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32
result(s) for
"Jia, Shuangfeng"
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Activation of subnanometric Pt on Cu-modified CeO2 via redox-coupled atomic layer deposition for CO oxidation
2020
Improving the low-temperature activity (below 100 °C) and noble-metal efficiency of automotive exhaust catalysts has been a continuous effort to eliminate cold-start emissions, yet great challenges remain. Here we report a strategy to activate the low-temperature performance of Pt catalysts on Cu-modified CeO
2
supports based on redox-coupled atomic layer deposition. The interfacial reducibility and structure of composite catalysts have been precisely tuned by oxide doping and accurate control of Pt size. Cu-modified CeO
2
-supported Pt sub-nanoclusters demonstrate a remarkable performance with an onset of CO oxidation reactivity below room temperature, which is one order of magnitude more active than atomically-dispersed Pt catalysts. The Cu-O-Ce site with activated lattice oxygen anchors deposited Pt sub-nanoclusters, leading to a moderate CO adsorption strength at the interface that facilitates the low-temperature CO oxidation performance.
Improving low-temperature activity and noble-metal efficiency remains a challenge for next generation exhaust catalysts. Here, the authors achieve the activation of subnanometric Pt on Cu-modified CeO
2
for low-temperature CO oxidation with an onset below room temperature.
Journal Article
Synergistic Mn-Co catalyst outperforms Pt on high-rate oxygen reduction for alkaline polymer electrolyte fuel cells
2019
Alkaline polymer electrolyte fuel cells are a class of fuel cells that enable the use of non-precious metal catalysts, particularly for the oxygen reduction reaction at the cathode. While there have been alternative materials exhibiting Pt-comparable activity in alkaline solutions, to the best of our knowledge none have outperformed Pt in fuel-cell tests. Here we report a Mn-Co spinel cathode that can deliver greater power, at high current densities, than a Pt cathode. The power density of the cell employing the Mn-Co cathode reaches 1.1 W cm
−2
at 2.5 A cm
−2
at 60
o
C. Moreover, this catalyst outperforms Pt at low humidity. In-depth characterization reveals that the remarkable performance originates from synergistic effects where the Mn sites bind O
2
and the Co sites activate H
2
O, so as to facilitate the proton-coupled electron transfer processes. Such an electrocatalytic synergy is pivotal to the high-rate oxygen reduction, particularly under water depletion/low humidity conditions.
Alkaline polymer electrolyte fuel cells are promising power sources, but performance is limited by catalytic activity. Here the authors report a non-precious metal-based catalyst for electrocatalytic oxygen reduction that imparts outstanding fuel cell performance.
Journal Article
Room-temperature oxygen vacancy migration induced reversible phase transformation during the anelastic deformation in CuO
2021
From the mechanical perspectives, the influence of point defects is generally considered at high temperature, especially when the creep deformation dominates. Here, we show the stress-induced reversible oxygen vacancy migration in CuO nanowires at room temperature, causing the unanticipated anelastic deformation. The anelastic strain is associated with the nucleation of oxygen-deficient CuO
x
phase, which gradually transforms back to CuO after stress releasing, leading to the gradual recovery of the nanowire shape. Detailed analysis reveals an oxygen deficient metastable CuO
x
phase that has been overlooked in the literatures. Both theoretical and experimental investigations faithfully predict the oxygen vacancy diffusion pathways in CuO. Our finding facilitates a better understanding of the complicated mechanical behaviors in materials, which could also be relevant across multiple scientific disciplines, such as high-temperature superconductivity and solid-state chemistry in Cu-O compounds, etc.
The effect of point defects on mechanical behaviour of materials is generally considered at high temperatures. This work reports a reversible stress-induced migration of point defects during anelastic deformation in CuO nanowires at room temperature resulting from heterogeneous strain distribution.
Journal Article
Ultrathin high-κ antimony oxide single crystals
2020
Ultrathin oxides have been reported to possess excellent properties in electronic, magnetic, optical, and catalytic fields. However, the current and primary approaches toward the preparation of ultrathin oxides are only applicable to amorphous or polycrystalline oxide nanosheets or films. Here, we successfully synthesize high-quality ultrathin antimony oxide single crystals via a substrate-buffer-controlled chemical vapor deposition strategy. The as-obtained ultrathin antimony oxide single crystals exhibit high dielectric constant (~100) and large breakdown voltage (~5.7 GV m
−1
). Such a strategy can also be utilized to fabricate other ultrathin oxides, opening up an avenue in broadening the applicaitons of ultrathin oxides in many emerging fields.
The ultrathin oxide nanosheets obtained through previous approaches usually exhibit amorphism or polycrystallinity, which limit their properties towards electronic devices. Here, the authors synthesize ultrathin antimony oxide single crystals with high dielectric constant (~100) and large breakdown voltage (~5.7 GV m
−1
).
Journal Article
Synergistic passivation and stepped-dimensional perovskite analogs enable high-efficiency near-infrared light-emitting diodes
2022
Formamidinium lead iodide (FAPbI
3
) perovskites are promising emitters for near-infrared light-emitting diodes. However, their performance is still limited by defect-assisted nonradiative recombination and band offset-induced carrier aggregation at the interface. Herein, we introduce a couple of cadmium salts with acetate or halide anion into the FAPbI
3
perovskite precursors to synergistically passivate the material defects and optimize the device band structure. Particularly, the perovskite analogs, containing zero-dimensional formamidinium cadmium iodide, one-dimensional δ-FAPbI
3
, two-dimensional FA
2
FA
n-1
Pb
n
I
3n+1
, and three-dimensional α-FAPbI
3
, can be obtained in one pot and play a pivotal and positive role in energy transfer in the formamidinium iodide-rich lead-based perovskite films. As a result, the near-infrared FAPbI
3
-based devices deliver a maximum external quantum efficiency of 24.1% together with substantially improved operational stability. Combining our findings on defect passivation and energy transfer, we also achieve near-infrared light communication with device twins of light emitting and unprecedented self-driven detection.
