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1.
Angew Chem Int Ed Engl ; : e202406007, 2024 Apr 30.
Artículo en Inglés | MEDLINE | ID: mdl-38687057

RESUMEN

While the mild production of syngas (a mixture of H2 and CO) from CO2 and H2O is a promising alternative to the coal-based chemical engineering technologies, the inert nature of CO2 molecules, unfavorable splitting pathways of H2O and unsatisfactory catalysts lead to the challenge in the difficult integration of high CO2 conversion efficiency with produced syngas with controllable H2/CO ratios in a wide range. Herein, we report an efficient plasma-driven catalytic system for mild production of pure syngas over porous metal-organic framework (MOF) catalysts with rich confined H2O molecules, where their syngas production capacity is regulated by the in situ evolved ligand defects and the plasma-activated intermediate species of CO2 molecules. Specially, the Cu-based catalyst system achieves 61.9 % of CO2 conversion and the production of pure syngas with wide H2/CO ratios of 0.05:1-4.3:1. As revealed by the experimental and theoretical calculation results, the in situ dynamic structure evolution of Cu-containing MOF catalysts favors the generation of coordinatively unsaturated metal active sites with optimized geometric and electronic characteristics, the adsorption of reactants, and the reduced energy barriers of syngas-production potential-determining steps of the hydrogenation of CO2 to *COOH and the protonation of H2O to *H.

2.
Proc Natl Acad Sci U S A ; 121(15): e2319525121, 2024 Apr 09.
Artículo en Inglés | MEDLINE | ID: mdl-38564637

RESUMEN

The fine regulation of catalysts by the atomic-level removal of inactive atoms can promote the active site exposure for performance enhancement, whereas suffering from the difficulty in controllably removing atoms using current micro/nano-scale material fabrication technologies. Here, we developed a surface atom knockout method to promote the active site exposure in an alloy catalyst. Taking Cu3Pd alloy as an example, it refers to assemble a battery using Cu3Pd and Zn as cathode and anode, the charge process of which proceeds at about 1.1 V, equal to the theoretical potential difference between Cu2+/Cu and Zn2+/Zn, suggesting the electricity-driven dissolution of Cu atoms. The precise knockout of Cu atoms is confirmed by the linear relationship between the amount of the removed Cu atoms and the battery cumulative specific capacity, which is attributed to the inherent atom-electron-capacity correspondence. We observed the surface atom knockout process at different stages and studied the evolution of the chemical environment. The alloy catalyst achieves a higher current density for oxygen reduction reaction compared to the original alloy and Pt/C. This work provides an atomic fabrication method for material synthesis and regulation toward the wide applications in catalysis, energy, and others.

3.
J Colloid Interface Sci ; 664: 938-945, 2024 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-38503079

RESUMEN

Supramolecular self-assembly is ubiquitous in living system and is usually controlled to proceed in time and space through sophisticated reaction-diffusion processes, underpinning various vital cellular functions. In this contribution, we demonstrate how spatiotemporal self-assembly of supramolecular hydrogels can be realized through a simple reaction-diffusion-mediated transient transduction of pH signal. In the reaction-diffusion system, a relatively faster diffusion of acid followed by delayed enzymatic production and diffusion of base from the opposite site enables a transient transduction of pH signal in the substrate. By coupling such reaction-diffusion system with pH-sensitive gelators, dynamic supramolecular hydrogels with tunable lifetimes are formed at defined locations. The hydrogel fibers show interesting dynamic growing behaviors under the regulation of transient pH signal, reminiscent of their biological counterpart. We further demonstrate a proof-of-concept application of the developed methodology for dynamic information encoding in a soft substrate. We envision that this work may provide a potent approach to enable transient transduction of various chemical signals for the construction of new colloidal materials with the capability to evolve their structures and functionalities in time and space.

