TY - JOUR
T1 - Physicochemical Heterogeneity in Silicon Anodes from Cycled Lithium-Ion Cells
AU - Pidaparthy, Saran
AU - Luo, Mei
AU - Rodrigues, Marco Tulio F.
AU - Zuo, Jian Min
AU - Abraham, Daniel P.
N1 - S.P. acknowledges support from the U.S. Department of Energy (DOE) Graduate Student Research (SCGSR) program. The SCGSR program is administered by the Oak Ridge Institute for Science and Education for DOE under contract number DE-SC0014664. M.L. acknowledges support from the National Science Foundation INTERNship program. D.A. and M.T.F.R. are grateful for support from DOE’s Vehicle Technologies Office (VTO). This work was carried out in part at the Materials Research Laboratory Central Research Facilities, University of Illinois. Use of the Advanced Photon Source (APS) at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. We are grateful to Saul Lapidus at the APS for help with the high-resolution X-ray powder diffraction experiments. Work performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. We are grateful to David Gosztola at the CNM for instrument training and helping with the Raman spectroscopy measurements. The electrodes used in this article are from Argonne’s Cell Analysis, Modeling and Prototyping (CAMP) Facility, which is fully supported by the VTO. We are grateful to our many colleagues at CAMP, especially Stephen Trask and Andrew Jansen. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government.
S.P. acknowledges support from the U.S. Department of Energy (DOE) Graduate Student Research (SCGSR) program. The SCGSR program is administered by the Oak Ridge Institute for Science and Education for DOE under contract number DE-SC0014664. M.L. acknowledges support from the National Science Foundation INTERNship program. D.A. and M.T.F.R. are grateful for support from DOE’s Vehicle Technologies Office (VTO). This work was carried out in part at the Materials Research Laboratory Central Research Facilities, University of Illinois. Use of the Advanced Photon Source (APS) at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. We are grateful to Saul Lapidus at the APS for help with the high-resolution X-ray powder diffraction experiments. Work performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. We are grateful to David Gosztola at the CNM for instrument training and helping with the Raman spectroscopy measurements. The electrodes used in this article are from Argonne’s Cell Analysis, Modeling and Prototyping (CAMP) Facility, which is fully supported by the VTO. We are grateful to our many colleagues at CAMP, especially Stephen Trask and Andrew Jansen. The submitted manuscript has been created by UChicago Argonne LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government.
PY - 2022/8/31
Y1 - 2022/8/31
N2 - The severe capacity fade of lithium-ion cells with silicon-dominant anodes has hindered their widescale commercialization. In this work, we link cell capacity fade to the heterogeneous physicochemical evolution of silicon anodes during battery cycling. Through a multilength scale characterization approach, we demonstrate that silicon particles near the anode surface react differently from those near the copper current collector. In particular, near the anode surface we find an amorphized wispy silicon encased in a highly fluorinated matrix of electrolyte-reduction products. In contrast, closer to the current collector, the silicon retains more of its initial morphology and structure, suggesting the presence of isolated particles. The results show that the accessibility of active silicon to lithium ions varies across the anode matrix. Material and cell designs, which minimize electrode expansion resulting from the in-filling of pores with the solid electrolyte interphase (SEI), are needed to enhance anode homogeneity during the electrochemical cycling.
AB - The severe capacity fade of lithium-ion cells with silicon-dominant anodes has hindered their widescale commercialization. In this work, we link cell capacity fade to the heterogeneous physicochemical evolution of silicon anodes during battery cycling. Through a multilength scale characterization approach, we demonstrate that silicon particles near the anode surface react differently from those near the copper current collector. In particular, near the anode surface we find an amorphized wispy silicon encased in a highly fluorinated matrix of electrolyte-reduction products. In contrast, closer to the current collector, the silicon retains more of its initial morphology and structure, suggesting the presence of isolated particles. The results show that the accessibility of active silicon to lithium ions varies across the anode matrix. Material and cell designs, which minimize electrode expansion resulting from the in-filling of pores with the solid electrolyte interphase (SEI), are needed to enhance anode homogeneity during the electrochemical cycling.
KW - Raman spectroscopy
KW - X-ray diffraction (XRD)
KW - energy-dispersive X-ray spectroscopy (EDS)
KW - lithium-ion batteries (LIBs)
KW - reference electrode
KW - scanning electron nanodiffraction (SEND)
KW - transmission electron microscopy (TEM)
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U2 - 10.1021/acsami.2c06991
DO - 10.1021/acsami.2c06991
M3 - Article
C2 - 35973075
AN - SCOPUS:85136735580
SN - 1944-8244
VL - 14
SP - 38660
EP - 38668
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 34
ER -