A multi-functional binder for high loading sulfur cathode

Lithium sulfur(Li-S)batteries are the promising power sources,but their commercialization is significantly impeded by poor energy-storage functions at high sulfur loading.Here we report that such an issue can be effectively addressed by using a mussel-inspired binder comprised of chitosan grafted with catecholic moiety for sulfur cathodes.The resulting sulfur cathodes possess a high loading up to 12.2 mg cm-2 but also exhibit one of the best electrochemical properties among their counterparts.The excellent performances are attributed to the strong adhesion of the binder to sulfur particles,conducting agent,current collector,and polysulfide.The versatile adhesion effectively increases the sulfur loading,depresses the shuttle effect,and alleviates mechanical pulverization during cycling processes.The present investigation offers a new insight into high performance sulfur cathodes through a bio-adhesion viewpoint.

Controllable synthesis of high loading LiFePO_4/C nanocomposites using bimodal mesoporous carbon as support for high power Li-ion battery cathodes

Mesoporous LiFePO4/C composites containing 80 wt% of highly dispersed LiFePO4 nanoparticles(4-6 nm) were fabricated using bimodal mesoporous carbon(BMC) as continuous conductive networks. The unique pore structure of BMC not only promises good particle connectivity for LiFePO4, but also acts as a rigid nano-confinement support that controls the particle size. Furthermore, the capacities were investigated respectively based on the weight of LiFePO4 and the whole composite. When calculated based on the weight of the whole composite, it is 120 mAh·g-1at 0.1 C of the high loading electrode and 42 mAh·g-1at 10 C of the low loading electrode. The electrochemical performance shows that high LiFePO4 loading benefits large tap density and contributes to the energy storage at low rates, while the electrode with low content of LiFePO4 displays superior high rate performance, which can mainly be due to the small particle size, good dispersion and high utilization of the active material, thus leading to a fast ion and electron diffusion.

Oxygen vacancies with localized electrons direct a functionalized separator toward dendrite-free and high loading LiFePO_(4)for lithium metal batteries

The pursuit of high energy density has promoted the development of high-performance lithium metal batteries(LMBs).However,the underestimated but non-negligible dendrites of Li anode have been observed to shorten battery lifespan.Herein,a composite separator(TiO_(2-x)@PP),in which TiO_(2)with electron-localized oxygen vacancies(TiO_(2-x))is coated on a commercial PP separator,is fabricated to homogenize lithium ion transport and stabilize the lithium anode interface.With the utilization of TiO_(2-x)@PP separators,the symmetric lithium metal battery displays enhanced cycle stability over 800 h under a high current density of 8 m A cm^(-2).Moreover,the LMBs assembled with high-loading LiFePO_(4)(9.24 mg cm^(-2))deliver a stable cycling performance over 900 cycles at a rate of 0.5 C.Comprehensive theoretical studies based on density functional theory(DFT)further unveil the mechanism.The favorable TiO_(2-x)is beneficial for facilitating fast Li+migration and impeding anions transfer.In addressing the Li dendrite issues,the use of TiO_(2-x)@PP separator potentially provides a facile and attractive strategy for designing well-performing LMBs,which are expected to meet the application requirements of rechargeable batteries.

A strategy to achieve high loading and high energy density Li-S batteries

Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3 D free-standing sulfur cathode scaffold is rationally designed and fabricated by coaxially coating polar Ti_3 C_2 T_x flakes on sulfur-impregnated carbon cloth(Ti_3 C_2 T_x@S/CC) to achieve high loading and high energy density Li-S batteries,in which,the flexible CC substrate with highly porous structure can accommodate large amounts of sulfur and ensure fast electron transfer,while the outer-coated Ti_3 C_2 T_x can serve as a polar and conductive protective layer to further promote the conductivity of the whole electrode,achieve physical blocking and chemical anchoring of lithium-polysulfides as well as catalyze their conversion.Due to these advantages,at a sulfur loading of 4 mg cm^(-2),Li-S cells with Ti_3 C_2 T_x@S/CC cathodes can deliver outstanding cycling stability(746.1 mAh g^(-1) after 200 cycles at1 C),superb rate performance(866.8 mAh g^(-1) up to 2 C) and a high specific energy density(564.2 Wh kg^(-1) after 100 cycles at 0.5 C).More significantly,they also show the commercial potential that can compete with current lithium-ion batteries due to the high areal capacity of 6.7 mAh cm^(-2) at the increased loading of 8 mg cm^(-2).

