Showing papers by "Miaofang Chi published in 2019"
TL;DR: Li et al. as mentioned in this paper studied three representative solid electrolytes with neutron depth profiling and identified high electronic conductivity as the root cause for the dendrite issue, which is the most common cause of lithium dendrites.
Abstract: Solid electrolytes (SEs) are widely considered as an ‘enabler’ of lithium anodes for high-energy batteries. However, recent reports demonstrate that the Li dendrite formation in Li7La3Zr2O12 (LLZO) and Li2S–P2S5 is actually much easier than that in liquid electrolytes of lithium batteries, by mechanisms that remain elusive. Here we illustrate the origin of the dendrite formation by monitoring the dynamic evolution of Li concentration profiles in three popular but representative SEs (LiPON, LLZO and amorphous Li3PS4) during lithium plating using time-resolved operando neutron depth profiling. Although no apparent changes in the lithium concentration in LiPON can be observed, we visualize the direct deposition of Li inside the bulk LLZO and Li3PS4. Our findings suggest the high electronic conductivity of LLZO and Li3PS4 is mostly responsible for dendrite formation in these SEs. Lowering the electronic conductivity, rather than further increasing the ionic conductivity of SEs, is therefore critical for the success of all-solid-state Li batteries. Despite its importance in lithium batteries, the mechanism of Li dendrite growth is not well understood. Here the authors study three representative solid electrolytes with neutron depth profiling and identify high electronic conductivity as the root cause for the dendrite issue.
901 citations
TL;DR: In this article, a hard-magnet core/shell L10-CoPt/Pt nanoparticles with 2-3 atomic layers of strained Pt shell was synthesized for ORR.
273 citations
TL;DR: Recent progress in scientific understanding of the physical origins of the non-idealities of memristive devices are summarized and a synergistic approach based on in situ characterization and device modeling to investigate switching mechanism is proposed.
Abstract: Owing to their attractive application potentials in both non-volatile memory and unconventional computing, memristive devices have drawn substantial research attention in the last decade. However, major roadblocks still remain in device performance, especially concerning relatively large parameter variability and limited cycling endurance. The response of the active region in the device within and between switching cycles plays the dominating role, yet the microscopic details remain elusive. This Review summarizes recent progress in scientific understanding of the physical origins of the non-idealities and propose a synergistic approach based on in situ characterization and device modeling to investigate switching mechanism. At last, the Review offers an outlook for commercialization viability of memristive technology. Memristor as the fourth basic element of electric circuits has drawn substantial attention for developing future computing technologies. Sun et al. report the progress and the challenges facing researchers on understanding memristive switching, and advocate continuous studies using a synergistic approach.
240 citations
TL;DR: In this paper, the reaction of lithium with LAGP electrolyte caused amorphization and volume expansion, which induced mechanical stress and fracture of the SSE along with a massive increase in impedance.
Abstract: The interfaces between many solid-state electrolytes (SSEs) and lithium metal are (electro)chemically unstable, and improved understanding of how interfacial transformations influence electrochemical degradation is necessary to stabilize these interfaces and therefore enable a wider range of viable SSEs for batteries. Here, the (electro)chemical reaction processes that occur at the interface between Li1.4Al0.4Ge1.6(PO4)3 (LAGP) electrolyte and lithium are studied using in situ transmission electron microscopy and ex situ techniques. The reaction of lithium with LAGP causes amorphization and volume expansion, which induce mechanical stress and fracture of the SSE along with a massive increase in impedance. The evolved interphase has a nonuniform morphology at high currents, which causes accelerated chemo-mechanical failure. This work demonstrates that the current-dependent nature of the reaction at the SSE/Li interface plays a crucial role in determining chemo-mechanical degradation mechanisms, with implic...
137 citations
TL;DR: The concept of asymmetric active sites is used to develop a class of doped Cu catalysts for C-C coupling, delivering record selectivity to n-propanol.