4.
Angew Chem Int Ed Engl ; : e202404258, 2024 Mar 07.
Artículo en Inglés | MEDLINE | ID: mdl-38454791

RESUMEN

Engineering advantageous defects to construct well-defined active sites in catalysts is promising but challenging to achieve efficient photocatalytic NH3 synthesis from N2 and H2O due to the chemical inertness of N2 molecule. Here, we report defective Fe-based metal-organic framework (MOF) photocatalysts via a non-thermal plasma-assisted synthesis strategy, where their NH3 production capability is synergistically regulated by two types of defects, namely, bridging organic ligands and terminal inorganic ligands (OH- and H2O). Specially, the optimized MIL-100(Fe) catalysts, where there are only terminal inorganic ligand defects and coexistence of dual defects, exhibit the respective 1.7- and 7.7-fold activity enhancement comparable to the pristine catalyst under visible light irradiation. As revealed by experimental and theoretical calculation results, the dual defects in the catalyst induce the formation of abundant and highly accessible coordinatively unsaturated Fe active sites and synergistically optimize their geometric and electronic structures, which favors the injection of more d-orbital electrons in Fe sites into the N2 π* antibonding orbital to achieve N2 activation and the formation of a key intermediate *NNH in the reaction. This work provides a guidance on the rational design and accurate construction of porous catalysts with precise defective structures for high-performance activation of catalytic molecules.

5.
Polymers (Basel) ; 15(18)2023 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-37765617

RESUMEN

Given the issues of soil cracking, poor water retention during drought, and erosion damage caused by rainfall, we conducted an in-depth study on the water retention properties, cracking resistance, and scouring resistance of biogel-amended clay using evaporation cracking and scouring tests. The hydrophysical properties and cohesive aggregation mechanism of biogel-amended clay were explored, and the results showed that the incorporation of biogel improved the water retention, cracking resistance, and scour resistance of the clay samples. With an increase in the biogel content, the biogel mucous membrane inside the samples improved the cohesion between soil particles, reduced the generation and development of cracks, and improved the cracking resistance. There was no significant cracking of the samples after the biogel content reached 0.3%, which changed the migration of water in the sample, prevented water evaporation, and improved the water retention of the clay samples. Biofilm can change the migration of water in the sample, prevent some evaporation, and reduce the evaporation rate. To a certain extent, it can enhance the water retention capacity of the sample. Enhanced biofilm content significantly reduced scouring in the process of rainfall and runoff erosion of the sample, and biofilm content of 0.2% significantly reduced the surface of the specimen damaged by erosion. The hydrophysical properties of the composite-adhesive-amended clay samples were significantly improved compared with those of the single-bioadhesive-amended clay samples.

7.
Innovation (Camb) ; 4(4): 100468, 2023 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-37427353

RESUMEN

The radiation tolerance of energy storage batteries is a crucial index for universe exploration or nuclear rescue work, but there is no thorough investigation of Li metal batteries. Here, we systematically explore the energy storage behavior of Li metal batteries under gamma rays. Degradation of the performance of Li metal batteries under gamma radiation is linked to the active materials of the cathode, electrolyte, binder, and electrode interface. Specifically, gamma radiation triggers cation mixing in the cathode active material, which results in poor polarization and capacity. Ionization of solvent molecules in the electrolyte promotes decomposition of LiPF6 along with its decomposition, and molecule chain breaking and cross-linking weaken the bonding ability of the binder, causing electrode cracking and reduced active material utilization. Additionally, deterioration of the electrode interface accelerates degradation of the Li metal anode and increases cell polarization, hastening the demise of Li metal batteries even more. This work provides significant theoretical and technical evidence for development of Li batteries in radiation environments.

8.
ACS Appl Mater Interfaces ; 14(38): 43825-43832, 2022 Sep 28.
Artículo en Inglés | MEDLINE | ID: mdl-36103624

RESUMEN

The movements of soft living tissues, such as muscle, have sparked a strong interest in the design of hydrogel actuators; however, so far, typical manmade examples still lag behind their biological counterparts, which usually function under nonequilibrium conditions through the consumption of high-energy biomolecules and show highly autonomous behaviors. Here, we report on self-resettable hydrogel actuators that are powered by a chemical fuel and can spontaneously return to their original states over time once the fuels are depleted. Self-resettable actuation originates from a chemical fuel-mediated transient change in the hydrophilicity of the hydrogel networks. The actuation extent and duration can be programmed by the fuel levels, and the self-resettable actuation process is highly recyclable through refueling. Furthermore, various proof-of-concept autonomous soft robots are created, resembling the movements of soft-bodied creatures in nature. This work may serve as a starting point for the development of lifelike soft robots with autonomous behaviors.