Long-lasting,reinforced electrical networking in a high-loading Li_(2)S cathode for high-performance lithium–sulfur batteries

Realizing a lithium sulfide(Li_(2)S)cathode with both high energy density and a long lifespan requires an innovative cathode design that maximizes electrochemical performance and resists electrode deterioration.Herein,a high-loading Li_(2)S-based cathode with micrometric Li_(2)S particles composed of two-dimensional graphene(Gr)and one-dimensional carbon nanotubes(CNTs)in a compact geometry is developed,and the role of CNTs in stable cycling of high-capacity Li–S batteries is emphasized.In a dimensionally combined carbon matrix,CNTs embedded within the Gr sheets create robust and sustainable electron diffusion pathways while suppressing the passivation of the active carbon surface.As a unique point,during the first charging process,the proposed cathode is fully activated through the direct conversion of Li_(2)S into S_(8) without inducing lithium polysulfide formation.The direct conversion of Li_(2)S into S_(8) in the composite cathode is ubiquitously investigated using the combined study of in situ Raman spectroscopy,in situ optical microscopy,and cryogenic transmission electron microscopy.The composite cathode demonstrates unprecedented electrochemical properties even with a high Li_(2)S loading of 10 mg cm^(–2);in particular,the practical and safe Li–S full cell coupled with a graphite anode shows ultra-long-term cycling stability over 800 cycles.

Defect engineering of high-loading single-atom catalysts for electrochemical carbon dioxide reduction

Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides an attractive approach to carbon capture and utilization for the production high-value-added products.However,CO_(2)RR still suffers from poor selectivity and low current density due to its sluggish kinetics and multitudinous reaction pathways.Single-atom catalysts(SACs)demonstrate outstanding activity,excellent selectivity,and remarkable atom utilization efficiency,which give impetus to the search for electrocatalytic processes aiming at high selectivity.There appears significant activity in the development of efficient SACs for CO_(2)RR,while the density of the atomic sites remains a considerable barrier to be overcome.To construct high-metal-loading SACs,aggregation must be prevented,and thus novel strategies are required.The key to creating high-density atomically dispersed sites is designing enough anchoring sites,normally defects,to stabilize the highly mobile separated metal atoms.In this review,we summarized the advances in developing high-loading SACs through defect engineering,with a focus on the synthesis strategies to achieve high atomic site loading.Finally,the future opportunities and challenges for CO_(2)RR in the area of high-loading single-atom electrocatalysts are also discussed.

Liquid metal welding enabling high loading binder/carbon-free layered oxide cathode toward high-performance liquid and solid-state battery

