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Non‐equilibrium defects often dictate the macroscopic properties of materials. They largely define the reversibility and kinetics of processes in intercalation hosts in rechargeable batteries. Recently, imaging methods have demonstrated that transient dislocations briefly appear in intercalation hosts during ion diffusion. Despite new discoveries, the understanding of impact, formation and self‐healing mechanisms of transient defects, including and beyond dislocations, is lacking. Here, operando X‐ray Bragg Coherent Diffractive Imaging (BCDI) and diffraction peak analysis capture the stages of formation of a unique metastable domain boundary, defect self‐healing, and resolve the local impact of defects on ionic diffusion in NaxNi1−yMnyO2 intercalation hosts in a charging sodium‐ion battery. Results, applicable to a wide range of layered intercalation materials due to the shared nature of framework layers, elucidate new dynamics of transient defects and their connection to macroscopic properties, and suggest how to control the nanostructure dynamics. [ABSTRACT FROM AUTHOR]

Despite their safe and cost‐effective merits, the cycling durability of aqueous zinc–organic batteries is hindered by cathode dissolution and low coulombic efficiency of Zn metal anodes. Herein, a Zn metal‐free all‐organic zinc‐ion battery (ZIB) is proposed by using quinoxalino[2,3‐i]diquinoxalino[2′,3′:6,7]quinoxalino[2,3‐a:2,3‐c] phenazine (QDPA) cathode coupled with a 1,4,5,8‐Naphthalenetetracarboxylic diimide (NPI) anode, rendering excellent electrochemical reversibility with high utilization. Based on the molecular architecture strategy, a QDPA cathode with an enlarged aromatic ring system is designed and synthesized, which not only effectively inhibits structural collapse during cycling but also enhances the working voltage without lowering the active group ratio. Moreover, theoretical calculations and experimental results confirm the rapid H+ storage mechanism in the CN active sites of QDPA, affording ultra‐fast electrochemical kinetics. Thus, it delivers a negligible capacity decay of 0.002% up to 13 000 cycles at 20 A g−1. Moreover, the QDPA//NPI all‐organic aqueous ZIB with a high energy density of 43.1 Wh kg−1 is demonstrated to be easily disassembled and recycled by the incineration treatment after battery failure, ensuring outstanding environmental sustainability. [ABSTRACT FROM AUTHOR]

Batteries, diffraction, operando, single-particles, sodium-ions Disorder Dynamics in Battery Nanoparticles During Phase Transitions Revealed by Operando Single-Particle Diffraction (Adv. Keywords: batteries; diffraction; operando; single-particles; sodium-ions EN batteries diffraction operando single-particles sodium-ions 1 1 1 03/28/22 20220324 NES 220324 B Sodium-Ion Batteries b In article number 2103521, Jason J. Huang and co-workers use operando single particle X-ray diffraction to probe disorder dynamics in individual cathode particles of Nax[Ni SB 1/3 sb Mn SB 2/3 sb ]O SB 2 sb , an archetypal cathode material for sodium-ion batteries. [Extracted from the article]