Asunto(s)
Hidrogeles , Robótica , Hidrogeles/química , Interacciones Hidrofóbicas e Hidrofílicas , Movimiento , Músculos
9.
Oxid Med Cell Longev ; 2022: 7655142, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-35265264

RESUMEN

Activation of the proinflammatory-associated cytokine, tumor necrosis factor-α (TNF-α), in nucleus pulposus (NP) cells is essential for the pathogenesis of intervertebral disc degeneration (IDD). Restoring autophagic flux has been shown to effectively protect against IDD and is a potential target for treatment. The goal of this study was to explore particular autophagic signalings responsible for the protective effects of naringin, a known autophagy activator, on human NP cells. The results showed that significantly increased autophagic flux was observed in NP cells treated with naringin, with pronounced decreases in the inflammatory response and oxidative stress, which rescued the disturbed cellular homeostasis induced by TNF-α activation. Autophagic flux inhibition was detectable in NP cells cotreated with 3-methyladenine (3-MA, an autophagy inhibitor), partially offsetting naringin-induced beneficial effects. Naringin promoted the expressions of autophagy-associated markers via SIRT1 (silent information regulator-1) activation by AMPK (AMP-activated protein kinase) phosphorylation. Either AMPK inhibition by BML-275 or SIRT1 silencing partially counteracted naringin-induced autophagic flux enhancement. These findings indicate that naringin boosts autophagic flux through SIRT1 upregulation via AMPK activation, thus protecting NP cells against inflammatory response, oxidative stress, and impaired cellular homeostasis. Naringin can be a promising inducer of restoration autophagic flux restoration for IDD.


Asunto(s)
Proteínas Quinasas Activadas por AMP/metabolismo , Autofagia/efectos de los fármacos , Flavanonas/uso terapéutico , Homeostasis/efectos de los fármacos , Inflamación/tratamiento farmacológico , Núcleo Pulposo/efectos de los fármacos , Sirtuina 1/metabolismo , Factor de Necrosis Tumoral alfa/metabolismo , Flavanonas/farmacología , Humanos , Estrés Oxidativo/efectos de los fármacos , Transfección
10.
Nat Commun ; 13(1): 5, 2022 Jan 10.
Artículo en Inglés | MEDLINE | ID: mdl-35013151

RESUMEN

Extra-terrestrial explorations require electrochemical energy storage devices able to operate in gravity conditions different from those of planet earth. In this context, lithium (Li)-based batteries have not been fully investigated, especially cell formation and cycling performances under supergravity (i.e., gravity > 9.8 m s-2) conditions. To shed some light on these aspects, here, we investigate the behavior of non-aqueous Li metal cells under supergravity conditions. The physicochemical and electrochemical characterizations reveal that, distinctly from earth gravity conditions, smooth and dense Li metal depositions are obtained under supergravity during Li metal deposition on a Cu substrate. Moreover, supergravity allows the formation of an inorganic-rich solid electrolyte interphase (SEI) due to the strong interactions between Li+ and salt anions, which promote significant decomposition of the anions on the negative electrode surface. Tests in full Li metal pouch cell configuration (using LiNi0.8Co0.1Mn0.1O2-based positive electrode and LiFSI-based electrolyte solution) also demonstrate the favorable effect of the supergravity in terms of deposition morphology and SEI composition and ability to carry out 200 cycles at 2 C (400 mA g-1) rate with a capacity retention of 96%.

11.
Entropy (Basel) ; 23(5)2021 Apr 28.
Artículo en Inglés | MEDLINE | ID: mdl-33924967

RESUMEN

Depth maps obtained through sensors are often unsatisfactory because of their low-resolution and noise interference. In this paper, we propose a real-time depth map enhancement system based on a residual network which uses dual channels to process depth maps and intensity maps respectively and cancels the preprocessing process, and the algorithm proposed can achieve real-time processing speed at more than 30 fps. Furthermore, the FPGA design and implementation for depth sensing is also introduced. In this FPGA design, intensity image and depth image are captured by the dual-camera synchronous acquisition system as the input of neural network. Experiments on various depth map restoration shows our algorithms has better performance than existing LRMC, DE-CNN and DDTF algorithms on standard datasets and has a better depth map super-resolution, and our FPGA completed the test of the system to ensure that the data throughput of the USB 3.0 interface of the acquisition system is stable at 226 Mbps, and support dual-camera to work at full speed, that is, 54 fps@ (1280 × 960 + 328 × 248 × 3).