Abstract: The electroreduction of C1 feedgas to high-energy-density fuels provides an attractive avenue to the storage of renewable electricity. Much progress has been made to improve selectivity to C1 and C2 products, however, the selectivity to desirable high-energy-density C3 products remains relatively low. We reason that C3 electrosynthesis relies on a higher-order reaction pathway that requires the formation of multiple carbon-carbon (C-C) bonds, and thus pursue a strategy explicitly designed to couple C2 with C1 intermediates. We develop an approach wherein neighboring copper atoms having distinct electronic structures interact with two adsorbates to catalyze an asymmetric reaction. We achieve a record n-propanol Faradaic efficiency (FE) of (33 ± 1)% with a conversion rate of (4.5 ± 0.1) mA cm−2, and a record n-propanol cathodic energy conversion efficiency (EEcathodic half-cell) of 21%. The FE and EEcathodic half-cell represent a 1.3× improvement relative to previously-published CO-to-n-propanol electroreduction reports. Catalysts for CO electroreduction have focused on Cu, and their main products have been C2 chemicals. Here authors use the concept of asymmetric active sites to develop a class of doped Cu catalysts for C-C coupling, delivering record selectivity to n-propanol.
129 citations
TL;DR: The large-voltage hysteresis remains one of the biggest barriers to optimizing Li/Na-ion cathodes using lattice anionic redox reaction, despite their very high energy density and relative low cost.
Abstract: The large-voltage hysteresis remains one of the biggest barriers to optimizing Li/Na-ion cathodes using lattice anionic redox reaction, despite their very high energy density and relative low cost....
103 citations
TL;DR: In situ measurements suggest that both the octahedral shape and the fcc crystal structure can be well preserved up to 400 °C, which is more than 100 °C higher than what was reported for RuOctahedral nanocages.
Abstract: Ruthenium nanocrystals with both a face-centered cubic ( fcc) structure and well-controlled facets are attractive catalytic materials for various reactions. Here we report a simple method for the synthesis of Ru octahedral nanocrystals with an fcc structure and an edge length of 9 nm. The success of this synthesis relies on the use of 4.5 nm Rh cubes as seeds to facilitate the heterogeneous nucleation and overgrowth of Ru atoms. We choose Rh because it can resist oxidative etching under the harsh conditions for Ru overgrowth, it can be readily prepared as nanocubes with edge lengths less than 5 nm, and its atoms have a size close to that of Ru atoms. During the seed-mediated growth, the atomic packing of Ru overlayers follows an fcc lattice, in contrast to the conventional hexagonal close-packed ( hcp) lattice associated with bulk Ru. The final product takes an octahedral shape, with the surface enclosed by {111} facets. Our in situ measurements suggest that both the octahedral shape and the fcc crystal structure can be well preserved up to 400 °C, which is more than 100 °C higher than what was reported for Ru octahedral nanocages. When utilized as catalysts, the Ru octahedral nanocrystals exhibited 4.4-fold enhancement in terms of specific activity toward oxygen evolution relative to hcp-Ru nanoparticles. We also demonstrate that Ru{111} facets are more active than Ru{100} facets in catalyzing the oxygen evolution reaction. Altogether, this work offers an effective method for the synthesis of Ru nanocrystals with an fcc structure and well-defined {111} facets, as well as enhanced thermal stability and catalytic activity. We believe these nanocrystals will find use in various catalytic applications.
100 citations
TL;DR: A highly active and durable water oxidation electrocatalyst based on cubic nanocages with a composition of Ir44 Pd10 together with well-defined {100} facets and porous walls of roughly 1.1 nm in thickness is reported.
Abstract: We report a highly active and durable water oxidation electrocatalyst based on cubic nanocages with a composition of Ir44 Pd10 , together with well-defined {100} facets and porous walls of roughly 1.1 nm in thickness. Such nanocages substantially outperform all the water oxidation electrocatalysts reported in literature, with an overpotential of only 226 mV for reaching 10 mA cm-2geo at a loading of Ir as low as 12.5 μgIr cm-2 on the electrode in acidic media. When benchmarked against a commercial Ir/C electrocatalyst at 250 mV of overpotential, such a nanocage-based catalyst not only shows enhancements (18.1- and 26.2-fold, respectively) in terms of mass (1.99 A mg-1Ir ) and specific (3.93 mA cm-2Ir ) activities, but also greatly enhanced durability. The enhancements can be attributed to a combination of multiple merits, including a high utilization efficiency of Ir atoms and an open structure beneficial to the electrochemical oxidation of Ir to the active form of IrOx .
76 citations
TL;DR: It is shown that AgP2 is a stable, selective and efficient syngas catalyst for solar-to-fuel conversion with a 3-fold lower overpotential compared to the benchmark Ag catalyst.
