Correlating advanced microscopies reveals atomic-scale mechanisms limiting lithium-ion battery lifetime

The longevity of a lithium-ion battery is limited by cathode degradation. Combining atom probe tomography and scanning transmission electron microscopy reveals that the degradation results from atomic-scale irreversible structural changes once lithium leaves the cathode during charging, thereby inhibiting lithium intercalation back into the cathode as the battery discharges. This information unveils possible routes for improving the lifetime of lithium-ion batteries

On spinodal decomposition in alnico---a transmission electron microscopy and atom probe tomography study

Alnico is a prime example of a finely tuned nanostructure whose magnetic properties are intimately connected to magnetic annealing (MA) during spinodal transformation and subsequent lower temperature annealing (draw) cycles. Using a combination of transmission electron microscopy and atom probe tomography, we show how these critical processing steps affect the local composition and nanostructure evolution with impact on magnetic properties. The nearly 2-fold increase of intrinsic coercivity ($H_\text{ci}$) during the draw cycle is not adequately explained by chemical refinement of the spinodal phases. Instead, increased Fe-Co phase ($\alpha_1$) isolation, development of Cu-rich spheres/rods/blades and additional $\alpha_1$ rod precipitation that occurs during the MA and draw, likely play a key role in $H_\text{ci}$ enhancement. Chemical ordering of the Al-Ni-phase ($\alpha_2$) and formation of Ni-rich ($\alpha_3$) may also contribute. Unraveling of the subtle effect of these nano-scaled features is crucial to understanding on how to improve shape anisotropy in alnico magnets

Peierls barrier characteristic and anomalous strain hardening provoked by dynamic-strain-aging strengthening in a body-centered-cubic high-entropy alloy

The temperature effect on the mechanical behavior of the HfNbTaTiZr high entropy alloy (HEA) was investigated at 77–673 K. The decrease of the yield strength with increasing the temperature was mechanistically analyzed by considering contributions from various strengthening mechanisms. An anomalous dependence of strain hardening on temperature was observed and was justified to be caused by dynamic strain aging (DSA) as an extra strengthening mechanism at elevated temperatures. A model was constructed to split the overall strain hardening into forest hardening and DSA hardening, both of which were theoretically quantified at all temperatures considered. The work quantifies the height of Peierls barriers in the bcc HfNbTaTiZr HEA, and reveals dynamic strain aging as the strengthening mechanism causing the anomalous strain hardening at elevated temperatures

Elucidating the Structure and Composition of Individual Bimetallic Nanoparticles in Supported Catalysts by Atom Probe Tomography

Understanding and controlling the structure and composition of nanoparticles in supported metal catalysts are crucial to improve chemical processes. For this, atom probe tomography (APT) is a unique tool, as it allows for spatially resolved three-dimensional chemical imaging of materials with sub-nanometer resolution. However, thus far APT has not been applied for mesoporous oxide-supported metal catalyst materials, due to the size and number of pores resulting in sample fracture during experiments. To overcome these issues, we developed a high-pressure resin impregnation strategy and showcased the applicability to high-porous supported Pd-Ni-based catalyst materials, which are active in CO2 hydrogenation. Within the reconstructed volume of 3 × 105 nm3, we identified over 400 Pd-Ni clusters, with compositions ranging from 0 to 16 atom % Pd and a size distribution of 2.6 ± 1.6 nm. These results illustrate that APT is capable of quantitatively assessing the size, composition, and metal distribution for a large number of nanoparticles at the sub-nm scale in industrial catalysts. Furthermore, we showcase that metal segregation occurred predominately between nanoparticles, shedding light on the mechanism of metal segregation. We envision that the presented methodology expands the capabilities of APT to investigate porous functional nanomaterials, including but not limited to solid catalysts

Author Correction: Correlating advanced microscopies reveals atomic-scale mechanisms limiting lithium-ion battery lifetime (Nature Communications, (2021), 12, 1, (3740), 10.1038/s41467-021-24121-9)

The original version of this Article omitted a reference to previous work in “Chae, B. G. et al. Evolution and expansion of Li concentration gradient during charge–discharge cycling. Nat Commun 12, 3814 (2021)”. This has been added as reference [14] at “Chae et al. combined... [14]”. This has been corrected in the PDF and HTML versions of the Article. © 2021 The Author(s)