High loading cathode with high active material proportion is a practical demand but far below the desirable value to achieve high energy density lithium-ion batteries(LIBs).Normally,the Li^(+)/electron transport between active materials and electrolyte/c arbon,however,it is poor and areal resistance is extremely high for a high loading/thick cathode.In this manuscript,taking high-voltage lithium cobalt oxide LiCoO_(2)(LCO)as an example,we design a facile liquid metal welding method enabled by a low melting-point indium-tin oxide In_(2)O_(3)/SnO_(2)(ITO)during a thermal treatment process,the strongly adhesion active particles show robust mechanical property for the free-standing LCO cathode with a pellet architecture.We also demonstrate that the O_(2)atmosphere plays a critical role on the interfacial property,that is preventing the layered structure to rock-salt Co_(3)O_(4)as well as further enhancing the interfacial mechanical integration.As expected,the LCO-ITO free-standing cathode not only shows robust mechanical property with densely packed configuration but also provides a fast Li^(+)/electron pathway at the interface.Consequently,the LCO-ITO composite cathode exhibits excellent electrochemical cycling performance in both liquid and solid-state cells.For example,even at a high active material mass of 56 mg·cm^(-2),the LCO cathode still delivers a specific capacity of 151 mAh·g^(-1)and maintains132.5 mAh·g^(-1)(corresponding to 7.4 mAh·cm^(-2))after 80cycles.The LCO-ITO-O_(2)cathode is also applicable to a solidstate cell,which exhibits a high capacity of 100.4 mAh·g^(-1)after 200 cycles of long-term cycling.The excellent electrochemical of the LCO-ITO-O_(2)reveals the successful engineering mechanical architecture and interfacial carriers transport,which may be expected as an alternative approach to achieve high energy density LIBs.

Construction of strong built-in electric field in binary metal sulfide heterojunction to propel high-loading lithium-sulfur batteries

The practical application of lithium-sulfur(Li-S)batteries is greatly hindered by soluble polysulfides shuttling and sluggish sulfur redox kinetics.Rational design of multifunctional hybrid materials with superior electronic conductivity and high electrocatalytic activity,e.g.,heterostructures,is a promising strategy to solve the above obstacles.Herein,a binary metal sulfide MnS-MoS_(2) heterojunction electrocatalyst is first designed for the construction of high-sulfur-loaded and durable Li-S batteries.The MnS-MoS_(2) p-n heterojunction shows a unique structure of MoS_(2) nanosheets decorated with ample MnS nanodots,which contributes to the formation of a strong built-in electric field at the two-phase interface.The MnS-MoS_(2) hybrid host shows strong soluble polysulfide affinity,enhanced electronic conductivity,and exceptional catalytic effect on sulfur reduction.Benefiting from the synergistic effect,the as-derived S/MnS-MoS_(2) cathode delivers a superb rate capability(643 m A h g^(-1)at 6 C)and a durable cyclability(0.048%decay per cycle over 1000 cycles).More impressively,an areal capacity of 9.9 m A h cm^(-2)can be achieved even under an extremely high sulfur loading of 14.7 mg cm^(-2)and a low electrolyte to sulfur ratio of 2.9μL mg^(-1).This work provides an in-depth understanding of the interfacial catalytic effect of binary metal compound heterojunctions on sulfur reaction kinetics.

High drug loading hydrophobic cross-linked dextran microspheres as novel drug delivery systems for the treatment of osteoarthritis

Drug delivery via intra-articular(IA)injection has proved to be effective in osteoarthritis(OA)therapy,limited by the drug efficiency and short retention time of the drug delivery systems(DDSs).Herein,a series of modified cross-linked dextran(Sephadex,S0)was fabricated by respectively grafting with linear alkyl chains,branched alkyl chains or aromatic chain,and acted as DDSs after ibuprofen(Ibu)loading for OA therapy.This DDSs expressed sustained drug release,excellent anti-inflammatory and chondroprotective effects both in IL-1βinduced chondrocytes and OA joints.Specifically,the introduction of a longer hydrophobic chain,particularly an aromatic chain,distinctly improved the hydrophobicity of S0,increased Ibu loading efficiency,and further led to significantly improving OA therapeutic effects.Therefore,hydrophobic microspheres with greatly improved drug loading ratio and prolonged degradation rates show great potential to act as DDSs for OA therapy.

