Building Up an “Elemental Property—Adsorption Energy Descriptor—Decomposition Barrier” Three‐Tier Model for Screening Biatom Catalysts in Sodium–Sulfur Batteries

Abstract

Developing highly efficient catalysts for the Na 2 S redox process and sodium polysulfide anchoring is becoming increasingly important for high-performance sodium-sulfur (Na-S) batteries. The recently emerged graphene-supported biatom catalysts (G-BACs) exhibit great potential for providing high activity in both discharging and charging processes. However, the fast screening of promising G-BACs for Na-S batteries is hindered by the formidable computational cost for calculating Na 2 S decomposition barriers (E b ). Herein, this work develops an "elemental property-adsorption energy descriptor-decomposition barrier" three-tier model to accelerate this process and elucidates the origin of catalytic activity. It is found that E b during the charging process is linearly correlated with the adsorption energy difference between the initial and final states of Na 2 S decomposition (E diff ) for both homonuclear and heteronuclear transition metal G-BACs. This work further correlates E diff with intrinsic properties of metal elements by machine learning approaches and unravels the most significant elemental feature to be the outer electron number. This work not only accelerates the design of highly efficient G-BACs in Na-S batteries based on the structure-activity relationship, but also provides a feasible strategy for the fast screening of catalysts for other electrochemical reactions for potential experimental design.

Ultrafast Strategy to Fabricate Sulfur Cathodes for High-Performance Lithium–Sulfur Batteries

“…Especially, the obvious lower Gibbs free energies of the critical steps from liquid Li 2 S 4 to solid Li 2 S 2 /Li 2 S on NiS 2 indicate that NiS 2 dispersed in bitumen carbonized effectively boosts the LiS 2 precipitation process. 34 During charging, solid Li 2 S first decomposes into liquid lithium polysulfide. Herein, to further reveal the nature of this process, the decomposition energy barrier of Li 2 S was calculated to evaluate the reaction kinetics on the substrates of bitumen carbonized and NiS 2 .…”

High-Throughput Screening of Sulfur Reduction Reaction Catalysts Utilizing Electronic Fingerprint Similarity

“…The range from −7 to 7 eV already encompasses most features of the 1D-DOS spectrum, adequately characterizing different forms of interactions during the reaction process. Moreover, the center of the 0D d-band and p-band also lies within this range. − Because of the strong interaction between the adsorbed species and the sp-band DOS of MXene, both the d-band and sp-band must be considered . Therefore, TDOS is used to calculate the 1D-DOS fingerprint similarity.…”

“…By considering the p-band center of MXene surface functional groups and the electronegativity of the subsurface metal, a scaling relationship between Δ G min and the descriptor was revealed . Huang et al used machine learning to reveal a strong correlation between the decomposition barrier of Na 2 S and the number of outermost electrons of the metal element . Based on the valence electrons and electronegativity of MXene surface and subsurface atoms, several potential MXene catalysts with good C–N coupling performance were discovered …”

“…7 Huang et al used machine learning to reveal a strong correlation between the decomposition barrier of Na 2 S and the number of outermost electrons of the metal element. 8 Based on the valence electrons and electronegativity of MXene surface and subsurface atoms, several potential MXene catalysts with good C−N coupling performance were discovered. 9 All the above-mentioned studies highlight the pivotal role of electronic structure in catalytic reactions, 10 indicating the fingerprint effect of electronic structure.…”

Ferroelectric Materials for High Energy Density Batteries: Progress and Outlook

“…Thus, immobilizing soluble polysulfides and strengthening polysulfide conversion kinetics to simultaneously suppress the shuttling effect are crucial. − …”