Covalent organic frameworks (COF) possess a robust and porous crystalline structure, making them an appealing candidate for energy storage. Herein, we report an exfoliated polyimide COF composite ...(P‐COF@SWCNT) prepared by an in situ condensation of anhydride and amine on the single‐walled carbon nanotubes as advanced anode for potassium‐ion batteries (PIBs). Numerous active sites exposed on the exfoliated frameworks and the various open pathways promote the highly efficient ion diffusion in the P‐COF@SWCNT while preventing irreversible dissolution in the electrolyte. During the charging/discharging process, K+ is engaged in the carbonyls of imide group and naphthalene rings through the enolization and π‐K+ effect, which is demonstrated by the DFT calculation and XPS, ex‐situ FTIR, Raman. As a result, the prepared P‐COF@SWCNT anode enables an incredibly high reversible specific capacity of 438 mA h g−1 at 0.05 A g−1 and extended stability. The structural advantage of P‐COF@SWCNT enables more insights into the design and versatility of COF as an electrode.
We prepare a polyimide covalent organic framework composite anode by effective in‐situ condensation of anhydride and amine on the surface of single‐walled carbon nanotubes. The construction of the conductive network accelerates the transport of electron. Dual electroactive sites in the framework, carbonyls and aromatic naphthalene rings, could store more potassium ions by the enolization and π‐K+ effect.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Hard carbon is regarded as a promising anode material for sodium‐ion batteries (SIBs). However, it usually suffers from the issues of low initial Coulombic efficiency (ICE) and poor rate performance, ...severely hindering its practical application. Herein, a flexible, self‐supporting, and scalable hard carbon paper (HCP) derived from scalable and renewable tissue is rationally designed and prepared as practical additive‐free anode for room/low‐temperature SIBs with high ICE. In ether electrolyte, such HCP achieves an ICE of up to 91.2% with superior high‐rate capability, ultralong cycle life (e.g., 93% capacity retention over 1000 cycles at 200 mA g−1) and outstanding low‐temperature performance. Working mechanism analyses reveal that the plateau region is the rate‐determining step for HCP with a lower electrochemical reaction kinetics, which can be significantly improved in ether electrolyte.
A self‐supporting, flexible, additive‐free and scalable hard carbon paper (HCP) derived from tissue is rationally developed, and it achieves outstanding Na‐storage properties in terms of high initial Coulombic efficiency (91.2%), superior high‐rate capability, ultralong cyclic stability, as well as outstanding low‐T performance in ether electrolyte. More significantly, the Na‐storage and capacity attenuation mechanism of the HCP anode is revealed.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Impossible voltage plateau regulation for the cathode materials with fixed active elemental center is a pressing issue hindering the development of Na‐superionic‐conductor (NASICON)‐type ...Na3V2(PO4)2F3 (NVPF) cathodes in sodium‐ion batteries (SIBs). Herein, a high‐entropy substitution strategy, to alter the detailed crystal structure of NVPF without changing the central active V atom, is pioneeringly utilized, achieving simultaneous electronic conductivity enhancement and diffusion barrier reduction for Na+, according to theoretical calculations. The as‐prepared carbon‐free high‐entropy Na3V1.9(Ca,Mg,Al,Cr,Mn)0.1(PO4)2F3 (HE‐NVPF) cathode can deliver higher mean voltage of 3.81 V and more advantageous energy density up to 445.5 Wh kg−1, which is attributed by the diverse transition‐metal elemental substitution in high‐entropy crystalline. More importantly, high‐entropy introduction can help realize disordered rearrangement of Na+ at Na(2) active sites, thereby to refrain from unfavorable discharging behaviors at low‐voltage region, further lifting up the mean working voltage to realize a full Na‐ion storage at the high voltage plateau. Coupling with a hard carbon (HC) anode, HE‐NVPF//HC SIB full cells can deliver high specific energy density of 326.8 Wh kg−1 at 5 C with the power density of 2178.9 W kg−1. This route means the unlikely potential regulation in NASICON‐type crystal with unchangeable active center becomes possible, inspiring new ideas on elevating the mean working voltage for SIB cathodes.
A high‐entropy effect is delicately introduced into fluorophosphate cathode for sodium‐ion batteries by in situ partial substitution of active V central atom, preparing a high‐entropy carbon‐free Na3V1.9(Ca,Mg,Al,Cr,Mn)0.1(PO4)2F3 cathode, suppressing the occurrence of detrimental phase transition process in the low‐voltage region, and further lifting up the mean working voltage of pristine Na3V2(PO4)2F3, enhancing sodium storage behavior, rate capability, and cycle performance.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Conventional ion batteries utilizing metallic ions as the single charge carriers are limited by the insufficient abundance of metal resources. Although supercapacitors apply both cations and anions ...to store energy through absorption and/or Faradic reactions occurring at the interfaces of the electrode/electrolyte, the inherent low energy density hinders its application. The graphite‐cathode‐based dual‐ion battery possesses a higher energy density due to its high working potential of nearly 5 V. However, such a battery configuration suffers from severe electrolyte decomposition and exfoliation of the graphite cathode, rendering an inferior cycle life. Herein, a new surface‐modification strategy is developed to protect the graphite cathode from the anion salvation effect and the deposition derived from electrolyte decomposition by generating an artificial solid electrolyte interphase (SEI). Such SEI‐modified graphite exhibits superior cycling stability with 96% capacity retention after 500 cycles under 200 mA g−1 at the upper cutoff voltage of 5.0 V, which is much improved compared with the pristine graphite electrode. Through several ex situ studies, it is revealed that the artificial SEI greatly stabilizes the interfaces of the electrode/electrolyte after reconstruction and gradual establishment of the optimal anion‐transport path. The findings shed light on a new avenue toward promoting the performance of the dual‐ion battery (DIB) and hence to make it practical finally.