Abstract: Production of syngas with tunable CO/H2 ratio from renewable resources is an ideal way to provide a carbon-neutral feedstock for liquid fuel production. Ag is a benchmark electrocatalysts for CO2-to-CO conversion but high overpotential limits the efficiency. We synthesize AgP2 nanocrystals (NCs) with a greater than 3-fold reduction in overpotential for electrochemical CO2-to-CO reduction compared to Ag and greatly enhanced stability. Density functional theory calculations reveal a significant energy barrier decrease in the formate intermediate formation step. In situ X-ray absorption spectroscopy (XAS) shows that a maximum Faradaic efficiency is achieved at an average silver valence state of +1.08 in AgP2 NCs. A photocathode consisting of a n+p-Si wafer coated with ultrathin Al2O3 and AgP2 NCs achieves an onset potential of 0.2 V vs. RHE for CO production and a partial photocurrent density for CO at −0.11 V vs. RHE (j−0.11, CO) of −3.2 mA cm−2. Conversion of CO2 into value-added chemicals by use of renewable energy is promising to achieve a carbon-neutral energy cycle. Here, the authors show that AgP2 is a stable, selective and efficient syngas catalyst for solar-to-fuel conversion with a 3-fold lower overpotential compared to the benchmark Ag catalyst.
73 citations
TL;DR: A ternary CoPtAu nanoparticle catalyst system, in which Co and Pt form an intermetallic L1₀-structure and Au segregates on the surface to alloy with Pt, which holds great promise as a general fuel cell anode catalyst for renewable energy applications.
Abstract: Efficient electro-oxidation of formic acid, methanol, and ethanol is challenging owing to the multiple chemical reaction steps required to accomplish full oxidation to CO2 . Herein, a ternary CoPtAu nanoparticle catalyst system is reported in which Co and Pt form an intermetallic L10 -structure and Au segregates on the surface to alloy with Pt. The L10 -structure stabilizes Co and significantly enhances the catalysis of the PtAu surface towards electro-oxidation of ethanol, methanol, and formic acid, with mass activities of 1.55 A/mgPt , 1.49 A/mgPt , and 11.97 A/mgPt , respectively in 0.1 m HClO4 . The L10 -CoPtAu catalyst is also stable, with negligible degradation in mass activities and no obvious Co/Pt/Au composition changes after 10 000 potential cycles. The in situ surface-enhanced infrared absorption spectroscopy study indicates that the ternary catalyst activates the C-C bond more efficiently for ethanol oxidation.
66 citations
TL;DR: In situ growth of sub-2-nm Pt particles on a commercial carbon support via the galvanic reaction between a Pt(II) precursor and a uniform film of amorphous Se pre-deposited on the support is reported, leading to a catalytic system with extraordinary activity and durability toward ORR.
Abstract: Carbon-supported Pt nanoparticles are used as catalysts for a variety of reactions including the oxygen reduction reaction (ORR) key to proton-exchange membrane fuel cells, but their catalytic perf...
TL;DR: A simple strategy for developing a cost-effective and efficient Ir-based catalyst toward the oxygen evolution reaction (OER) is to construct a core-shell structure with most of the Ir atoms serving as catalysts as discussed by the authors.
Abstract: A simple strategy for developing a cost-effective and efficient Ir-based catalyst toward the oxygen evolution reaction (OER) is to construct a core–shell structure with most of the Ir atoms serving...
TL;DR: In this paper, a novel and simple route for the conversion of amorphous boron nitride precursors into highly crystalline h-BNs was achieved through a successive dissolution-precipitation/crystallization process in the presence of magnesium.
Abstract: Hexagonal boron nitride (h-BN) is regarded as a graphene analogue and exhibits important characteristics and vast application potentials. However, discovering a facile method for the preparation of nanoporous crystalline h-BN nanosheets (h-BNNS) is still a challenge. Herein, a novel and simple route for the conversion of amorphous h-BN precursors into highly crystalline h-BNNS was achieved through a successive dissolution-precipitation/crystallization process in the presence of magnesium. The h-BNNS has high crystallinity, high porosity with a surface area of 347 m2 g-1 , high purity, and enhanced thermal stability. Improved catalytic performance of crystalline h-BNNS was evidenced by its much higher catalytic efficiency in the dehydrogenation of dodecahydro-N-ethylcarbazole, compared with its amorphous h-BN precursor, as well as other precious-metal-loaded heterogeneous catalysts.
