The need for enhanced energy storage and improved catalysts has led researchers to explore advanced functional materials for sustainable energy production and storage. Herein, we demonstrate a reductive electrosynthesis approach to prepare a layer-by-layer (LbL) assembled trimetallic Fe−Co−Ni metal−organic framework (MOF) in which the metal cations within each layer or at the interface of the two layers are linked to one another by bridging 2-amino-1,4-benzenedicarboxylic acid linkers. Tailoring catalytically active sites in an LbL fashion affords a highly porous material that exhibits excellent trifunctional electrocatalytic activities toward the hydrogen evolution reaction (η j=10 = 116 mV), oxygen evolution reaction (η j=10 = 254 mV), as well as oxygen reduction reaction (half-wave potential = 0.75 V vs reference hydrogen electrode) in alkaline solutions. The dispersion-corrected density functional theory calculations suggest that the prominent catalytic activity of the LbL MOF toward the HER, OER, and ORR is due to the initial negative adsorption energy of water on the metal nodes and the elongated O−H bond length of the H 2 O molecule. The Fe−Co−Ni MOF-based Zn−air battery exhibits a remarkable energy storage performance and excellent cycling stability of over 700 cycles that outperform the commercial noble metal benchmarks. When assembled in an asymmetric device configuration, the activated carbon||Fe−Co−Ni MOF supercapacitor provides a superb specific energy and a power of up to 56.2 W h kg −1 and 42.2 kW kg −1 , respectively. This work offers not only a novel approach to prepare an LbL assembled multimetallic MOF but also provides a benchmark for a multifunctional electrocatalyst for water splitting and Zn−air batteries.

Gas flows are often analyzed with the theoretical descriptions formulated over a century ago and constantly challenged by the emerging architectures of narrow channels, slits, and apertures. Here, we report atomic-scale defects in two-dimensional (2D) materials as apertures for gas flows at the ultimate quasi-0D atomic limit. We establish that pristine monolayer tungsten disulfide (WS2) membranes act as atomically thin barriers to gas transport. Atomic vacancies from missing tungsten (W) sites are made in freestanding (WS2) monolayers by focused ion beam irradiation and characterized using aberration-corrected transmission electron microscopy. WS2 monolayers with atomic apertures are mechanically sturdy and showed fast helium flow. We propose a simple yet robust method for confirming the formation of atomic apertures over large areas using gas flows, an essential step for pursuing their prospective applications in various domains including molecular separation, single quantum emitters, sensing and monitoring of gases at ultralow concentrations.

We report the formation of nanobubbles on graphene with a radius of the order of 1 nm, using ultralow energy implantation of noble gas ions (He, Ne, Ar) into graphene grown on a Pt(111) surface. We show that the universal scaling of the aspect ratio, which has previously been established for larger bubbles, breaks down when the bubble radius approaches 1 nm, resulting in much larger aspect ratios. Moreover, we observe that the bubble stability and aspect ratio depend on the substrate onto which the graphene is grown (bubbles are stable for Pt but not for Cu) and trapped element. We interpret these dependencies in terms of the atomic compressibility of the noble gas as well as of the adhesion energies between graphene, the substrate, and trapped atoms.

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Despite their low cost, safety, environmentally friendliness, and intrinsic non‐flammable nature, the widespread application of aqueous rechargeable zinc‐based batteries has been held back by their low coulombic efficiency and the notorious dendritic growth at the zinc‐based anodes, along with the fast capacity fading of the cathodes. Herein, an aqueous Zn superbattery that consists of a mixed ZnCO3 MnCO3 grafted onto a graphene aerogel (ZMG) negative electrode and a nanotubular sulfidated NiCoFe layered double hydroxide (LDHS) positive electrode is reported. The alkaline ZMG││LDHS superbattery delivers an excellent capacity and a superb rate capability (356 mA h g−1cathode (89 mA h g−1total mass) at 12 A g−1; 108 mA h g−1cathode at 300 A g−1), extremely high specific energy and power (568 W h kg−1cathode or 15.8 mW h cm−3, 429 kW kg−1cathode or 11.9 W cm−3), along with a high output voltage (1.8 V). The device also exhibits unprecedented cycling stability (99.2% capacity retention after 17,000 cycles at 100% depth of discharge) thanks to an electrochemical pulse‐driven regenerative mechanism.