Defect-assisted nonradiative recombination and carrier aggregation at the interface hinder the potential of perovskites as emitter for light-emitting diodes. Here, Fang et al. achieve an external quantum efficiency of 24.1% by combining multidimensional perovskite with cascade conduction bands.
Journal Article
3D Porous MXene Aerogel through Gas Foaming for Multifunctional Pressure Sensor
2022
The development of smart wearable electronic devices puts forward higher requirements for future flexible electronics. The design of highly sensitive and high-performance flexible pressure sensors plays an important role in promoting the development of flexible electronic devices. Recently, MXenes with excellent properties have shown great potential in the field of flexible electronics. However, the easy-stacking inclination of nanomaterials limits the development of their excellent properties and the performance improvement of related pressure sensors. Traditional methods for constructing 3D porous structures have the disadvantages of complexity, long period, and difficulty of scalability. Here, the gas foaming strategy is adopted to rapidly construct 3D porous MXene aerogels. Combining the excellent surface properties of MXenes with the porous structure of aerogel, the prepared MXene aerogels are successfully used in high-performance multifunctional flexible pressure sensors with high sensitivity (306 kPa -1 ), wide detection range (2.3 Pa to 87.3 kPa), fast response time (35 ms), and ultrastability (>20,000 cycles), as well as self-healing, waterproof, cold-resistant, and heat-resistant capabilities. MXene aerogel pressure sensors show great potential in harsh environment detection, behavior monitoring, equipment recovery, pressure array identification, remote monitoring, and human-computer interaction applications.
Journal Article
Author Correction: Activation of subnanometric Pt on Cu-modified CeO2 via redox-coupled atomic layer deposition for CO oxidation
2020
A Correction to this paper has been published: https://doi.org/10.1038/s41467-020-19663-3.
Journal Article
Atomistic insight into ordered defect superstructures at novel grain boundaries in CuO nanosheets: From structures to electronic properties
by
Zheng, He
,
Peng, Huayu
,
Zhao, Lulu
in
Atomic/Molecular Structure and Spectra
,
Biomedicine
,
Biotechnology
2019
Determining atomistic structures of grain boundaries (GBs) is essential to understand structure–property interplay in oxides. Here, different GB superstructures in CuO nanosheets, including
(
11
1
¯
)
and (114) twinning boundaries (TBs) and (002)/(223) GB, are investigated. Unlike the lower-energy stoichiometric
(
11
1
¯
)
TB, both experimental and first-principles investigations reveal a severe segregation of Cu and O vacancies and a nonstoichiometric property at (114) TB, which may facilitate ionic transportation and provide space for elemental segregation. More importantly, the calculated electronic structures have shown the increased conductivity as well as the unanticipated magnetism in both (114) TB and (002)/(223) GB. These findings could contribute to the race towards the property-directing structural design by GB engineering.
Journal Article
Atomic-scale observation of a two-stage oxidation process in Cu2O
by
Huihui Liu He Zheng Lei Li Huaping Sheng Shuangfeng Jia Fan Cao Xi Liu Boyun Chen Ru Xing Dongshan Zhao Jianbo Wang
in
Atomic structure
,
Atomic/Molecular Structure and Spectra
,
Biomedicine
2017
Atomic-scale oxidation dynamics of Cu2O nanocrystallines (NCs) are directly observed by in situ high-resolution transmission electron microscopy. A two-stage oxidation process is observed: (1)The initial oxidation stage is dominated by the dislocation-mediated oxidation behavior of Cu2O NCs via solid-solid transformations, leading to the formation of a new intermediate CuOx phase. The possible crystal structure of the CuOx phase is discussed. (2) Subsequently, CuOx is transformed into CuO by layer-by-layer oxidation. These results will help in understanding the oxidation mechanisms of copper oxides and pave the way for improving their structural diversity and exploiting their potential industrial applications.
Journal Article
Transmission electron microscopic study of the fine-grained vein matrix in the Suizhou L6 meteorite
by
Xiangping, Gu
,
Xiande, Xie
,
Jianbo, Wang
in
Crystallization
,
Crystals
,
Earth and Environmental Science
2016
The mineralogy of shock vein matrix in the Suizhou meteorite has been investigated by optical and transmission electron microscopy. It was revealed that the vein matrix is composed of majorite-pyrope garnet, magnesiowüstite, and ringwoodite, with FeNi–FeS intergrowths. The observation and character of ring-like selected electron diffraction (SAED) patterns indicate that the idiomorphic garnet crystals in the vein matrix have different orientations. The polycrystalline nature of magnesiowüstite is also confirmed by a ring-like SAED pattern. Both garnet and magnesiowüstite crystals showed sharp diffraction spots, signifying the good crystallinity of these two minerals. The SAED pattern of cryptocrystalline ringwoodite shows only diffuse concentric diffraction rings. FeNi metal and troilite (FeS), which were molten during the shock event, occur in the matrix as fine eutectic FeNi–FeS intergrowths filling the interstices between garnet and magnesiowüstite grains. Based on the phase diagram of the Allende chondrite and the results of this TEM study, it is inferred that majorite-pyrope garnet first crystallized from the Suizhou chondritic melt at 22–26 GPa, followed by crystallization of magnesiowüstite at 20–24 GPa, and then ringwoodite at 18–20 GPa. The eutectic intergrowths of FeNi-metal and troilite are proposed to have crystallized during meteorite cooling and solidified at the last stage of vein formation.
Journal Article