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Jung, Sung Hoo,Oh, Kyungbae,Nam, Young Jin,Oh, Dae Yang,Brü,ner, Philipp,Kang, Kisuk,Jung, Yoon Seok American Chemical Society 2018 Chemistry of materials Vol.30 No.22
<P>Most inorganic solid electrolytes (SEs) suffer from narrow intrinsic electrochemical windows and incompatibility with electrode materials, which results in the below par electrochemical performances of all-solid-state Li-ion or Li batteries (ASLBs). Unfortunately, in-depth understanding on the interfacial evolution and interfacial engineering via scalable protocols for ASLBs to mitigate these issues are at an infancy stage. Herein, we report on rationally designed Li<SUB>3</SUB>BO<SUB>3</SUB>-Li<SUB>2</SUB>CO<SUB>3</SUB> (LBO-LCO or Li<SUB>3-<I>x</I></SUB>B<SUB>1-<I>x</I></SUB>C<SUB><I>x</I></SUB>O<SUB>3</SUB> (LBCO)) coatings for LiCoO<SUB>2</SUB> in ASLBs employing sulfide SE of Li<SUB>6</SUB>PS<SUB>5</SUB>Cl. The new aqueous-solution-based LBO-coating protocol allows us to convert the surface impurity on LiCoO<SUB>2</SUB> and Li<SUB>2</SUB>CO<SUB>3</SUB>, into highly Li<SUP>+</SUP>-conductive LBCO layers (6.0 × 10<SUP>-7</SUP> S cm<SUP>-1</SUP> at 30 °C for LBCO vs 1.4 × 10<SUP>-9</SUP> S cm<SUP>-1</SUP> at 100 °C for Li<SUB>2</SUB>CO<SUB>3</SUB> or 1.4 × 10<SUP>-9</SUP> S cm<SUP>-1</SUP> at 30 °C for LBO), which also offer interfacial stability with sulfide SE. By applying these high-surface-coverage LBCO coatings, significantly enhanced electrochemical performances are obtained in terms of capacity, rate capability, and durability. It is elucidated that the LBCO coatings suppress the evolution of detrimental mixed conducting interphases containing Co<SUB>3</SUB>S<SUB>4</SUB> and effectively passivate the interfaces by the formation of alternative interface phases.</P> [FIG OMISSION]</BR>
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Belsey, Natalie A.,Cant, David J. H.,Minelli, Caterina,Araujo, Joyce R.,Bock, Bernd,Brü,ner, Philipp,Castner, David G.,Ceccone, Giacomo,Counsell, Jonathan D. P.,Dietrich, Paul M.,Engelhard, Mark American Chemical Society 2016 The Journal of Physical Chemistry Part C Vol.120 No.42
<P>We report the results of a Versailles Project on Advanced Materials and Standards (VAMAS) interlaboratory study on the measurement of the shell thickness and chemistry of nanoparticle coatings. Peptide-coated gold particles were supplied to laboratories in two forms: a colloidal suspension in pure water and particles dried onto a silicon wafer. Participants prepared and analyzed these samples using either X-ray photoelectron spectroscopy (XPS) or low energy ion scattering (LEIS). Careful data analysis revealed some significant sources of discrepancy, particularly for XPS. Degradation during transportation, storage, or sample preparation resulted in a variability in thickness of 53%. The calculation method chosen by XPS participants contributed a variability of 67%. However, variability of 12% was achieved for the samples deposited using a single method and by choosing photoelectron peaks that were not adversely affected by instrumental transmission effects. The study identified a need for more consistency in instrumental transmission functions and relative sensitivity factors since this contributed a variability of 33%. The results from the LEIS participants were more consistent, with variability of less than 10% in thickness, and this is mostly due to a common method of data analysis. The calculation was performed using a model developed for uniform, flat films, and some participants employed a correction factor to account for the sample geometry, which appears warranted based upon a simulation of LEIS data from one of the participants and comparison to the XPS results.</P>
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