High loading Pt nanoparticles on ordered mesoporous carbon sphere arrays for highly active methanol electro-oxidation

Three-dimensionally（3D） ordered mesoporous carbon sphere arrays（OMCS） are explored to support high loading（60 wt%） Pt nanoparticles as electrocatalysts for the methanol oxidation reaction（MOR）.The OMCS has a unique hierarchical nanostructure with ordered large mesopores and macropores that can facilitate high dispersion of the Pt nanoparticles and fast mass transport during the reactions. The prepared Pt/OMCS exhibits uniformly dispersed Pt nanoparticles with an average size of- 2.0 nm on the mesoporous walls of the carbon spheres. The Pt/OMCS catalyst shows significantly enhanced specific electrochemically active surface area（ECSA）（73.5 m^2g^-1） and electrocatalytic activity（0.69 mA cm^-2）for the MOR compared with the commercial 60 wt% Pt/C catalyst.

Microwave-assisted synthesis of ultrafine Au nanoparticles immobilized on MOF-199 in high loading as efficient catalysts for a three-component coupling reaction

Controlled integration of ultrafine metal nanoparticles （MNPs） and metal- organic frameworks （MOFs） has drawn much attention due to their unique physical and chemical properties. However, the development of a one-step strategy for preparing ultrafine MNPs within MOFs still remains a great challenge. Herein, a facile synthetic approach toward the abovementioned composites was developed. In contrast to the conventional approach, these hybrids were prepared by the direct mixing of metal and MOF precursors in the reaction solution assisted by microwave irradiation. Impressively, the Au/MOF-199 composite with uniformly distributed ultrafine Au nanoparticles could be fabricated in only two minutes, and the Au loading could be increased up to a level of 5.13%. The multifunctional Au/MOF-199 catalysts exhibited high turnover numbers （TONs） and turnover frequencies （TOFs） in the three-component coupling reaction of formaldehyde, phenylacetylene, and piperidine （AB-coupling）. Owing to the confinement effect of MOF-199, the 5.13%Au/MOF-199 catalyst could be recycled for five runs without serious loss of activity, with no obvious aggregation of Au NPs detected.

Towards full demonstration of high areal loading sulfur cathode in lithium–sulfur batteries

Lithium–sulfur(Li–S)batteries have been recognized as promising substitutes for current energy-storage technologies owing to their exceptional advantages in very high-energy density and excellent material sustainability.The cathode with high sulfur areal loading is vital for the practical applications of Li–S batteries with very high energy density.However,the high sulfur loading in an electrode results in poor rate and cycling performances of batteries in most cases.Herein,we used diameters of 5.0(D5)and 13.0(D13)mm to probe the effect of electrodes with different sizes on the rate and cycling performances under a high sulfur loading(4.5 mg cm^-2).The cell with D5 sulfur cathode exhibits better rate and cycling performances comparing with a large(D13)cathode.Both the high concentration of lithium polysulfides and corrosion of lithium metal anode impede rapid kinetics of sulfur redox reactions,which results in inferior battery performance of the Li–S cell with large diameter cathode.This work highlights the importance of rational matching of the large sulfur cathode with a high areal sulfur loading,carbon modified separators,organic electrolyte,and Li metal anode in a pouch cell,wherein the sulfur redox kinetics and lithium metal protection should be carefully considered under the flooded lithium polysulfide conditions in a working Li–S battery.

Comprehensive Design of the High-Sulfur-Loading Li–S Battery Based on MXene Nanosheets

The lithium-sulfur battery is the subject of much recent attention due to the high theoretical energy density,but practical applications are challenged by fast decay owing to polysulfide shuttle and electrode architecture degradation.A comprehensive study of the sulfur host microstructure design and the cell architecture construction based on the MXene phase(Ti3C2Tx nanosheets) is performed,aiming at realize stable cycling performance of Li-S battery with high sulfur areal loading.The interwoven KB@Ti3C2Tx composite formed by self-assembly of MXene and Ktej en black,not only provides superior conductivity and maintains the electrode integrality bearing the volume expansion/shrinkage when used as the sulfur host,but also functions as an interlayer on separator to further retard the polysulfide cross-diffusion that possibly escaped from the cathode.The KB@Ti3C2Tx interlayer is only 0.28 mg cm-2 in areal loading and 3 μm in thickness,which accounts a little contribution to the thick sulfur electrode;thus,the impacts on the energy density is minimal.By coupling the robust KB@Ti3C2Tx cathode and the effective KB@Ti3C2Tx modified separator,a stable Li-S battery with high sulfur areal loading(5.6 mg cm-2) and high areal capacity(6.4 mAh cm-2) at relatively lean electrolyte is achieved.

