Operando leaching of pre-incorporated Al and mechanism in transition-metal hybrids on carbon substrates for enhanced charge storage

•A "nano-tailoring" strategy via electrochemical leaching of Al species is proposed•Defective and highly active materials were formed the strategy•The integrated oxygen vacancies can boost charge storage potassium-birnessite•The reducibility M2+ identified as key descriptor for reconstruction rate From viewpoint optimizing charge-storage dynamics, we first time propose a universal to fabricate low-crystalline electrochemically dynamic pre-incorporated Al. With M2+Al hydroxides precursor, potassium-birnessite MnO2 with abundant defective sites enriched edge-active configured, resulting in enhanced capability. Soft XAS Raman mapping techniques are adopted finely track principles intrinsic sites. It found that serves rate, which correspondingly divided into two branches: oxidization-boosting type non-oxidization type. This work provide novel avenue spark new ideas modulate ameliorate electrode advanced energy conversion applications future. Insufficient exposure utilization often induces an inferior reactivity transition-metal-based two-dimensional (2D) materials. In response, incorporate defects low-crystallinity nanosheets by species. MnAl layered double (LDHs) representative example, (AK-MnO2) edge successfully produced. The shown help optimize electron-transfer ion-adsorption These advantages endow AK-MnO2 high capacitance value 239 F g−1 at 100 A g−1. By further combining soft X-ray absorption spectroscopy techniques, unravel M2+Al-LDH rate. some important implications clues manipulating 2D efficient conversion. development social science technology, strong need fast, sustainable, high-power energy-storage systems has led quick supercapacitors, be kinds: electric double-layer capacitors (EDLCs) pseudocapacitors (PCs).1Simon P. Gogotsi Y. Perspectives related devices.Nat. Mater. 2020; 19: 1151-1163Crossref PubMed Scopus (478) Google Scholar,2Noori A. El-Kady M.F. Rahmanifar M.S. Kaner R.B. 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Interestingly, due irreversible intercalation K+, undergo emergence release strain, positively tailored vacancies. Also, functional theory (DFT) calculation demonstrates capable facilitating adsorption ions, optimized kinetics storage. As such, as-formed deliver 356 1 retention 67% super-large current indicative More importantly, universality deeply verified We reveal transformation dependent M2+, acts prominent factor believed unique stimulate broad interest inspiration researchers configure properties. illustrated Figure 1A, involves M2+Al-based binary where breakage happens during scanning medium. process, MnAl-LDH will MnAl-based accompanied partial Al, when soaked short (2 min), yielding Mn(Al)-OH intermediate. Subsequently, reconstructed birnessite-type K+ interlayer cyclic voltammetry (CV) cycling treatment, denoted AK-MnO2. ex electron microscopy (SEM) images size distributions. Figures 1B–1D, large broken smaller stacking density. average decreases 726 nm 202 finally 55 (about 13 times decrease size). Notably, small dense numerous short-distance channels fast transfer, beneficial uncovered transmission (TEM) images. depicted S1A, precursor size, spacing 0.26 corresponds (012) plane LDH. Mn(Al)-OH, situ-formed holes observed, 0.33 (100) Mn(OH)2 (Figure S1B). Impressively, well-tailored densely stacked ultrasmall nanosheet 1E) crystallinity, high-resolution (HR)-TEM image 1F). selected diffraction (SAED), no patterns detected 1F), generation distortion randomly construction. 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