TL;DR: In this article, the authors quantitatively reveal the mobility and lattice occupancy of the two ions individually in protonated cubic Li6.25Al0.25La3Zr2O12 (LLZO).
Abstract: A major challenge toward realizing high-performance aqueous lithium batteries (ALBs) is the utilization of a metallic lithium anode. However, an ideal solid electrolyte that can protect metallic lithium from reacting with aqueous solutions while still maintaining a high lithium ion conduction is not currently available. One obstacle is the lack of a reliable experimental tool to differentiate the conduction behaviour of H+ and Li+ ions in a solid electrolyte. Here, by correlating neutron and electron spectroscopy, we quantitatively reveal the mobility and lattice occupancy of the two ions individually in protonated cubic Li6.25Al0.25La3Zr2O12 (LLZO). Our results not only highlight LLZO as a potential effective separation layer for ALBs but also present a robust method to quantify the mobility of individual mobile ions in solid-state ion conductors.
TL;DR: This work demonstrates the rational synthesis of Ru cuboctahedral nanoframes with enhanced catalytic performance toward hydrazine decomposition and offers the opportunity to engineer both the morphology and crystal phase of Ru nanocrystals for catalytic applications.
Abstract: Owing to their highly open structure and a large number of low-coordination sites on the surface, noble-metal nanoframes are intriguing for catalytic applications. Here, we demonstrate the rational...
11 Jan 2019
TL;DR: In this paper, Al2O3 ALD coatings on LiNi0.8Mn0.1Co0.15Al 0.05O2 (NCA) cathodes prevented surface phase transitions, reduced impedance, and extended cycle life in high voltage cells.
Abstract: Recent achievements in high-energy batteries have been made by using Ni-rich NMC cathodes (LiNixMnyCo1–x–yO 2with x > 0.5) in conjunction with higher cell voltages. However, these gains have come at a cost of fast capacity fade and poor rate performace. In our previous study, we showed that Al2O3 ALD coatings on LiNi0.8Mn0.1Co0.1O2 (NMC811) and LiNi0.8Co0.15Al0.05O2 (NCA) cathodes prevented surface phase transitions, reduced impedance, and extended cycle life in high voltage cells. Here, neutron diffraction (ND), X-ray photoelectron spectroscopy (XPS), and electron energy loss spectroscopy (EELS) are used to fully investigate the mechanism by which ALD surface coatings mitigate NMC811 cathode degredation. Refinement of ND patterns indicated no changes in the bulk crystal structure of cycled cathodes with or without the Al2O3 coating. Rather, the improved performance of ALD-coated cathodes is clearly due to surface stabilization. EELS established that all three transition metal oxidation states were reduce...
TL;DR: In this article, a facile one-pot synthesis of Pd@Pt1L (1L: one atomic layer) core-shell octahedra using a solution-phase method was reported.
Abstract: A successful strategy for reducing the content of Pt without compromising the activity of a Pt-based catalyst is to deposit Pt as an ultrathin overlayer on the surface of another metal. Here, we report a facile one-pot synthesis of Pd@Pt1L (1L: one atomic layer) core–shell octahedra using a solution-phase method. The success of this method relies on the use of metal precursors with markedly different reduction kinetics. In a typical synthesis, the ratio between the initial reduction rates of the Pd(II) and Pt(II) precursors differed by almost 100 times, favoring the formation of Pd–Pt bimetallic octahedra with a core–shell structure. The reduction of the Pt(II) precursor at a very slow rate and the use of a high temperature allowed the deposited Pt atoms to spread and cover the entire surface of Pd octahedral seeds formed in the initial stage. More importantly, we were able to scale up this synthesis using continuous-flow reactors without compromising product quality. Compared to a commercial Pt/C catalys...
TL;DR: A systematic study of the photothermal transformation of Au-Ag nanocages with a localized surface plasmon resonance at ca.
