Abstract
This work probes the slurry architecture of a high silicon content electrode slurry with and without low molecular weight polymeric dispersants as a function of shear rate to mimic electrode casting conditions for poly(acrylic acid) (PAA) and lithium neutralized poly(acrylic acid) (LiPAA) based electrodes. Rheology coupled ultra-small angle neutron scattering (rheo-USANS) was used to examine the aggregation and agglomeration behavior of each slurry as well as the overall shape of the aggregates. The addition of dispersant has opposing effects on slurries made with PAA or LiPAA binder. With a dispersant, there are fewer aggregates and agglomerates in the PAA based silicon slurries, while LiPAA based silicon slurries become orders of magnitude more aggregated and agglomerated at all shear rates. The reorganization of the PAA and LiPAA binder in the presence of dispersant leads to a more homogeneous slurry and a more heterogeneous slurry, respectively. This reorganization ripples through to the cast electrode architecture and is reflected in the electrochemical cycling of these electrodes.
| Original language | English |
|---|---|
| Pages (from-to) | 1049-1058 |
| Number of pages | 10 |
| Journal | ChemPhysChem |
| Volume | 22 |
| Issue number | 11 |
| DOIs | |
| State | Published - Jun 4 2021 |
Funding
This research (MKBT, BLA, STE, AMR, GMV) was supported by the U.S. Department of Energy's Vehicle Technologies Office under the Silicon Consortium Project, directed by Brian Cunningham, and managed by Anthony Burrell. The authors thank Paul D. Butler and Markus Bleuel for facilitating the measurements at NIST and for their helpful discussions. The authors would also like to acknowledge Ryan Armstrong for his inciteful observations that sent us down this research path. Access to the NG7-SANS and BT-5 USANS instruments was provided by the Center for High Resolution Neutron Scattering, a partnership between the National Institute of Standards and Technology and the National Science Foundation under Agreement No. DMR-1508249. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory (MD and LH). This work benefited from the use of the SasView application, originally developed under NSF award DMR-0520547. SasView contains code developed with funding from the European Union's Horizon 2020 research and innovation program under the SINE2020 project, grant agreement no. 654000. This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow other to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). Commercial equipment and materials identified in this work do not imply recommendation nor endorsement by the National Institute of Standards and Technology. This research (MKBT, BLA, STE, AMR, GMV) was supported by the U.S. Department of Energy's Vehicle Technologies Office under the Silicon Consortium Project, directed by Brian Cunningham, and managed by Anthony Burrell. The authors thank Paul D. Butler and Markus Bleuel for facilitating the measurements at NIST and for their helpful discussions. The authors would also like to acknowledge Ryan Armstrong for his inciteful observations that sent us down this research path. Access to the NG7‐SANS and BT‐5 USANS instruments was provided by the Center for High Resolution Neutron Scattering, a partnership between the National Institute of Standards and Technology and the National Science Foundation under Agreement No. DMR‐1508249. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory (MD and LH). This work benefited from the use of the SasView application, originally developed under NSF award DMR‐0520547. SasView contains code developed with funding from the European Union's Horizon 2020 research and innovation program under the SINE2020 project, grant agreement no. 654000. This manuscript has been authored by UT‐Battelle, LLC, under Contract DE‐AC05‐00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid‐up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow other to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe‐public‐access‐plan). Commercial equipment and materials identified in this work do not imply recommendation nor endorsement by the National Institute of Standards and Technology.
| Funders | Funder number |
|---|---|
| DOE Public Access Plan | |
| United States Government | |
| National Science Foundation | DMR‐1508249, DMR‐0520547 |
| U.S. Department of Energy | |
| National Institute of Standards and Technology | NG7-SANS |
| Office of Science | |
| Oak Ridge National Laboratory | |
| Horizon 2020 | 654000, DE‐AC05‐00OR22725 |
Keywords
- aggregation
- electrode architecture
- rheology
- silicon
- slurry dynamics
- ultra-small angle neutron scattering