Nonmetallic‐Bonding Fe–Mn Diatomic Pairs Anchored on Hollow Carbonaceous Nanodisks for High‐Performance Li–S Battery

Abstract

The issues of polysulfide shuttling and lethargic sulfur redox reaction (SROR) kinetics are the toughest obstacles of lithium–sulfur (Li–S) battery. Herein, integrating the merits of increased density of metal sites and synergistic catalytic effect, a unique single‐atom catalyst (SAC) with nonmetallic‐bonding Fe–Mn diatomic pairs anchored on hollow nitrogen‐doped carbonaceous nanodisk (denoted as FeMnDA@NC) is successfully constructed and well characterized by aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy, X‐ray absorption spectroscopy, etc. Density functional theory calculation indicates that the Fe–Mn diatomic pairs can effectively inhibit the shuttle effect by enhancing the adsorption ability retarding the polysulfide migration and accelerate the SROR kinetics. As a result, the Li–S battery assembled with FeMnDA@NC modified separator possesses an excellent electrochemical performance with ultrahigh specific capacities of 1419 mAh g−1 at 0.1 C and 885 mAh g−1 at 3.0 C, respectively. An outstanding specific capacity of 1165 mAh g−1 is achieved at 1.0 C and maintains at 731 mAh g−1 after 700 cycles. Notably, the assembled Li–S battery with a high sulfur loading of 5.35 mg cm−2 harvests a practical areal capacity of 5.70 mAh cm−2 at 0.2 C. A new perspective is offered here to construct advanced SACs suitable for the Li–S battery.

High-Entropy Metal Oxide-Coated Carbon Cloth as Catalysts for Long-Life Li–S Batteries

“…Electrochemical impedance spectroscopy (EIS) testing for the cell with CC and CC/HEO is tested at 100 to 0.1 kHz, shown in Figure c. The Nyquist plots for the cells can be divided into three parts: in the high-frequency area, the X -axis intercept represents the ohmic resistance, while in the middle- and low-frequency areas, it means the charge transfer resistance ( R ct ). − It is clear that the cell with CC/HEO shows smaller R ct (9.2 Ω) compared to the cell with CC (15.4 Ω).…”

Rational Design of Janus Metal Atomic‐Site Catalysts for Efficient Polysulfide Conversion and Alkali Metal Deposition: Advances and Prospects

“…In addition, the impregnation method is also a common wet‐chemistry strategy for preparing SACs. [ 62–64 ] For example, a homogeneous mixture composed of ZIF‐8 dodecahedral nanocrystals, polyacrylonitrile, and Co(NO 3 ) 2 ⋅6H 2 O was electrostatically spun into nanofibers. Thereafter, the internal components of ZIF‐8 were dissociated and dispersed into the polyacrylonitrile fibers and then carbonized during the high‐temperature thermal process, generating nanovesicles in their initial positions.…”

“…[ 90,191–193 ] To date, the research of dual‐atom catalysts remains in its infancy, the reported literatures so far mainly focused on heterogeneous diatomic catalysts and heteronuclear diatomic catalysts for M–S batteries. [ 88,194,195 ]…”

Promoting overall sulfur redox kinetics for Li–S batteries via interfacial synergy in a NiS–NiTe2 heterostructure-modified separator

“…Although the separator is not an active component within the battery, its role in inuencing crucial aspects such as cost, cycle life, and safety cannot be overstated. [18][19][20][21] The pores in the separator allow lithium ions to conduct between the anode and the cathode during the charge and discharge cycles, facilitating stable electrochemical reactions. Moreover, the separator serves a dual purpose by providing a physical barrier, preventing internal short circuits.…”