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Phenyl Disulfide Additive for Solution‐Mediated Carbon Dioxide Utilization in Li–CO 2 Batteries
Author(s) -
Pipes Robert,
Bhargav Amruth,
Manthiram Arumugam
Publication year - 2019
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201900453
Subject(s) - materials science , carbon dioxide , fourier transform infrared spectroscopy , electrochemistry , lithium (medication) , decomposition , electrolyte , carbon fibers , electrochemical reduction of carbon dioxide , carbon disulfide , chemical engineering , inorganic chemistry , chemistry , organic chemistry , catalysis , electrode , carbon monoxide , medicine , composite number , engineering , composite material , endocrinology
Phenyl disulfide (PDS) is employed as an electrolyte additive in lithium–carbon dioxide (Li–CO 2 ) batteries to allow for a solution‐mediated carbon dioxide reduction pathway. Thiophenolate anions, generated via electrochemical reduction of PDS, act as CO 2 capture agents by forming the adduct S ‐phenyl carbonothioate (SPC − ) in solution. A mechanism of SPC − ‐mediated CO 2 capture and utilization is proposed and supported via carbon‐13 nuclear magnetic resonance spectroscopy and Fourier‐transform infrared spectroscopy. Reversible formation and decomposition of lithium carbonate and amorphous carbon during cycling, facilitated by the solution‐mediated pathway, are demonstrated with an array of characterization techniques. Li–CO 2 batteries employing the PDS additive show vastly improved capacity, energy efficiency, and cycle life. The enhanced Li–CO 2 battery performance offered by the proposed solution‐mediated reaction pathway offers a compelling step forward in the pursuit of reversible CO 2 utilization.

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