Implanting Single Zn Atoms Coupled with Metallic Co Nanoparticles into Porous Carbon Nanosheets Grafted with Carbon Nanotubes for High‐Performance Lithium‐Sulfur Batteries

Abstract

The electrochemical performance of lithium‐sulfur (Li‐S) batteries is severely hindered by the sluggish sulfur redox kinetics and the shuttle effect of lithium polysulfides (LiPSs). Herein, an integrated composite catalyst consisting of Co nanoparticles and single‐atom (SA) Zn co‐implanted in nitrogen‐doped porous carbon nanosheets grafted with carbon nanotubes (Co/SA‐Zn@N‐C/CNTs) is rationally developed toward this challenge. Experimental and theoretical investigations indicate that the synergistically dual active sites of Co and atomic Zn‐N4 moieties with an optimal charge redistribution not only strongly confine the LiPSs but also effectively catalyze its conversion reactions by lowering the energy barrier from Li2S2 to Li2S while the N‐doped porous carbon‐grafted CNTs enables a large surface area for more active site exposure and provides a fast electron/ion pathway. Benefiting from synergies, Li‐S batteries equipped with the Co/SA‐Zn@N‐C/CNTs‐based sulfur cathode exhibit a high reversible capacity of 1302 mAh g−1 at 0.2 C and a low capacity fading rate of 0.033% per cycle over 800 cycles at 1 C. Moreover, a high areal capacity of 4.5 mAh cm−2 at 0.2 C with the sulfur loading of 5.1 mg cm−2 can be achieved. The present work may provide new insight into the design of high‐performance sulfur‐based cathodes for Li‐S batteries.

MXene supported transition metal nanoparticles accelerate sulfur reduction reaction kinetics

“…The obtained excellent performance of the CoNPs@MXene/S cathode is superior to most of the reported thick sulfur cathodes (>2 mg cm À2 ) with SRR catalysts (Table S1 †), further demonstrating its great promise in practical Li-S batteries. 26,[39][40][41][42][43][44][45][46][47][48][49][50][51][52] The electrochemical impedance spectra (EIS) plot of the cycled Li-S cells with the CoNPs@MXene/S cathode show the smallest charge transfer resistance among all cathodes (Fig. 5d).…”

“…According to the previous reports, the Co@N-C/CNT catalyst endows the Li-S cell with higher areal capacity and better cycling stability compared to the CNTs/Co catalyst. 39,40 The hetero-atom doping could increase the LiPS affinity of carbon materials, which further activates the SRR catalysts. It is consistent with our results above.…”

“…The obtained excellent performance of the CoNPs@MXene/S cathode is superior to most of the reported thick sulfur cathodes (>2 mg cm −2 ) with SRR catalysts (Table S1†), further demonstrating its great promise in practical Li–S batteries. 26,39–52…”

Advanced preparation and application of transition metal selenides in lithium–sulfur batteries: a review

“…(4) Sufficient electrochemical activity sites to achieve better effects. 35 It has been found that carbon materials (porous carbon, 36 graphene, 37 hollow carbon spheres, 38 carbon nanosheets, 39 etc.) as a scaffold for the sulfur cathode can accelerate the transport rate of particles due to high conductivity.…”

NiS1−xSex Nanoparticles Anchored on Nitrogen-Doped Reduced Graphene Oxide as Highly Stable Anode for Sodium-Ion Battery

“…Lithium-ion batteries (LIBs) have been extensively applied in all aspects of our lives, but the limited lithium resources cannot satisfy the ever-growing demand for future electrical storage system (EES) devices [1][2][3][4][5][6]. Sodium-ion batteries (SIBs) are deemed to be a highly promising alternative, due to the abundant resources, low-cost and, especially, similar working mechanism to LIBs [7][8][9].…”