2 ) demonstrated favorable cream cheese simulation performance in appearance, viscoelastic properties, melting behavior, and texture characteristics. Sequential degradation of each phase during digestion (O 2 -W-O 1 ) increased the intestinal release of PTS and GA by up to 3.3-fold and 1.8-fold, respectively, over conventional bigels (O/W or bicontinuous). Among the bigels, cream cheese texture similarity ranked O 1 /W/O 2 > bicontinuous>O/W. The delivery efficiency for hydrophobic PTS followed O 1 /W/O 2 > O/W > bicontinuous, while that for hydrophilic GA followed O 1 /W/O 2 > bicontinuous>O/W. This study highlights broad application prospects of WGB(O 1 /W/O 2 ) for fat-reduced and nutrient-enhanced dual-functional foods, while advances understanding of bigel microstructure evolution-properties relationships.
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APPLIED CATALYSIS A-GENERAL
·
2011
·
IF 3.384
Hua Yang,Jia-Qi Chen,Jun Li,Ying Lv,Shuang Gao
Hydroxylation of benzene to phenol in the [(CH 3 ) 4 N] 4 PMo 11 VO 40 /ascorbic acid/TEMPO/O 2 catalytic system was carefully investigated. UV–vis, ESR and 1 H NMR studies showed ascorbic acid radicals were formed through the hydrogen exchange of ascorbic acid with TEMPO (2,2,6,6-tetramethyl-1-piperidine-N-oxyl radicals) during the reaction. In acetonitrile, the ascorbic acid would be partly oxidized to 2-hydroxy-2-buten-4-olide (α-tetronic acid, isotetronic acid, compound 1 ) without TEMPO. The interaction of TEMPO and ascorbic acid restrained the oxidative dissociation of ascorbic acid and promoted the rate of the hydroxylation. Aqueous acetic acid solvent can also restrain the oxidative dissociation of ascorbic acid. In aqueous acetic acid, the yield of phenol could reach 18.9% in the [(CH 3 ) 4 N] 4 PMo 11 VO 40 /ascorbic acid/TEMPO/O 2 catalytic system with sufficient ascorbic acid after 400 min.
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ELECTROCHIMICA ACTA
·
2018
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IF 5.116
Chaoqun Niu,Mingke Zhang,Guangping Chen,Bokai Cao,Jiwei Shi,Jie Du,Yong Chen
Polyacrylate polymer is a promising polymer matrix for gel polymer electrolyte (GPE) in lithium-ion batteries . Herein, in-situ polymerized poly(ethylene glycol phenyl etheracrylate) (PEGPEA) based GPE combined with 1 M LiPF6 in ethylene carbonate/dimethyl carbonate/ethyl methyl carbonate (EC/DMC/EMC, 1:1:1 in volume) solvents was introduced. The maximum recoverable strain of the in-situ polymerized PEGPEA-GPE was up to 99%. The outstanding interfacial compatibility between PEGPEA-GPE and the lithium electrode was also obtained. Surprisingly, lithium dendrite was effectively suppressed in charge-discharge cycling because of polymer-enhanced solid electrolyte interphase (SEI) and excellent contact interface. Furthermore, the PEGPEA-GPE exhibited wide electrochemical stability window up to 4.9 V versus Li + /Li, and achieved an ionic conductivity of 3.35 × 10 −3 S cm −1 at 25 °C. When used as electrolyte, the Li[Ni 0.5 Co 0.2 Mn 0.3 ]O 2 /PEGPEA-GPE/Li batteries showed high discharge capacity retention rate of 97.5% after 70 charge-discharge cycles and considerable discharge rate capability, i.e., 155 mAh g −1 0.2C, 142 mAh g −1 0.5C, 120 mAh g −1 1C, 60 mAh g −1 2C. These results demonstrate that this highly elastic in-situ polymerized PEGPEA-GPE is a potential electrolyte system for high-performance polymer electrolyte lithium-ion batteries and has excellent application prospects in wearable and flexible batteries.
研究领域:
材料科学
·
电化学
·
电池技术
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