Lithium–sulfur (Li–S) batteries are regarded as promising next-generation high energy density storage devices for both portable electronics and electric vehicles due to their high energy density, low cost, and environmental friendliness. However, there remain some issues yet to be fully addressed with the main challenges stemming from the ionically insulating nature of sulfur and the dissolution of polysulfides in electrolyte with subsequent parasitic reactions leading to low sulfur utilization and poor cycle life. The high flammability of sulfur is another serious safety concern which has hindered its further application. Herein, an aqueous inorganic polymer, ammonium polyphosphate (APP), has been developed as a novel multifunctional binder to address the above issues. The strong binding affinity of the main chain of APP with lithium polysulfides blocks diffusion of polysulfide anions and inhibits their shuttling effect. The coupling of APP with Li ion facilitates ion transfer and promotes the kinetics of the cathode reaction. Moreover, APP can serve as a flame retardant, thus significantly reducing the flammability of the sulfur cathode. In addition, the aqueous characteristic of the binder avoids the use of toxic organic solvents, thus significantly improving safety. As a result, a high rate capacity of 520 mAh g–1 at 4 C and excellent cycling stability of ∼0.038% capacity decay per cycle at 0.5 C for 400 cycles are achieved based on this binder. This work offers a feasible and effective strategy for employing APP as an efficient multifunctional binder toward building next-generation high energy density Li–S batteries.
Heterostructure engineering is one of the most promising modification strategies toward improving sluggish kinetics for the anode of sodium ion batteries (SIBs). Herein, we report a systemic investigation on the different types of heterostructure interfaces’ effects of discharging products (Na2O, Na2S, Na2Se) on the rate performance. First-principle calculations reveal that the Na2S/Na2Se interface possesses the lowest diffusion energy barrier (0.39 eV) of Na among three kinds of interface structures (Na2O/Na2S, Na2O/Na2Se, and Na2S/Na2Se) due to its smallest recorded interface deformation, similar electronegativity, and lattice constant. The experimental evidence confirms that the metal sulfide/metal selenide (SnS/SnSe2) hierarchical anode exhibits outstanding rate performance, where the normalized capacity at 10 A g–1 compared to 0.1 A g–1 is 45.6%. The proposed design strategy in this work is helpful to design high rate performance anodes for advanced battery systems.
Sulfur is an attractive cathode material for next-generation lithium batteries due to its high theoretical capacity and low cost. However, dissolution of its lithiated product (lithium polysulfides) into the electrolyte limits the practical application of lithium sulfur batteries. Here we demonstrate that sulfur particles can be hermetically encapsulated by leveraging on the unique properties of two-dimensional materials such as molybdenum disulfide (MoS). The high flexibility and strong van der Waals force in MoS nanoflakes allows effective encapsulation of the sulfur particles and prevent its sublimation during in situ TEM studies. We observe that the lithium diffusivities in the encapsulated sulfur particles are in the order of 10 m s. Composite electrodes made from the MoS-encapsulated sulfur spheres show outstanding electrochemical performance, with an initial capacity of 1660 mAh g and long cycle life of more than 1000 cycles.
Electrocatalysis represents a promising method to generate renewable fuels and chemical feedstock from the carbon dioxide reduction reaction (CO 2 RR). However, traditional electrocatalysts based on transition metals are not efficient enough because of the high overpotential and slow turnover. MXenes, a family of two-dimensional metal carbides and nitrides, have been predicted to be effective in catalyzing CO 2 RR, but a systematic investigation into their catalytic performance is lacking, especially on hydroxyl (−OH)-terminated MXenes relevant in aqueous reaction conditions. In this work, we utilized first-principles simulations to systematically screen and explore the properties of MXenes in catalyzing CO 2 RR to CH 4 from both aspects of thermodynamics and kinetics. Sc 2 C(OH) 2 was found to be the most promising catalyst with the least negative limiting potential of −0.53 V vs RHE. This was achieved through an alternative reaction pathway, where the adsorbed species are stabilized by capturing H atoms from the MXene's OH termination group. New scaling relations, based on the shared H interaction between intermediates and MXenes, were established. Bader charge analyses reveal that catalysts with less electron migration in the *(H)COOH → *CO elementary step exhibit better CO 2 RR performance. This study provides new insights regarding the effect of surface functionalization on the catalytic performance of MXenes to guide future materials design.
3D macroporous hierarchical Ag-G-NCF can efficiently convert CO2 to ethanol with a low overpotential, high faradaic efficiency and high selectivity.
hydrogen electrode). [5,6] In fact, lithium metal has been applied in space exploration, petroleum prospecting in 1970s. However, the further application of LMB is plagued with practical issues that puzzled researchers for more than 40 years. [7,8] The most critical issue is that deposition of lithium metal tends to be highly dendritic during the repeated plating and dissolution process, which not only continue to consume the electrolyte and induce the "dead lithium" leading to capacity fading, but also face the severe safety problems of short-circuit due to the crack of separator by continuous ramified growth of lithium dendrites. [9,10] During the past half-century, many up-and-coming methods have been carried out to suppress dendrite growth and achieved partially success. These strategies can be broadly divided into three areas: i) electrolyte modification (such as selfhealing electrostatic shield mechanism by inducing Cs + , [11] replacing traditional liquid electrolyte by solid state electrolyte [12] ), ii) artificial solidelectrolyte interphase (SEI) (such as manufacturing the Li 3 N, [13] LiF, [14] Li-Sn alloy [15] layers to improve the mechanical strength, ionic diffusion performance, and stability to suppress the dendrite); iii) the multifunctional nanostructured anodes design to manipulate the nucleation of lithium (such as Ni foam, [16] 3D skeleton Cu matrix, [17] Cu-Zn alloy matrix [18] ). The former two strategies are based primarily on suppressing the protrusions, while the last one mainly focuses on modulating the initial nucleation process of dendrite, before the extension of dendrites into the electrolyte. Designing the excellent LMB requires the joint effort of these methods. However, if we can eliminate or mitigate the lithium dendrite from the initial nucleation process, it will be a highly efficient and convenient measure for its industrial production. Thus, finding an ideal nucleating anode material is very important to solve the dendrite problem.Based on Chazalviel's theory, [19,20] designing high-surface area anode can suppress the local current density and thus improve the electrical performance. Graphene, who possesses very high specific surface area, shows great advantage on its potential application in lithium metal anode field. [21][22][23] However, the pristine graphene (PG) shows poor performances in the actual application. [24][25][26] Doping or modulating the graphene can adjust its performance which has already made some Lithium metal is the most promising anode material for next-generation batteries, owing to its high theoretical specific capacity and low electrochemical potential. However, the practical application of lithium metal batteries (LMBs) has been plagued by the issues of uncontrollable lithium deposition. The multifunctional nanostructured anode can modulate the initial nucleation process of lithium before the extension of dendrites. By combing the theoretical design and experimental validation, a novel nucleation strategy is developed by introducing sulfur (S) to gr...
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