PMID- 34693714
OWN - NLM
STAT- PubMed-not-MEDLINE
LR  - 20211104
IS  - 1944-8252 (Electronic)
IS  - 1944-8244 (Linking)
VI  - 13
IP  - 43
DP  - 2021 Nov 3
TI  - Unraveling the Role of Neutral Units for Single-Ion Conducting Polymer 
      Electrolytes.
PG  - 51525-51534
LID - 10.1021/acsami.1c15641 [doi]
AB  - With the cationic transference number close to unity, single-ion conducting 
      polymer electrolytes (SICPEs) are recognized as an advanced electrolyte system 
      with improved energy efficiency for battery application. The relatively low ionic 
      conductivity for most of the SICPEs in comparison with liquid electrolytes 
      remains the major "bottleneck" for their practical applications. Polyethylene 
      oxide (PEO) has been recognized as a benchmark for solid polymer electrolytes due 
      to its high salt solubility and reasonable ionic conductivity. PEO has two 
      advantages: (i) the polar ether groups coordinate well with lithium ions (Li(+)) 
      providing good dissociation from anions, and (ii) the low T(g) provides fast 
      segmental dynamics at ambient temperature and assists rapid charge transport. 
      These properties lead to active use of PEO as neutral plasticizing units in 
      SICPEs. Herein, we present a detailed comparison of new SICPEs copolymerized with 
      PEO units vs SICPEs copolymerized with other types of neutral units possessing 
      either flexible or polar structures. The presented analysis revealed that the 
      polarity of side chains has a limited influence on ion dissociation for 
      copolymer-type SICPEs. The Li(+)-ion dissociation seems to be controlled by the 
      charge delocalization on the polymerized anion. With good miscibility between 
      plasticizing neutral units and ionic conductive units, the ambient ionic 
      conductivity of synthesized SICPEs is still mainly controlled by the T(g) of the 
      copolymer. This work sheds light on the dominating role of PEO in SICPE systems 
      and provides helpful guidance for designing polymer electrolytes with new 
      functionalities and structures. Furthermore, based on the presented results, we 
      propose that designing polyanions with a highly delocalized charge may be another 
      promising route for achieving sufficient lithium ionic conductivity in 
      solvent-free SICPEs.
FAU - Zhao, Sheng
AU  - Zhao S
AD  - Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, 
      United States.
FAU - Song, Shenghan
AU  - Song S
AD  - Department of Chemistry & Chemical Biology, The University of New Mexico, 
      Albuquerque, New Mexico 87131, United States.
FAU - Wang, Yingqi
AU  - Wang Y
AD  - Department of Chemistry & Chemical Biology, The University of New Mexico, 
      Albuquerque, New Mexico 87131, United States.
FAU - Keum, Jong
AU  - Keum J
AD  - Center for Nanophase Materials Science and Neutron Scattering Division, Oak Ridge 
      National Laboratory, Oak Ridge, Tennessee 37830, United States.
FAU - Zhu, Jiadeng
AU  - Zhu J
AUID- ORCID: 0000-0003-4709-4115
AD  - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 
      37830, United States.
FAU - He, Yi
AU  - He Y
AUID- ORCID: 0000-0002-6884-5312
AD  - Department of Chemistry & Chemical Biology, The University of New Mexico, 
      Albuquerque, New Mexico 87131, United States.
FAU - Sokolov, Alexei P
AU  - Sokolov AP
AUID- ORCID: 0000-0002-8187-9445
AD  - Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, 
      United States.
AD  - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 
      37830, United States.
FAU - Cao, Peng-Fei
AU  - Cao PF
AUID- ORCID: 0000-0003-2391-1838
AD  - Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 
      37830, United States.
LA  - eng
PT  - Journal Article
DEP - 20211025
PL  - United States
TA  - ACS Appl Mater Interfaces
JT  - ACS applied materials & interfaces
JID - 101504991
SB  - IM
OTO - NOTNLM
OT  - Coulombic interaction
OT  - activation energy
OT  - polyethylene oxide (PEO)
OT  - polymer electrolyte
OT  - single-ion conducting
EDAT- 2021/10/26 06:00
MHDA- 2021/10/26 06:01
CRDT- 2021/10/25 08:39
PHST- 2021/10/26 06:00 [pubmed]
PHST- 2021/10/26 06:01 [medline]
PHST- 2021/10/25 08:39 [entrez]
AID - 10.1021/acsami.1c15641 [doi]
PST - ppublish
SO  - ACS Appl Mater Interfaces. 2021 Nov 3;13(43):51525-51534. doi: 
      10.1021/acsami.1c15641. Epub 2021 Oct 25.