Abstract: Pulsed laser irradiation has emerged as an effective means to photothermally transform plasmonic nanostructures after their use in different biomedical applications. However, the ability to predict the products after photothermal transformation requires extensive ex situ studies. Here, we report a systematic study of the photothermal transformation of Au-Ag nanocages with a localized surface plasmon resonance at ca. 750 nm under pulsed laser irradiation at different fluences and a pulse duration of 5 ns. At biologically relevant laser energies, the pulsed laser transforms Au-Ag nanocages into pseudo-spherical, solid nanoparticles. The solid nanoparticles contained similar numbers of Au and Ag atoms to the parent Au-Ag nanocages. At increased laser fluences (>16 mJ cm-2) and number of pulses (>150), the average diameter of the resulting pseudo-spherical particles increased due to the involvement of Ostwald ripening and/or attachment-based growth. The changes in optical properties as a result of the transformation were validated using simulations based on the discrete dipole approximation method, where the spectral profiles and peak positions of the initial and final states matched well with the experimentally derived data. The results may have implications for the future use of Au-Ag nanocages in biomedicine, catalysis, and sensing.
TL;DR: In this article, the authors discuss experimental techniques that allow for atomic-to-microscale understanding of ion transport and stability in SEs and at their interfaces, specifically highlighting the applications of state-of-the-art and emerging ex situ and in situ transmission electron microscopy (TEM) and scanning TEM (STEM).
Abstract: Solid electrolytes (SEs) have gained increased attention for their promise to enable higher volumetric energy density and enhanced safety required for future battery systems. SEs are not only a key constituent in all-solid-state batteries, but also important “protectors” of Li metal anodes in next-generation battery configurations, such as Li–air, Li–S, and redox flow batteries. The impedance at interfaces associated with SEs, e.g., internal grain/phase boundaries and their interfacial stability with electrodes, represents two key factors limiting the performance of SEs, yet analyzing these interfaces experimentally at the nano/atomic scale is generally challenging. A mechanistic understanding of the possible instability at interfaces and propagation of interfacial resistance will pave the way to the design of high-performance SE-based batteries. In this review, we briefly introduce the fundamentals of SEs and challenges associated with their interfaces. Next, we discuss experimental techniques that allow for atomic-to-microscale understanding of ion transport and stability in SEs and at their interfaces, specifically highlighting the applications of state-of-the-art and emerging ex situ and in situ transmission electron microscopy (TEM) and scanning TEM (STEM). Representative examples from the current literature that exemplify recent fundamental insights gained from these S/TEM techniques are highlighted. Applicable strategies to improve ion conduction and interfaces in SE-based batteries are also discussed. This review concludes by highlighting opportunities for future research that will significantly promote the fundamental understanding of SEs, specifically further developments in S/TEM techniques that will bring new insights into the design of high-performance interfaces for future electrical energy storage.
TL;DR: In this paper, a hollow nanosheet using Co2SiO4 as demonstrating example is presented, which exhibits a high and stable capacity of 1456 mAh g−1 after 200 cycles at 0.2 A g− 1, and an excellent rate-performance after three rounds of cycling.
19 Aug 2019
TL;DR: In this paper, a facile synthesis of Pd@Rh core-shell nanocrystals with octahedral and cubic shapes was reported, and the results indicated that there was no significant difference between the octagonal and cubic Pd-@Rh nanocrysts in terms of performance towards CO oxidation while both of them are advantageous over Rh nanocubes or Rh/C.
Abstract: Here we report a facile synthesis of Pd@Rh core–shell nanocrystals with octahedral and cubic shapes. Under optimized conditions, Rh atoms can be deposited on Pd octahedral or cubic seeds in a layer-by-layer fashion to generate core–shell nanocrystals with a well-controlled shape. We then use CO oxidation as a probe to evaluate the catalytic performance of the core–shell nanocrystals with reference to a number of commercial catalysts. When supported on mesoporous silica, both the octahedral and cubic Pd@Rh nanocrystals show CO to CO2 conversion levels similar to that of a commercial Pt/Al2O3 catalyst while the two catalysts based on pure Rh (commercial Rh/C and Rh nanocubes/silica) needed much higher temperatures to reach the same level of conversion. In terms of ignition temperature, the Rh nanocubes show a value of 260 °C while those of the octahedral and cubic Pd@Rh nanocrystals are as low as 140 and 150 °C, respectively. Our results suggest that there is no significant difference between the octahedral and cubic Pd@Rh nanocrystals in terms of performance towards CO oxidation while both of them are advantageous over Rh nanocubes or Rh/C.
TL;DR: In this paper, the authors reported a facile route to the quick synthesis of Pt icosahedral nanocrystals with tunable sizes by simply varying the amount of the precursor.