High-loading Pt-alloy catalysts for boosted oxygen reduction reaction performance

To improve performance of membrane electrode assembly(MEA)at large current density region,efficient mass transfer at the cathode is desired,for which a feasible strategy is to lower catalyst layer thickness by constructing high loading Pt-alloy catalysts on carbon.But the high loading may induce unwanted par-ticle aggregation.In this work,H-PtNi/C with 33%(mass)Pt loading on carbon and monodisperse distri-bution of 3.55 nm PtNi nanoparticles,was prepared by a bimodal-pore route.In electrocatalytic oxygen reduction reaction(ORR),H-PtNi/C displays an activity inferior to the low Pt loading catalyst L-PtNi/C(13.3%(mass))in the half-cell.While in H_(2)-0_(2) MEA,H-PtNi/C delivers the peak power density of 1.51 W·cm^(-2) and the mass transfer limiting current density of 4.4 A·cm^(-2),being 21%and 16%higher than those of L-PtNi/C(1.25 W·cm^(-2),3.8 A·cm^(-2))respectively,which can be ascribed to enhanced mass trans-fer brought by the thinner catalyst layer in the former.In addition,the same method can be used to pre-pare PtFe alloy catalyst with a high-Pt loading of 36%(mass).This work may lead to a range of catalyst materials for the large current density applications,such as fuel cell vehicles.

Hot Spot in Materials with Structural Defects under High Shear Loading Rates

The response of three-dimensional sample of Al, containing vacancy complex, under shear loading was simulated. The molecular dynamics method was used and interaction between atoms was described on the base of pseudopotential theory Solitary waves were generated in the sample under mechanical loading. Their interaction with the vacancy complexes was shown to be able to initiate hot spot in that local region of the complexes. Some parameters of the hot spot as well as solitary waves were calculated. The initiation of the hot spot is accompanied with sufficient local structural relaxation.

A fast approach to optimize dye loading of photoanode via ultrasonic technique for highly efficient dye-sensitized solar cells

A distinctive method is proposed by simply utilizing ultrasonic technique in Ti02 electrode fabrication in order to improve the optoelectronic performance of dye-sensitized solar cells （DSSCs）. Dye molecules are at random and single molecular state in the ultrasonic field and the ultrasonic wave favors the diffusion and adsorption processes of dye molecules. As a result, the introduction of ultrasonic technique at room temperature leads to faster and more well-distributed dye adsorption on TiO2 as well as higher cell efficiency than regular deposition, thus the fabrication time is markedly reduced. It is found that the device based on 40 kHz ultrasonic （within 1 h） with N719 exhibits a Voc of 789 mV, Jsc of 14.94 mA]cm2 and fill factor （FF） of 69.3, yielding power conversion efficiency （PCE） of 8.16%, which is higher than device regularly dyed for 12 h （PCE = 8.06%）. In addition, the DSSC devices obtain the best efficiency （PCE = 8.68%） when the ultrasonic deposition time increases to 2.5 h. The DSSCs fabricated via ultrasonic technique presents more dye loading, larger photocurrent, less charge recombination and higher photovoltage. The charge extraction and electron impedance spectroscopy （EIS） were performed to understand the influence of ultrasonic technique on the electron recombination and performance of DSSCs.