12.
Adv Mater ; 33(5): e2006323, 2021 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-33326157

RESUMEN

Lithium metal is the "holy grail" of anodes, capable of unlocking the full potential of cathodes in next-generation batteries. However, the use of pure lithium anodes faces several challenges in terms of safety, cycle life, and rate capability. Herein, a solution-processable conjugated microporous thermosetting polymer (CMP) is developed. The CMP can be further converted into a large-scale membrane with nanofluidic channels (5-6 Å). These channels can serve as facile and selective Li-ion diffusion pathways on the surfaces of lithium anodes, thereby ensuring stable lithium stripping/plating even at high areal current densities. CMP-modified lithium anodes (CMP-Li) exhibit cycle stability of 2550 h at an areal current density of 20 mA cm-2 . Furthermore, CMP is readily amenable to solution-processing and spray coating, rendering it highly applicable to continuous roll-to-roll lithium metal treatment processes. Pouch cells with CMP-Li as the anode and LiNi0.8 Co0.1 Mn0.1 O2 (NCM811) as the cathode exhibits a stable energy density of 400 Wh kg-1 .

13.
Adv Mater ; 32(7): e1907079, 2020 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-31867806

RESUMEN

Rechargeable lithium (Li) metal batteries hold great promise for revolutionizing current energy-storage technologies. However, the uncontrollable growth of lithium dendrites impedes the service of Li anodes in high energy and safety batteries. There are numerous studies on Li anodes, yet little attention has been paid to the intrinsic electrocrystallization characteristics of Li metal and their underlying mechanisms. Herein, a guided growth of planar Li layers, instead of random Li dendrites, is achieved on self-assembled reduced graphene oxide (rGO). In situ optical observation is performed to monitor the morphology evolution of such a planar Li layer. Moreover, the underlying mechanism during electrodeposition/stripping is revealed using ab initio molecular dynamics simulations. The combined experiment and simulation results show that when Li atoms are deposited on rGO, each layer of Li atoms grows along (110) crystallographic plane of the Li crystals because of the fine in-plane lattice matching between Li and the rGO substrate, resulting in planar Li deposition. With this specific topographic characteristic, a highly flexible lithium-sulfur (Li-S) full cell with rGO-guided planar Li layers as the anode exhibits stable cycling performance and high specific energy and power densities. This work enriches the fundamental understanding of Li electrocrystallization without dendrites and provides guidance for practical applications.

14.
Front Chem ; 6: 517, 2018.
Artículo en Inglés | MEDLINE | ID: mdl-30460226

RESUMEN

Lithium (Li) metal, with ultra-high theoretical capacity and low electrochemical potential, is the ultimate anode for next-generation Li metal batteries. However, the undesirable Li dendrite growth usually results in severe safety hazards and low Coulombic efficiency. In this work, we design a three-dimensional CuO@Cu submicron wire sponge current collector with high mechanical strength SEI layer dominated by Li2O during electrochemical reaction process. The 3D CuO@Cu current collector realizes an enhanced CE of above 91% for an ultrahigh current of 10 mA cm-2 after 100 cycles, and yields decent cycle stability at 5 C for the full cell. The exceptional performances of CuO@Cu submicron wire sponge current collector hold promise for further development of the next-generation metal-based batteries.

15.
Opt Express ; 25(22): 26468-26482, 2017 Oct 30.
Artículo en Inglés | MEDLINE | ID: mdl-29092136

RESUMEN

Discrete Fourier transform spread orthogonal frequency-division multiplexing (DFT-S-OFDM) has demonstrated its capability in reducing peak to average ratio (PAPR), while maintaining reliable transmissions. This paper investigates the application of DFT-S-OFDM technology in visible light communications (VLC), and reveals the mechanism on how a multiple lighting distributed layout affects its performance. In addition, an optimization approach of lighting layout is proposed through making a trade-off between the strong interfered areas and the maximum delay spread inside. Eventually, a Gbit/s DFT-S-OFDM based multiple lighting VLC downlink prototype is achieved for the first time in the form of real-time baseband modem and compact size components.

16.
Opt Express ; 23(7): 8409-21, 2015 Apr 06.
Artículo en Inglés | MEDLINE | ID: mdl-25968680

RESUMEN

Discrete multi-tone (DMT) modulation is an attractive modulation format for short-reach applications to achieve the best use of available channel bandwidth and signal noise ratio (SNR). In order to realize polarization-multiplexed DMT modulation with direct detection, we derive an analytical transmission model for dual polarizations with intensity modulation and direct diction (IM-DD) in this paper. Based on the model, we propose a novel polarization-interleave-multiplexed DMT modulation with direct diction (PIM-DMT-DD) transmission system, where the polarization de-multiplexing can be achieved by using a simple multiple-input-multiple-output (MIMO) equalizer and the transmission performance is optimized over two distinct received polarization states to eliminate the singularity issue of MIMO demultiplexing algorithms. The feasibility and effectiveness of the proposed PIM-DMT-DD system are investigated via theoretical analyses and simulation studies.

