Binder-free S@Ti3C2Tx sandwich structure film as a high-capacity cathode for a stable aluminum-sulfur battery

Zheng

Chen

et al. 2022

ACS Materials Lett.

Self Cite

As an alternative energy storage system, the stable cycle and high-rate performance of aluminum–sulfur (Al–S) batteries are increasingly affected by the dissolution of intermediate Al polysulfide (Al2S n ) into the electrolyte. Introducing anchoring materials that can promote Al2S n conversion is an effective way to solve this problem. However, the lack of an interaction mechanism between Al2S n and anchoring materials hinders the design of anchoring materials. Here, we used single-atom-loaded MXene (SA@MXene) as a representative anchoring material to systematically investigate the binding strength between SA@MXene and Al2S n , the sulfur reduction process on MXene, and their geometric configurations, stabilities, and electronic structures. We evaluated the reaction activity of the various SA@MXene nanosheets and discovered four high-performance cathode candidates for Al–S batteries (SA = Y, Nb, Mo, Tc) with a minimum reaction energy barrier of 0.23 eV. Importantly, to unravel the interaction mechanism between Al2S n and the anchoring material, we proposed an activity volcano by consolidating the decisive S8*, Al2S8*, and Al2S12* binding strengths, which provides a significant roadmap for designing cathodes for Al–S batteries. The proposed study of the Al–S conversion process will benefit the understanding of sulfur chemistry and provide valuable inspiration for the design of other catalytic reaction processes.

mentioning

confidence: 72%

“…12,32,33 The process of charging and discharging proceeding through the formation of Al 2 S n can be described as eqs 3 and 4. 10,22 + + 2Al 14AlCl 8Al Cl 6e 4 2 7…”

mentioning

confidence: 99%

Unraveling the Anchoring Effect of MXene-Supported Single Atoms as Cathodes for Aluminum–Sulfur Batteries

Zheng

Chen

et al. 2022

ACS Materials Lett.

Self Cite

“…The reason why MXene is functionalized that bare Ti 2 C 3 will be terminated on the surface by S which means carrying out a reversible reaction impossibly. [75][76][77] Similarly, in Lv et al works, sulfate formed by the reaction of dissociated -OH with S is identified through a peak at 532.0 eV of SO 4 2À , which restrains the dissolution of Reproduced by permission. 74 Copyright 2019, American Chemical Society.…”

Section: Doping Mechanism Of Mxene/sulfur Compositementioning

confidence: 93%

“… 73 The DFT calculation proves that S/O better anchors the polysulfides and S. To analyze the effect of functional groups on the kinetics of nucleation and decomposition of Li‐S, diffusion barriers are sorted and it is found that the minimum Li + diffusion barriers on Ti 3 C 2 O 2 and Ti 3 C 2 S 2 are fairly low, while the boding between Li + and N greatly hindering the dynamics (Figure 3D). The reason why MXene is functionalized that bare Ti 2 C 3 will be terminated on the surface by S which means carrying out a reversible reaction impossibly 75‐77 . Similarly, in Lv et al works, sulfate formed by the reaction of dissociated ‐OH with S is identified through a peak at 532.0 eV of SO 4 2− , which restrains the dissolution of LiPSs 53 .…”

Section: Doping Mechanism Of Mxene/sulfur Compositementioning

confidence: 94%

Atomic surface modification strategy ofMXenematerials forhigh‐performancemetal sulfur batteries

Intl J of Energy Research

Zhang

et al. 2022

Improved MXenes based on heteroatom doping endow them with various new or optimized physicochemical, optical and structural properties. This greatly expands the library of MXenes materials and their potential for a range of applications. In this article, we comprehensively and critically discuss the synthesis and performance of the growing heteroatom doping and its family of composite MXenes materials in metal-sulfur batteries. We first summarize the heteroatom doping and its composite strategy of high-performance MXenes and analyze and summarize the mechanism of atomic element doping from three aspects: structure optimization, functional substitution and interface modification, aiming to provide clues for the development of new controllable synthetic routes. Emerging synthesis and optimization mechanisms related to metal-sulfur batteries are highlighted. Finally, we propose future opportunities and challenges for multifunctional high-performance MXenes research and metal-sulfur batteries. This work could open up new prospects for the development of high-performance MXenes in metal-sulfur batteries.

“…[8,[10][11][12] However, most reported Al-S batteries were driven by the reversible reduction of S, which only deliver low discharge voltages (≈0.4-1.0 V, theoretical voltage is 1.25 V vs Al 3+ /Al) with large voltage hysteresis at room temperature. [13][14][15][16][17][18][19][20][21][22][23] Therefore, it is of high merit to innovate the Al-S electrochemistry to significantly lift the discharge voltage for enhanced energy density. [12,19] The reversible electrochemical oxidation of S with high intrinsic electromotive force can provide such an opportunity.…”

mentioning

confidence: 99%

High‐Voltage Aluminium‐Sulfur Batteries with Functional Polymer Membrane

Zhang

Chu

et al. 2022

Adv Funct Materials

A high-voltage aluminium-sulfur (Al-S) battery is developed by employing the reversible electrochemical oxidation of S, favoring a high discharge voltage of around 1.8 V (vs Al 3+ /Al). The reversible multiple-electron transformation between positive-and negative-valence S compounds is further realized for activating a high-capacity Al-S battery. The formation of sulfur chlorides as charge products of S, including S 2 Cl 2 (l) as the dominant one, has been clearly identified. Benefiting from a functional polymer membrane infiltrated with AlCl 3 /acetamide electrolyte, which can suppress unwanted electrolyte reactions, restrict the shuttling of sulfur chlorides across the separator, and stabilize the Al anode against degradation, the Al-S battery can deliver largely enhanced performance, with a capacity of 861 mAh g −1 , capacity retentions of 92.1%/79.0% within 50/200 cycles, and durability of 490 cycles. The new electrochemistry scenarios shed light on the development of S-based secondary batteries with higher energy densities for future.