High mass loading NiCo_(2)O_(4) with shell-nanosheet/core-nanocage hierarchical structure for high-rate solid-state hybrid supercapacitors

Rational design of advanced structure for transition metal oxides(TMOs) is attractive for achieving high-performance supercapacitors.However, it is hampered by sluggish reaction kinetics, low mass loading, and volume change upon cycling. Herein, hierarchical Ni Co_(2)O_(4) architectures with 2D-nanosheets-shell and 3D-nanocages-core(2D/3D h-NCO) are directly assembled on nickel foam via a facile one-step way.The 2D nanosheets are in-situ generated from the self-evolution of initial NCO nanospheres. This 2D/3D hierarchical structures ensure fast ion/electron transport and maintain the structural integrity to buffer the volume expansion. The 2D/3D h-NCO electrode with an ultrahigh mass loading(30 mg cm^(-2)) achieves a high areal capacity of 4.65 C cm^(-2)(equivalent to 1.29 mAh cm^(-2)) at a current density of 4 mA cm^(-2), and retains 3.7 C cm^(-2) even at 50 mA cm^(-2). Furthermore, the assembled solid-state hybrid supercapacitor yields a high volumetric energy density of 4.25 mWh cm^(-3) at a power density of 39.3 mW cm^(-3), with a high capacity retention of 92.4% after 5000 cycles. Therefore, this work provides a new insight to constuct hierarchical electrodes for energy storage application.

Computer Simulation of Plastic Deformation in GrainBoundary Region under High Rate Loading

The computer simulation of Al three-dimensional crystallite containing grain boundary of special type was carried out and its behaviour under high rate loading was investigated. The molecular dynamics method was used and interaction betwen atoms was described based on pseudopotential method. Vortical character of the atom movements in the grain boundary region is realized under shear loading in certain directions. Back and forth movements of atoms in the direction which is perpendicular to the shear also arise. Amplitude of such movements is approximately equal to an interplanar distance in this direction.

Sustainable Lignin-Derived Carbon as Capacity-Kinetics Matched Cathode and Anode towards 4.5 V High-Performance Lithium-Ion Capacitors

The Li-ion capacitors(LICs)develop rapidly due to their double-high features of high-energy density and high-power density.However,the relative low capacity of cathode and sluggish kinetics of anode seriously impede the development of LICs.Herein,the precisely pore-engineered and heteroatomtailored defective hierarchical porous carbons(DHPCs)as large-capacity cathode and high-rate anode to construct high-performance dual-carbon LICs have been developed.The DHPCs are prepared based on triple-activation mechanisms by direct pyrolysis of sustainable lignin with urea to generate the interconnected hierarchical porous structure and plentiful heteroatominduced defects.Benefiting from these advanced merits,DHPCs show the well-matched high capacity and fast kinetics of both cathode and anode,exhibiting large capacities,superior rate capability and long-term lifespan.Both experimental and computational results demonstrate the strong synergistic effect of pore and dopants for Li storage.Consequently,the assembled dual-carbon LIC exhibits high voltage of 4.5 V,high-energy density of 208 Wh kg^(−1),ultrahigh power density of 53.4 kW kg^(−1)and almost zerodecrement cycling lifetime.Impressively,the full device with high mass loading of 9.4 mg cm^(−2)on cathode still outputs high-energy density of 187 Wh kg^(−1),demonstrative of their potential as electrode materials for high-performance electrochemical devices.

Combustion Properties of Some High Solid Loading Butalites Compositions

The combustion （ballistic） properties of a high solid loading composite solid propellant family （Butalites） was studied experimentally by using propellant formulations based on hydroxy-terminated polybutadiene pre-polymer （HTPB） as a fuel binder main backbone, bimodal system ammonium perchlorate oxidizer （AP） and aluminum powder （AI） as metallic fuel. Burning rates were doubled at various pressures, when solids loading （AP and 17% A1） were increased from 80 to 88% and the measured characteristic velocity values were increased by about 100m/sec. The pressure exponent （n） values were lower with 80-85% solids loading. The burning rates were increased by about 2-5% when comparing the data obtained by static firing with those obtained by the strand burner method.