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Title: A Janus protein-based nanofabric for trapping polysulfides and stabilizing lithium metal in lithium–sulfur batteries
The shuttling of polysulfides and uncontrollable growth of lithium dendrites remain the most critical obstacles deteriorating the performance and safety of lithium–sulfur batteries. The separator plays a key role in molecule diffusion and ion transport kinetics; thus, endowing the separator with functions to address the two abovementioned issues is an urgent need. Herein, a protein-based, low-resistance Janus nanofabric is designed and fabricated for simultaneously trapping polysulfides and stabilizing lithium metal. The Janus nanofabric is achieved via combining two functional nanofabric layers, a gelatin-coated conductive nanofabric (G@CNF) as a polysulfide-blocking layer and a gelatin nanofabric (G-nanofabric) as an ion-regulating layer, into a heterostructure. The gelatin coating of G@CNF effectively enhances the polysulfide-trapping ability owing to strong gelatin–polysulfide interactions. The G-nanofabric with exceptional wettability, high ionic conductivity (4.9 × 10 −3 S cm −1 ) and a high lithium-ion transference number (0.73) helps stabilize ion deposition and thus suppresses the growth of lithium dendrites. As a result, a Li/Li symmetric cell with the G-nanofabric delivers ultra-long cycle life over 1000 h with very stable performance. Benefiting from the synergistic effect of the two functional layers of the Janus nanofabric, the resulting Li–S batteries demonstrate excellent capacity, rate performance and cycling stability ( more » e.g. initial discharge capacity of 890 mA h g −1 with a decay rate of 0.117% up to 300 cycles at 0.5 A g −1 ). « less
Authors:
; ; ;
Award ID(s):
1929236
Publication Date:
NSF-PAR ID:
10191474
Journal Name:
Journal of Materials Chemistry A
Volume:
8
Issue:
15
Page Range or eLocation-ID:
7377 to 7389
ISSN:
2050-7488
Sponsoring Org:
National Science Foundation
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Density functional theory calculation reveals the electronic state variance between the structures with and without defects, the structure with defects demonstrates the higher kinetic condition for sulfur conversion. To further identify the favorable reaction dynamic process, the in-situ XRD is used to characterize the transformation between soluble and insoluble polysulfides, which is the main barrier in the charge and discharge process of Li-S batteries. The results show the oCVD coated 3D printed sulfur cathode exhibits a much higher kinetic process for sulfur conversion, which benefits from the highly tailored hierarchal hollow structure and the defects engineering on the cathode. Further, the oCVD coated 3D printed sulfur cathode also demonstrates higher stability during long cycling enabled by the oCVD PEDOT protection layer, which is verified by an absorption energy calculation of polysulfides at PEDOT. Such modeling and analysis help to elucidate the fundamental mechanisms that govern cathode performance and degradation in Li-S batteries. The current study also provides design strategies for the sulfur cathode as well as selection approaches to novel battery systems. References: Bhargav, A., (2020). Lithium-Sulfur Batteries: Attaining the Critical Metrics. Joule 4 , 285-291. Chung, S.-H., (2018). Progress on the Critical Parameters for Lithium–Sulfur Batteries to be Practically Viable. Advanced Functional Materials 28 , 1801188. Peng, H.-J.,(2017). Review on High-Loading and High-Energy Lithium–Sulfur Batteries. Advanced Energy Materials 7 , 1700260. Chu, T., (2021). 3D printing‐enabled advanced electrode architecture design. Carbon Energy 3 , 424-439. Shi, Z., (2021). Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives. Advanced Energy Materials 11 . Figure 1« less
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