Abstract: Platinum icosahedral nanocrystals are intriguing catalytic materials owing to the presence of a large number of twin boundaries and well‐defined {111} facets on the surface. However, there are only two protocols available for their synthesis and the protocols required either the involvement of a metal carbonyl as the reductant or a very long reaction time up to one week. Here we report a facile route to the quick synthesis of Pt icosahedral nanocrystals with tunable sizes. The synthesis only involved Pt(acac)2, tetraethylene glycol, poly(vinyl pyrrolidone), and as the metal precursor, solvent/reductant, and colloidal stabilizer, respectively. Noticeably, the synthesis could be completed within 20 min. By simply varying the amount of the precursor, we were able to tune the size of the Pt icosahedral nanocrystals in the range of 10–25 nm. Additionally, when ascorbic acid was introduced as a co‐reductant to facilitate the reduction of the precursor, the size of the Pt icosahedral nanocrystals could be further reduced down to 7–12 nm. When used as a catalyst towards the oxygen reduction reaction, the Pt icosahedral nanocrystals with different sizes all exhibited a specific activity more than 2.4 times greater than that of commercial Pt/C. Moreover, their specific activity increased with the particle size. After 5,000 cycles of the accelerated durability test, the specific activities of the Pt icosahedral nanocrystals with three different sizes were still more than 2 times as high as that of the commercial Pt/C catalyst.
TL;DR: A three-dimensional all-in-one Sn-Co alloy anode is reported for the first time, which delivers a high capacity along with a stable coulombic efficiency as well as good temperature tolerance.
TL;DR: In this paper, a yolk-shell-like FePt-FeOx nanoparticles (NPs) were designed for CO oxidation at relatively low temperatures, which exhibited notably enhanced activity and stability towards CO oxidation.
TL;DR: In this article, Nelson et al. presented a model of the nanophase materials at the Center for Nanophase Materials Sciences (CNMMS) at Oak Ridge National Laboratory (ORNL).
Abstract: 1. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN USA. 2. Materials Science and Engineering, Pennsylvania State University, State College, PA USA. 3. Materials Science and Engineering, University of Tennessee, Knoxville, TN USA. 4. Materials Science and Engineering, University of California, Berkeley, CA USA. 5. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA USA. * Corresponding author: nelsonct@ornl.gov
TL;DR: In this paper, the intrinsic defects in boron arsenide (BAs) have been identified and direct observation and identification of these defects have become quite urgent for growth of high quality BAs crystals or films.
Abstract: As microelectronic devices become faster and smaller, materials with ultrahigh thermal conductivity (κ) are becoming important for new generation electronic devices. Recently, based on first-principles calculations, boron arsenide (BAs) with a zinc blende-type cubic structure was predicted to possess an unusually high κ at room temperature of over 2000 Wm K, comparable to that of diamond [1]. However, the experimentally measured κ of BAs single crystals was only 200~350 Wm K for a few years, an order of magnitude lower than the predicted value [2-3]. Although theoretical calculations [4] and x-ray photoelectron spectroscopy (XPS) studies [2,3] reveal that As vacancies (VAs), even with very low concentration, could significantly suppress κ, VAs in BAs materials has never been directly observed to date. Therefore, direct observation and identification of the intrinsic defects in BAs that suppress κ become quite urgent for growth of high-quality BAs crystals or films.
TL;DR: In this paper, LiNi0.8Co0.15Al0.05O2 and LiNi1-x-yCoxMnyO2 (NCM, 1 x-y≥0.5) are two representative layered oxide materials that have attracted the most attention; however, NCA experiences significant capacity fade during long-term cycling.
Abstract: Nickel-rich layered oxides have been widely used in commercial Li-ion batteries (LIB) due to their high capacity (~ 200 mAh/g until ~4.6 V vs. Li/Li+) and excellent rate performance. Among this family, LiNi0.8Co0.15Al0.05O2 (NCA) and LiNi1-x-yCoxMnyO2 (NCM, 1-x-y≥0.5) are two representative layered oxide materials that have attracted the most attention; however, NCA experiences significant capacity fade during long-term cycling [1]. Even though NCM possesses improved energy density and better thermal stability compared to NCA, the performance deterioration is still a critical challenge for LIBs. Thus, understanding the underlying mechanisms of the performance degradation is essential for developing state-of-the-art LIBs, which are suitable for applications in electric vehicles and grid energy storage systems.