High-voltage operation is essential for the energy and power densities of battery cathode materials, but its stabilization remains a universal challenge. To date, the degradation origin has been mostly attributed to cycling-initiated structural deformation while the effect of native crystallographic defects induced during the sophisticated synthesis process has been significantly overlooked. Here, using in situ synchrotron X-ray probes and advanced transmission electron microscopy to probe the solid-state synthesis and charge/discharge process of sodium layered oxide cathodes, we reveal that quenching-induced native lattice strain plays an overwhelming role in the catastrophic capacity degradation of sodium layered cathodes, which runs counter to conventional perception-phase transition and cathode interfacial reactions. We observe that the spontaneous relaxation of native lattice strain is responsible for the structural earthquake (e.g., dislocation, stacking faults and fragmentation) of sodium layered cathodes during cycling, which is unexpectedly not regulated by the voltage window but is strongly coupled with charge/discharge temperature and rate. Our findings resolve the controversial understanding on the degradation origin of cathode materials and highlight the importance of eliminating intrinsic crystallographic defects to guarantee superior cycling stability at high voltages.

Lattice (music)

10.1038/s41467-022-28052-x

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Citations (62)

In situ microscopy and spectroscopy characterization of microsized Sn anode for sodium-ion batteries

Nano Energy (2023)

Amine Daali Xinwei Zhou Chen Zhao Inhui Hwang Zhenzhen Yang

10.1016/j.nanoen.2023.108753

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Sustainable layered cathode with suppressed phase transition for long-life sodium-ion batteries

Nature Sustainability (2024)

Yonglin Tang Qinghua Zhang Wenhua Zuo Shiyuan Zhou Guifan Zeng

Capacity loss

Sodium-ion battery

10.1038/s41893-024-01288-9

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Dispersion and stability mechanism of Pt nanoparticles on transition-metal oxides

Scientific Reports (2022)

Eun‐Suk Jeong Inhui Hwang Sang-Wook Han

The heterogeneous catalysts of Pt/transition-metal oxides are typically synthesized through calcination at 500 °C, and Pt nanoparticles are uniformly and highly dispersed when hydrogen peroxide (H2O2) is applied before calcination. The influence of H2O2 on the dispersion and the stability of Pt nanoparticles on titania-incorporated fumed silica (Pt/Ti-FS) supports was examined using X-ray absorption fine structure (XAFS) measurements at the Pt L3 and Ti K edges as well as density functional theory (DFT) calculations. The local structural and chemical properties around Pt and Ti atoms of Pt/Ti-FS with and without H2O2 treatment were monitored using in-situ XAFS during heating from room temperature to 500 °C. XAFS revealed that the Pt nanoparticles of H2O2-Pt/Ti-FS are highly stable and that the Ti atoms of H2O2-Pt/Ti-FS support form into a distorted-anatase TiO2. DFT calculations showed that Pt atoms bond more stably to oxidized-TiO2 surfaces than they do to bare- and reduced-TiO2 surfaces. XAFS measurements and DFT calculations clarified that the presence of extra oxygen atoms due to the H2O2 treatment plays a critical role in the strong bonding of Pt atoms to TiO2 surfaces.

Rutile

10.1038/s41598-022-17638-6

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The influence of structural disorder and phonon on metal-to-insulator transition of VO 2

Scientific Reports (2017)

Inhui Hwang Zhenlan Jin Chang-In Park Sang-Wook Han

We used temperature-dependent x-ray absorption fine structure (XAFS) measurements to examine the local structural properties around vanadium atoms at the V K edge from VO2 films. A direct comparison of the simultaneously-measured resistance and XAFS regarding the VO2 films showed that the thermally-driven structural transition occurred prior to the resistance transition during a heating, while this change simultaneously occured during a cooling. Extended-XAFS (EXAFS) analysis revealed significant increases of the Debye-Waller factors of the V-O and V-V pairs in the {111} direction of the R-phase VO2 that are due to the phonons of the V-V arrays along the same direction in a metallic phase. The existance of a substantial amount of structural disorder on the V-V pairs along the c-axis in both M1 and R phases indicates the structural instability of V-V arrays in the axis. The anomalous structural disorder that was observed on all atomic sites at the structural phase transition prevents the migration of the V 3d1 electrons, resulting in a Mott insulator in the M2-phase VO2.

Metal–insulator transition

10.1038/s41598-017-14235-w

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Citations (16)