The structure design and atomic modulation of catalysts are two sides of the same coin, both of which are deemed critical factors to regulate the intrinsic electrocatalytic activity. Herein, cobalt single‐atom anchored on nitrogen‐doped graphene‐sheet@tube (CoSAs‐NGST) is derived from a novel Co, Zn‐coordinated zeolitic imidazolate framework (CoZn‐ZIF) in the presence of dicyandiamide. CoSAs‐NGST exhibited a hybrid structure with a bamboo‐like graphene tube and sheet. The atomic configuration of intrinsic defects is characterized by electron energy loss spectroscopy. The morphology differentiation from cake‐shape structure to low‐dimension hybrid not only enhances the dispersity of single atoms but also induces defect state evolution, which results in the formation of a CoN4‐rich graphene tube. Density functional theory (DFT) modeling revealed that the coupling effect on oxygen reduction reaction and oxygen evolution reaction (ORR/OER) pathways of Co‐N4‐tube and Co‐N4‐sheet is responsible for the enhanced activity of CoSAs‐NGST. In addition to the superb ORR/OER bifunctional catalytic performance, CoSAs‐NGST also demonstrates a notably small charge–discharge voltage drop of 0.93 V when applied in the rechargeable zinc–air battery outperforming Pt/C + RuO2 catalyst. The present study provides an insight into the relationship between the structure design and atomic modulation of the carbon based catalysts.

Transition metal dichalcogenides (TMDs) (MX 2 , M = Mo or W, X = S, Se, or Te) have attracted intense interest for developing ultrascaled electronics and optoelectronics by virtue of their attractive 2D layered structures and unique physical properties that are absent in their bulk counterparts. [1][2][3][4][5] Monolayer semiconducting TMDs show sizable direct bandgaps, quantum confinement effects, large exciton binding energies and effective valley polarizations, which unveils widespread applications in field-effect transistors (FETs), photodetectors, light-emitting diodes, pumped lasers, solar cells, and valleytronic devices. [6][7][8][9][10] More excitingly, their 2D structures offer superior electrostatic controllability and exemptible short-channel effects, rendering TMDs promising candidates for future sub-10 nm complimentary metal-oxide-semiconductor (CMOS) devices. [5,11,12] The applications of exfoliated TMD flakes in building high-performance prototypes of electronics, photonics, and optoelectronics have already been demonstrated. [13][14][15][16] The exfoliated flakes, however, suffer from Monolayer MoTe 2 , with the narrowest direct bandgap of ≈1.1 eV among Mo-and W-based transition metal dichalcogenides, has attracted increasing attention as a promising candidate for applications in novel near-infrared electronics and optoelectronics. Realizing 2D lateral growth is an essential prerequisite for uniform thickness and property control over the large scale, while it is not successful yet. Here, layer-by-layer growth of 2 in. wafer-scale continuous monolayer 2H-MoTe 2 films on inert SiO 2 dielectrics by molecular beam epitaxy is reported. A single-step Mo-flux controlled nucleation and growth process is developed to suppress island growth. Atomically flat 2H-MoTe 2 with 100% monolayer coverage is successfully grown on inert 2 in. SiO 2 /Si wafer, which exhibits highly uniform in-plane structural continuity and excellent phonon-limited carrier transport behavior. The dynamics-controlled growth recipe is also extended to fabricate continuous monolayer 2H-MoTe 2 on atomic-layer-deposited Al 2 O 3 dielectric. With the breakthrough in growth of wafer-scale continuous 2H-MoTe 2 monolayers on device compatible dielectrics, batch fabrication of high-mobility monolayer 2H-MoTe 2 field-effect transistors and the three-level integration of vertically stacked monolayer 2H-MoTe 2 transistor arrays for 3D circuitry are successfully demonstrated. This work provides novel insights into the scalable synthesis of monolayer 2H-MoTe 2 films on universal substrates and paves the way for the ultimate miniaturization of electronics.

The argyrodite sulfides are getting more and more attractive as highly promising solid-state electrolytes (SSEs) for high-performance all-solid-state batteries (ASSBs), owing to their high ionic conductivity, adequate plasticity, and decent mechanical strength.However, their poor incompatibility with Li metal anode and high voltage cathodes and as well as serious sensitivity to air significantly hinder their practical applications. Herein, we have devised an effective strategy to overcome these challenging shortcomings through modification of chalcogen chemistry under the guidance of theoretical modeling. The resultant Li6.25PS4O1.25Cl0.75 delivered excellent electrochemical compatibility with both pure Li anode and high-voltage LiCoO2 cathode, without detrimental impact upon the superb ionic conductivity of the pristine sulfide. Furthermore, the current SSE also exhibited highly improved stability to oxygen and moisture in air, with further advantage being more insulating to electrons. The remarkably enhanced compatibility with electrodes is attributed to in situ formation of solid anode electrolyte interphase (AEI) and cathode electrolyte interphase (CEI) layers. The formation of in situ AEI enabled ultra-stable Li plating/stripping at a record high current density up to 1 mAh cm -2 in Li|Li6.25PS4O1.25Cl0.75|Li symmetric cells over 1800 hours. The in situ CEI facilitated protection of the SSE from decomposition at elevated voltage. Consequently, the synergistic effect of AEI and CEI helped the LiCoO2|Li6.25PS4O1.25Cl0.75|Li battery cell to achieve markedly better cycling stability than that using the pristine Li6PS5Cl as SSE, at a high areal loading of the active cathode material (4 mg cm -2 ). This work adds a desirable SSE in the argyrodite sulfide family, so that highperformance solid battery cells could even be fabricated in ambient air.