17.
Opt Express ; 23(9): 11412-23, 2015 May 04.
Artículo en Inglés | MEDLINE | ID: mdl-25969236

RESUMEN

We present a method to mitigate the chromatic dispersion (CD)-induced power fading effect (PFE) in high-speed and short-reach carrier-less amplitude and phase (CAP) systems using the degenerate four-wave mixing (DFWM) effect and a decision feedback equalizer (DFE). Theoretical and numerical investigations reveal that DFWM components produced by the interaction between the main carrier and the signal sideband help to mitigate PFE in direct detection systems. By optimizing the launch power, a maximum reach of 60 km in single mode fiber (SMF-e + ) at 1530nm is experimentally demonstrated for a 40 Gbit/s CAP32 system. In addition, we study the performance of a decision feedback equalizer (DFE) and a traditional linear equalizer (LE) in a channel with non-flat in-band frequency response. The superior PFE tolerance of DFE is experimentally validated, and thereby, the maximum reach is extended to 80 km. To the best of our knowledge, this is the twice the longest transmission distance reported so far for a single-carrier 40 Gbit/s CAP system around 1550 nm.

18.
Opt Express ; 23(2): 882-94, 2015 Jan 26.
Artículo en Inglés | MEDLINE | ID: mdl-25835848

RESUMEN

We experimentally demonstrate improved intra-channel nonlinearity tolerance of the root M-shaped pulse (RMP) with respect to the root raised cosine (RRC) pulse in spectrally efficient 128 Gbit/s PDM-16QAM coherent transmission systems. In addition we evaluate the impact of dispersion map and fiber dispersion parameter on the intra-channel nonlinearity tolerance of the RRC pulse and the RMP via both simulation and experimentation. The RMP is shown to have a better nonlinear tolerance than the RRC pulse for most investigated scenarios except for links with zero residual dispersion percentage per span or the zero dispersion region of a fiber. Therefore, the RMP is suitable for extending the maximum reach of spectrally efficient coherent transmission systems in legacy links in addition to currently intensively studied standard single mode fiber (SSMF) based dispersion unmanaged links.

19.
Opt Express ; 23(2): 1176-89, 2015 Jan 26.
Artículo en Inglés | MEDLINE | ID: mdl-25835877

RESUMEN

Advanced modulation formats combined with digital signal processing and direct detection is a promising way to realize high capacity, low cost and power efficient short reach optical transmission system. In this paper, we present a detailed investigation on the performance of three advanced modulation formats for 100 Gb/s short reach transmission system. They are PAM-4, CAP-16 and DMT. The detailed digital signal processing required for each modulation format is presented. Comprehensive simulations are carried out to evaluate the performance of each modulation format in terms of received optical power, transmitter bandwidth, relative intensity noise and thermal noise. The performance of each modulation format is also experimentally studied. To the best of our knowledge, we report the first demonstration of a 112 Gb/s transmission over 10km of SSMF employing single band CAP-16 with EML. Finally, a comparison of computational complexity of DSP for the three formats is presented.

20.
Opt Express ; 22(22): 27553-64, 2014 Nov 03.
Artículo en Inglés | MEDLINE | ID: mdl-25401902

RESUMEN

We propose a decision-aided algorithm to compensate the sampling frequency offset (SFO) between the transmitter and receiver for reduced-guard-interval (RGI) coherent optical (CO) OFDM systems. In this paper, we first derive the cyclic prefix (CP) requirement for preventing OFDM symbols from SFO induced inter-symbol interference (ISI). Then we propose a new decision-aided SFO compensation (DA-SFOC) algorithm, which shows a high SFO tolerance and reduces the CP requirement. The performance of DA-SFOC is numerically investigated for various situations. Finally, the proposed algorithm is verified in a single channel 28 Gbaud polarization division multiplexing (PDM) RGI CO-OFDM experiment with QPSK, 8 QAM and 16 QAM modulation formats, respectively. Both numerical and experimental results show that the proposed DA-SFOC method is highly robust against the standard SFO in optical fiber transmission.

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