Understanding the Influence of Surface Oxygen Groups on the Electrochemical Behavior of Porous Carbons as Anodes for Lithium-Ion Batteries

The present study elucidates the role of surface oxygen functional groups on the electrochemical behavior of porous carbons when used as anodes for Li-ion batteries. To achieve this objective, a carbon xerogel (CX) obtained by pyrolysis of a resorcinol–formaldehyde gel, was modified by different pos...

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Bibliographic Details
Published in:	ACS applied materials & interfaces 2020-08, Vol.12 (32), p.36054-36065
Main Authors:	Piedboeuf, Marie-Laure C, Job, Nathalie, Aqil, Abdelhafid, Busby, Yan, Fierro, Vanessa, Celzard, Alain, Detrembleur, Christophe, Léonard, Alexandre F
Format:	Article
Language:	eng
Subjects:	Carbon Xerogel Chemical Sciences Chemistry Chimie Electrolyte accessibility Energy, Environmental, and Catalysis Applications Engineering, computing & technology Ingénierie, informatique & technologie Li-ion battery Material chemistry Materials science & engineering Physical, chemical, mathematical & earth Sciences Physique, chimie, mathématiques & sciences de la terre Polydopamine Science des matériaux & ingénierie Surface Oxygen Groups
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Summary:	The present study elucidates the role of surface oxygen functional groups on the electrochemical behavior of porous carbons when used as anodes for Li-ion batteries. To achieve this objective, a carbon xerogel (CX) obtained by pyrolysis of a resorcinol–formaldehyde gel, was modified by different postsynthesis treatments in order to modulate its surface chemistry while maintaining its external surface constant. Various surface modifications were obtained by oxidation in air, in situ polymerization of dopamine, and finally by grafting of a polyethylene oxide layer on the polydopamine coating. While oxidation in air did not affect the pore texture of the CX, modifications by coating techniques substantially decreased the micropore fraction. Detailed electrochemical characterizations of the materials processed as electrodes were performed by capacitance measurements and galvanostatic cycling. Surface chemistry results, from X-ray photoelectron spectroscopy, show that the accessibility and the capacity increase when carbonyl (R–CO) groups are formed on the CX, but not with oxides and hydroxyls. The amount of surface carbonyls, and in particular, aldehyde (OCH) groups, is found to be the key parameter because it is directly correlated with the modified CX electrochemical behavior. Overall, the explored surface coatings tend to reduce the micropore volume and add mainly hydroxyl functional groups but hardly change the Li+ insertion/deinsertion capacities, while oxidation in air adds carbonyl groups, increasing the Li+ ion storage capacity, thanks to an improved accessibility to the carbon network, which is not caused by any textural change.
ISSN:	1944-8244 1944-8252 1944-8252