[en] 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 post-synthesis 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, by 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 as the key parameter since 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/de-insertion capacities, while oxidation in air adds carbonyl groups, increasing the Li+ ions storage capacity thanks to an improved accessibility to the carbon network, which is not caused by any textural change
Research Center/Unit :
Center for Education and Research on Macromolecules (CERM) CESAM - Complex and Entangled Systems from Atoms to Materials - ULiège Chemical engineering - Nanomaterials Catalysis Electrochemistry
Disciplines :
Chemistry Materials science & engineering
Author, co-author :
Piedboeuf, Marie-Laure ; University of Liège (ULiège), Department of Chemical Engineering – Nanomaterials, Catalysis, Electrochemistry
Job, Nathalie ; University of Liège (ULiège), Department of Chemical Engineering – Nanomaterials, Catalysis, Electrochemistry
Aqil, Abdelhafid ; University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit, Center for Education and Research on Macromolecules (CERM), Belgium
Busby, Yan; University of Namur, (UNamur) Institute of Structured Matter, Belgium > French-German Research Institute of Saint-Louis, Nanomatériaux pour les Systèmes Sous Sollicitations Extrêmes, France
Fierro, Vanessa; University of Lorraine, Institut Jean Lamour, France
Celzard, Alain; University of Lorraine, Institut Jean Lamour, France
Detrembleur, Christophe ; University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit, Center for Education and Research on Macromolecules (CERM), Belgium
Léonard, Alexandre ; University of Liège (ULiège), Department of Chemical Engineering – Nanomaterials, Catalysis, Electrochemistry
Language :
English
Title :
Understanding the influence of surface oxygen groups on the electrochemical behavior of porous carbons as anodes for lithium-ion batteries
Publication date :
21 July 2020
Journal title :
ACS Applied Materials and Interfaces
ISSN :
1944-8244
eISSN :
1944-8252
Publisher :
American Chemical Society (ACS), United States - District of Columbia
Volume :
12
Pages :
36054-36065
Peer reviewed :
Peer Reviewed verified by ORBi
Name of the research project :
BATWAL project; Programme des fonds Spéciaux pour la Recherche, Promotee
Funders :
F.R.S.-FNRS - Fonds de la Recherche Scientifique FRIA - Fonds pour la Formation à la Recherche dans l'Industrie et dans l'Agriculture Région wallonne RFCS - European Commission. Research Fund for Coal and Steel ULiège - Université de Liège
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