TY - JOUR
T1 - Fe-single-atom catalyst nanocages linked by bacterial cellulose-derived carbon nanofiber aerogel for Li-S batteries
AU - Lin, Xueyan
AU - Li, Wenyue
AU - Nguyen, Vy
AU - Wang, Shu
AU - Yang, Shize
AU - Ma, Lu
AU - Du, Yonghua
AU - Wang, Bin
AU - Fan, Zhaoyang
N1 - Publisher Copyright:
© 2023
PY - 2023/12/1
Y1 - 2023/12/1
N2 - Li-S battery (LSB) is promising for achieving high capacity. Still, its development is hindered by the complex redox process with sluggish kinetics and particularly the resulting lithium polysulfides (LiPS) shuttle effects. Single-atom catalysts (SACs), with their maximized atom utilization, could effectively chemisorb soluble LiPSs and expedite the sulfide conversion reaction kinetics. Here we report incorporating Fe single metal atom catalyst (Fe-SAC) in the sulfur cathode design and its electrocatalytic effects. Fe-doped ZIF-8 nanocages were introduced into a cheap biomass bacteria cellulose. A pyrolysis process converted them into an aerogel structure with Fe-SAC-functionalized N-doped carbon nanocages linked by a carbon nanofiber network (FeSA-NC@CBC), which was applied as a scaffold to fabricate freestanding and binder-free sulfur cathodes. We conducted electrochemical measurements to reveal Fe-SAC functions including lowering energy barriers for S8 reduction to liquid-phase LiPSs and further to solid-phase Li2S2/Li2S and accelerating Li2S2/Li2S nucleation and deposition, as corroborated by our theoretical calculation results. Benefiting from the synergistic effects of highly active Fe-SAC and three-dimensional conductive network, the sulfide reaction kinetics is improved, which can diminish LiPS shuttle effects and therefore improve LBS rate performance and cycling stability. Accordingly, the fabricated FeSA-NC@CBC composite cathode delivers an excellent rate capability at 2C with a reversible capacity of 840 mAh/g and a long-term cyclic stability of 800 mAh/g at 1C after 500 cycles.
AB - Li-S battery (LSB) is promising for achieving high capacity. Still, its development is hindered by the complex redox process with sluggish kinetics and particularly the resulting lithium polysulfides (LiPS) shuttle effects. Single-atom catalysts (SACs), with their maximized atom utilization, could effectively chemisorb soluble LiPSs and expedite the sulfide conversion reaction kinetics. Here we report incorporating Fe single metal atom catalyst (Fe-SAC) in the sulfur cathode design and its electrocatalytic effects. Fe-doped ZIF-8 nanocages were introduced into a cheap biomass bacteria cellulose. A pyrolysis process converted them into an aerogel structure with Fe-SAC-functionalized N-doped carbon nanocages linked by a carbon nanofiber network (FeSA-NC@CBC), which was applied as a scaffold to fabricate freestanding and binder-free sulfur cathodes. We conducted electrochemical measurements to reveal Fe-SAC functions including lowering energy barriers for S8 reduction to liquid-phase LiPSs and further to solid-phase Li2S2/Li2S and accelerating Li2S2/Li2S nucleation and deposition, as corroborated by our theoretical calculation results. Benefiting from the synergistic effects of highly active Fe-SAC and three-dimensional conductive network, the sulfide reaction kinetics is improved, which can diminish LiPS shuttle effects and therefore improve LBS rate performance and cycling stability. Accordingly, the fabricated FeSA-NC@CBC composite cathode delivers an excellent rate capability at 2C with a reversible capacity of 840 mAh/g and a long-term cyclic stability of 800 mAh/g at 1C after 500 cycles.
KW - Bacterial cellulose
KW - Li-S battery
KW - Metal organic framework (MOF)
KW - Single atom catalyst
KW - Sulfide reaction kinetics
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U2 - 10.1016/j.cej.2023.146977
DO - 10.1016/j.cej.2023.146977
M3 - Article
AN - SCOPUS:85175475783
SN - 1385-8947
VL - 477
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 146977
ER -