An artificial layer of a solid electrolyte interphase is fabricated on a graphite cathode for a dual‐ion battery (DIB). Such surface modification can alleviate the electrolyte decomposition at the high working voltage of the anion de‐/intercalation processes and the solvation effect of anions, much improving the cycling stability of the Li//graphite DIB.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
As a cathode for sodium‐ion batteries (SIBs), Na3V2(PO4)2F3 (NVPF) with 3D open framework is a promising candidate due to its high working voltage and large theoretical capacity. However, the severe ...capacity degradation and poor rate capability hinder its practical applications. The present study demonstrated the optimization of Na‐storage performance of NVPF via delicate lattice modulation. Aliovalent substitution of V3+ at Na+ in NVPF induces the generation of electronic defects and expansion of Na+‐migration channels, resulting in the enhancement in electronic conductivity and acceleration of Na+‐migration kinetics. It is disclosed that the formed stronger NaO bonds with high ionicity than VO bonds lead to the significant increase in structural stability and ionicity in the Na+‐substituted NVPF (NVPF‐Nax). The aforementioned effects of Na+ substitution achieve the unprecedented electrochemical performance in the optimized Na3.14V1.93Na0.07(PO4)2F3 (NVPF‐Na0.07). As a result, NVPF‐Na0.07 delivers a high‐rate capability (77.5 mAh g−1 at 20 C) and ultralong cycle life (only 0.027% capacity decay per cycle over 1000 cycles at 10 C). Sodium‐ion full cells are designed using NVPF‐Na0.07 as cathode and Se@reduced graphene oxide as anode. The full cells exhibit excellent wide‐temperature electrochemical performance from −25 to 25°C with an outstanding rate capability (96.3 mAh g−1 at 20 C). Furthermore, it delivered an excellent cycling performance over 300 cycles with a capacity retention exceeding 90% at 0.5 C under different temperatures. This study demonstrates a feasible strategy for the development of advanced cathode materials with excellent electrochemical properties to achieve high‐efficiency energy storage.
An advanced Na3.14V1.93Na0.07(PO4)2F3 cathode with high ionicity and excellent energy‐storage performance is prepared via aliovalent substitution of V3+ at Na+ sites. It exhibits the higher structural stability and improved electron/ion‐transport kinetics than the pristine Na3V2(PO4)2F3 owing to the stronger NaO and VO bonds, thereby extending the cycle life of NASICON cathode materials.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
There are still many problems that hinder the development of sodium‐ion batteries (SIBs), including poor rate performance, short‐term cycle lifespan, and inferior low‐temperature property. Herein, ...excellent Na‐storage performance in fluorophosphate (Na3V2(PO4)2F3) cathode is achieved by lattice regulation based on charge balance theory. Lattice regulation of aliovalent Mn2+ for V3+ increases both electronic conductivity and Na+‐migration kinetics. Because of the maintaining of electrical neutrality in the material, aliovalent Mn2+‐introduced leads to the coexistence of V3+ and V4+ from charge balance theory. It decreases the particle size and improves the structural stability, suppressing the large lattice distortion during cathode reaction processes. These multiple effects enhance the specific capacity (123.8 mAh g−1), outstanding high‐rate (68% capacity retention at 20 C), ultralong cycle (only 0.018% capacity attenuation per cycle over 1000 cycles at 1 C) and low‐temperature (96.5% capacity retention after 400 cycles at −25 °C) performances of Mn2+‐induced Na3V1.98Mn0.02(PO4)2F3 when used as cathode in SIBs. Importantly, a feasible sodium‐ion full battery is assembled, achieving outstanding rate capability and cycle stability. The strategy of aliovalent ion‐induced lattice regulation constructs cathode materials with superior performances, which is available to improve other electrode materials for energy storage systems.
