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Operating a lithium‐ion battery (LIB) in a wide temperature range is essential for ensuring a stable electricity supply amidst fluctuating temperatures caused by climate or terrain changes. Electrolyte plays a pivotal role in determining the temperature durability of batteries. However, specialized electrolytes designed for either low or high temperatures typically possess distinct features. Therefore, wide‐temperature electrolytes (WTEs) are necessary as they encompass a combination of diverse properties, which complicates the clear instruction of WTE design. Here we represent an artificial intelligence (Al)‐assisted workflow of WTE design through stepwise parameterizations and calculations. Linear mono‐nitriles are identified as ideal wide‐liquidus‐range solvents that can "softly" solvate lithium ions by weak interactions. In addition, the explainable modules revealed the halogenoid similarity of cyanide as fluorine on the electrolyte properties (e.g. boiling point and dielectric constant). With the further introduction of an ether bond, 3‐methoxypropionitrile (MPN) has been eventually determined as a main electrolyte solvent, enabling the battery operation from −60 to 120 °C. Particularly, a LiCoO2/Li cell using the proposed WTE can realize stable cycling with capacity retention reaching 72.3 % after 50 cycles under a high temperature of 100 °C. [ABSTRACT FROM AUTHOR]

The atom‐cluster interaction has recently been exploited as an effective way to increase the performance of metal‐nitrogen‐carbon catalysts for oxygen reduction reaction (ORR). However, the rational design of such catalysts and understanding their structure‐property correlations remain a great challenge. Herein, we demonstrate that the introduction of adjacent metal (M)−N4 single atoms (SAs) could significantly improve the ORR performance of a well‐screened Fe atomic cluster (AC) catalyst by combining density functional theory (DFT) calculations and experimental analysis. The DFT studies suggest that the Cu−N4 SAs act as a modulator to assist the O2 adsorption and cleavage of O−O bond on the Fe AC active center, as well as optimize the release of OH* intermediates to accelerate the whole ORR kinetic. The depositing of Fe AC with Cu−N4 SAs on nitrogen doped mesoporous carbon nanosheet are then constructed through a universal interfacial monomicelles assembly strategy. Consistent with theoretical predictions, the resultant catalyst exhibits an outstanding ORR performance with a half‐wave potential of 0.92 eV in alkali and 0.80 eV in acid, as well as a high power density of 214.8 mW cm−2 in zinc air battery. This work provides a novel strategy for precisely tuning the atomically dispersed poly‐metallic centers for electrocatalysis. [ABSTRACT FROM AUTHOR]

Charge compensation on anionic redox reaction (ARR) has been promising to realize extra capacity beyond transition metal redox in battery cathodes. The practical development of ARR capacity has been hindered by high‐valence oxygen instability, particularly at cathode surfaces. However, the direct probe of surface oxygen behavior has been challenging. Here, the electronic states of surface oxygen are investigated by combining mapping of resonant Auger electronic spectroscopy (mRAS) and ambient pressure X‐ray photoelectron spectroscopy (APXPS) on a model LiCoO2 cathode. The mRAS verified that no high‐valence oxygen can sustain at cathode surfaces, while APXPS proves that cathode electrolyte interphase (CEI) layer evolves and oxidizes upon oxygen gas contact. This work provides valuable insights into the high‐valence oxygen degradation mode across the interface. Oxygen stabilization from surface architecture is proven a prerequisite to the practical development of ARR active cathodes. [ABSTRACT FROM AUTHOR]

To boost the performance for various applications, a rational bottom‐up design on materials is necessary. The defect engineering on nanoparticle at the atomic level can efficiently tune the electronic behavior, which offers great opportunities in enhancing the catalytic performance. In this paper, we optimized the surface oxygen vacancy concentration and created the lattice distortion in rare‐earth‐based perovskite oxide through gradient replacement of the B site with valence alternated element. The dual defects make the electron spin state transit from low spin state to high spin state, thus decreasing the charge transport resistance. Furthermore, assembly the modified nanoparticle subunits into the micro‐sized hollow multishelled structures can provide porous shells, abundant interior space and effective contact, which enables an enhanced mass transfer and a shorter charge transport path. As a result, the systemic design in the electronic and nano‐micro structures for catalyst has brought an excellent oxygen evolution performance. [ABSTRACT FROM AUTHOR]