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A fundamental look at electrocatalytic sulfur reduction reaction

Journal Article · · Nature Catalysis
 [1];  [2];  [2];  [2];  [2];  [2];  [2];  [2];  [3];  [2];  [3];  [4];  [5];  [2];  [2];  [2];  [2];  [2]
  1. Univ. of California, Los Angeles, CA (United States); OSTI
  2. Univ. of California, Los Angeles, CA (United States)
  3. Univ. of Oxford (United Kingdom); Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.
  4. Univ. of California, Los Angeles, CA (United States); King Saud Univ., Riyadh (Saudi Arabia)
  5. King Saud Univ., Riyadh (Saudi Arabia)
+ Show Author Affiliations
The fundamental kinetics of the electrocatalytic sulfur reduction reaction (SRR), a complex 16-electron conversion process in lithium–sulfur batteries, is so far insufficiently explored. In this study, by directly profiling the activation energies in the multistep SRR, we reveal that the initial reduction of sulfur to the soluble polysulfides is relatively easy owing to the low activation energy, whereas the subsequent conversion of the polysulfides into the insoluble Li2S2/Li2S has a much higher activation energy, contributing to the accumulation of polysulfides and exacerbating the polysulfide shuttling effect. We use heteroatom-doped graphene as a model system to explore electrocatalytic SRR. We show that nitrogen and sulfur dual-doped graphene considerably reduces the activation energy to improve SRR kinetics. Density functional calculations confirm that the doping tunes the p-band centre of the active carbons for an optimal adsorption strength of intermediates and electroactivity. This study establishes electrocatalysis as a promising pathway to tackle the fundamental challenges facing lithium–sulfur batteries.
Research Organization:
Univ. of California, Los Angeles, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0019381
OSTI ID:
1803764
Journal Information:
Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 9 Vol. 3; ISSN 2520-1158
Publisher:
Springer NatureCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
batteries
chemistry
electrocatalysis