An advanced Na3V1.98Mn0.02(PO4)2F3 cathode with excellent energy‐storage performance is prepared via aliovalent substitution of V3+ at Mn2+ sites. It exhibits higher structural stability and improved electron/ion‐transport kinetics than pristine Na3V2(PO4)2F3 owing to aliovalent Mn2+ induced lattice regulation based on charge balance theory leads to the coexistence of V3+/4+, thereby extending the cycle life of NASICON cathode materials.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
In this paper, we investigate physical-layer security of the uplink millimeter wave communications for a cellular vehicle-to-everything (C-V2X) network comprised of a large number of base stations ...(BSs) and different categories of V2X nodes, including vehicles, pedestrians, and road side units. Considering the dynamic change and randomness of the topology of the C-V2X network, we model the roadways, the V2X nodes on each roadway, and the BSs by a Poisson line process, a 1D Poisson point process (PPP), and a 2D PPP, respectively. We propose two uplink association schemes for a typical vehicle, namely, the smallest-distance association (SDA) scheme and the largest-power association (LPA) scheme, and we establish a tractable analytical framework to comprehensively assess the security performance of the uplink transmission, by leveraging the stochastic geometry theory. Specifically, for each association scheme, we first obtain new expressions for the association probability of the typical vehicle, and then derive the overall connection outage probability and secrecy outage probability by calculating the Laplace transform of the aggregate interference power. Numerical results are presented to validate our theoretical analysis, and we also provide interesting insights into how the security performance is influenced by various system parameters, including the densities of V2X nodes and BSs. Moreover, we show that the LPA scheme outperforms the SDA scheme in terms of secrecy throughput.
Flexible power sources featuring high-performance, prominent flexibility and raised safety have received mounting attention in the area of wearable electronic devices. However, many great challenges ...remain to be overcome, notably the design and fabrication of flexible electrodes with excellent electrochemical performance and matching them with safe and reliable electrolytes. Herein, a facile approach for preparing flexible electrodes, which employs carbon cloth derived from commercial cotton cloth as the substrate of cathode and a flexible anode, is proposed and investigated. The promising cathode (NVPOF@FCC) with high conductivity and outstanding flexibility is prepared by efficiently coating Na
3
V
2
(PO
4
)
2
O
2
F (NVPOF) on flexible carbon cloth (FCC), which exhibits remarkable electrochemical performance and the significantly improved reaction kinetics. More importantly, a novel flexible quasi-solid-state sodium-ion full battery (QSFB) is feasibly assembled by sandwiching a P(VDF-HFP)-NaClO
4
gel-polymer electrolyte film between the advanced NVPOF@FCC cathode and FCC anode. And the QSFBs are further evaluated in flexible pouch cells, which not only demonstrates excellent energy-storage performance in aspect of great cycling stability and high-rate capability, but also impressive flexibility and safety. This work offers a feasible and effective strategy for the design of flexible electrodes, paving the way for the progression of practical and sustainable flexible batteries.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Metal oxide semiconductor heterojunctions (MOSHs) can enhance the performance of ethanol gas sensors substantially. Ethanol gas sensors based on MOSHs are cost-effective and have excellent sensing ...response, good selectivity, fast response and recovery, long-term stability or repeatability, a low operating temperature, a facile fabrication process, and versatile applications. This paper reviews the recent advances in gas sensors that are based on MOSHs and the advantages of using them to detect ethanol gas. According to the literature, compared with ethanol gas sensors that use single-component sensing materials, the MOSHs exhibit superior performance due to the synergy between the different components, which can amplify the reception and transduction components of the sensor signals. To the best of our knowledge, heterojunctions can be grouped into four main categories as metal oxide/metal oxide, metal oxide/metal sulfide, metal oxide/noble metal, and metal oxide/other materials, including rare-earth metals, g-C
3
N
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, and graphene, heterojunctions. The future trends and challenges that would be faced in the development of ethanol gas sensors based on MOSHs are discussed in detail. Finally, critical ideas and thinking regarding the future progress of MOSH-based gas sensors are presented.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Acute infection, if not kept in check, can lead to systemic inflammatory responses in the brain. Here, we show that within 2 hr of systemic inflammation, PDGFRβ mural cells of blood vessels rapidly ...secrete chemokine CCL2, which in turn increases total neuronal excitability by promoting excitatory synaptic transmission in glutamatergic neurons of multiple brain regions. By single-cell RNA sequencing, we identified Col1a1 and Rgs5 subgroups of PDGFRβ cells as the main source of CCL2. Lipopolysaccharide (LPS)- or Poly(I:C)-treated pericyte culture medium induced similar effects in a CCL2-dependent manner. Importantly, in Pdgfrb-Cre;Ccl2fl/fl mice, LPS-induced increase in excitatory synaptic transmission was significantly attenuated. These results demonstrate in vivo that PDGFRβ cells function as initial sensors of external insults by secreting CCL2, which relays the signal to the central nervous system. Through their gateway position in the brain, PDGFRβ cells are ideally positioned to respond rapidly to environmental changes and to coordinate responses.
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•PDGFRβ cells function as initial sensors of systemic inflammation in the brain•PDGFRβ cells relay the infection signal to neurons by secreting chemokine CCL2•Col1a1 and Rgs5 subgroups of PDGFRβ cells are sources of Ccl2 during early infection•PDGFRβ-specific Ccl2 knockout blocked LPS-induced increase in synaptic transmission
Yu and colleagues identified Rgs5 and Col1a1 subgroups of PDGFRβ cells as early responders to neuroinflammation. These cells rapidly synthesize and release the chemokine CCL2, which in term elevates neuronal excitability and excitatory synaptic transmission in multiple neuronal types.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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