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Single- or Poly-Crystalline Ni-Rich Layered Cathode, Sulfide or Halide Solid Electrolyte: Which Will be the Winners for All-Solid-State Batteries?

Single- or Poly-Crystalline Ni-Rich Layered Cathode, Sulfide or Halide Solid Electrolyte: Which Will be the Winners for All-Solid-State Batteries?
Han, YoonjaeJung, Sung HooKwak, HiramJun, SeunggooKwak, Hunho H.Lee, Jong HoonHong, Seung-TaeJung, Yoon Seok
DGIST Authors
Han, Yoonjae; Jung, Sung Hoo; Kwak, Hiram; Jun, Seunggoo; Kwak, Hunho H.; Lee, Jong Hoon; Hong, Seung-Tae; Jung, Yoon Seok
Issue Date
Advanced Energy Materials, 11(21), 2100126
Author Keywords
(electro)chemo-mechanical effectshalidesNi-rich layered oxide cathodessolid-state batteriessulfides
Aluminum compoundsBromine compoundsCathodesChlorine compoundsElectric dischargesElectrochemical oxidationLithium compoundsNanocrystalline materialsNickel oxideParticle size analysisScanning electron microscopySolid state devicesSolid-State BatteriesSulfur compoundsAll-solid state batteriesComplementary analysisCycling performanceDischarge capacitiesInitial Coulombic efficiencyLayered oxide cathodesMechanical degradationMicrostructural integritySolid electrolytes
Two newly emerging materials for application in all-solid-state batteries, namely, single-crystalline Ni-rich layered oxide cathode and halide solid electrolyte (SE), are of utmost interest because of their superior properties (good microstructural integrity and excellent electrochemical oxidation stability, respectively) to conventional polycrystalline layered oxides and sulfide SEs. In this work, four electrodes employing single- or polycrystalline LiNi0.88Co0.11Al0.01O2 (NCA) and Li3YCl6 or Li6PS5Cl0.5Br0.5 are rigorously characterized by complementary analyses. It is shown that the synergy of employing cracking-free single-crystalline NCA and oxidation-tolerable Li3YCl6 can be achieved by considering intercoupled engineering factors that are prone to overlook, such as size, lightness, and mixing of particles. Accordingly, the highest level of performances in terms of discharge capacity (199 mA h g−1 at 0.1C), initial Coulombic efficiency (89.6%), cycling performance (96.8% of capacity retention at the 200th cycle), and rate capability (130 mA h g−1 at 4C) are demonstrated at 30 °C. Severe side reactions occurring at the Li6PS5Cl0.5Br0.5/NCA interfaces are also quantified and probed. Importantly, an overlooked but significant contribution of the side reaction of Li6PS5Cl0.5Br0.5 to the detrimental electrochemo-mechanical degradation of polycrystalline NCA is revealed for the first time by postmortem scanning electron microscopy and operando electrochemical pressiometry measurements. © 2021 Wiley-VCH GmbH
John Wiley and Sons Inc
Related Researcher
  • Author Hong, Seung-Tae Battery Materials Discovery Laboratory
  • Research Interests Magnesium, calcium, and zinc ion batteries; lithium all-solid-state batteries; Inorganic materials discovery; Solid state chemistry; Crystallography; Mg, Ca, Zn 이온 이차전지; 리튬 전고체전지; 신 무기재료 합성; 고체화학; 결정화학
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Department of Energy Science and EngineeringBattery Materials Discovery Laboratory1. Journal Articles

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