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sitions between 2D semiconductors and probe molecules. Electron transition probability during the charge-transfer process can be expressed by Fermi's golden ruleThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202103442.

Aqueous zinc (Zn)‐ion batteries (ZIBs) have been considered as the most promising candidate for large‐scale energy storage system. However, the severe and uncontrollable dendrite growth of Zn anodes hinders the practical application. Herein, an ultraconformal horizontal Zn deposition is achieved, which is profiting from the epitaxial interface (InGaZn6O9) formed via spontaneously alloying between liquid Ga–In alloy (EGaIn) and Zn. The exposed (0016) plane of InGaZn6O9 matches well with (002) plane of Zn, inducing horizontal and dense Zn deposition. The resultant anode endows with prolonged cycling stability, and the full battery paired with MnO2 exhibits a stable lifespan over 4400 cycles at 5 A g−1. Meanwhile, the self‐formed ultraconformal interface realizes 360° no dead angle protection of anode, which is promising in flexible electronics. And there is no obvious capacity recession of the pouch cell even after bending 180°, demonstrating impressive flexibility. More importantly, the interface can be simply fabricated over a large area, displaying the large‐scale viability. The tailored approach delivers a constructive guideline for dendrite‐free Zn anode, showing great potential in the industrial production.

sources into fuels and value-added chemicals. [1−3] However, non-ideal catalytic activity primarily caused by the sluggish kinetics has long posed a crucial challenge in restricting the efficiency of electrocatalytic reactions. [4,5] Based on this, enormous research is devoted to enhancing the intrinsic activity of pre-existing active sites. For example, facet control can selectively expose the high-energy facets of catalysts to promote the adsorption of electrolytes, providing higher catalytic performance. [6] However, catalysts with high-energy facets are generally thermodynamic unstable and their preparations remain greatly challenging. Strain regulation can adjust the local coordination environment of active sites, [7] but its application is restricted by the stability of the modified structure with huge strain. Additionally, alloying with metals/nonmetals is also an effective strategy to decrease the reaction barrier for electrocatalytic reactions, [8] while the thermodynamic miscibility among the different elements is a necessary prerequisite. [9] In essence, the reaction kinetics is effectively triggered to promote the catalytic performance by these design approaches, which is ascribed to appropriate electronic structures. [10,11] Nevertheless, as for the existing catalytic materials, a rational design to tailor the optimal electronic structures is currently lacking, which is highly desired.Here, we propose a design principle, namely "dual self-built gating" to greatly boost the hydrogen evolution reaction (HER) performance of catalysts. Taking ReS 2 and WS 2 as an example, the dual self-built gating originated from in-plane ReS 2 -WS 2 covalent bonds and out-plane ReS 2 /WS 2 interlayer interaction induces electrons to directionally transfer from WS 2 to ReS 2 , [12,13] resulting in charge redistribution at the interface. In this case, owing to the tailored electronic structures, dual selfbuilt gating can balance the adsorption of intermediates and the desorption of hydrogen synergistically, leading to a dramatic improvement in reaction kinetics. As demonstrated by density functional theory (DFT) calculations, the dual gating region shows a Gibbs free energy close to zero (0.03 eV), suggesting that the charge redistribution at the interface enhances the intrinsic activity of active sites. More interestingly, on account of the adjustable carrier density, we also confirm the Optimizing the intrinsic activity of active sites is an appealing strategy for accelerating the kinetics of the catalytic process. Here, a design principle, namely "dual self-built gating", is proposed to tailor the electronic structures of catalysts. Catalytic improvement is confirmed in a model catalyst with a ReS 2 -WS 2 /WS 2 hybridized heterostructure. As demonstrated in experimental and theoretical results, the dual gating can bidirectionally guide electron transfer and redistribute at the interface, endowing the model catalyst with an electron-rich region. The tailored electronic structures balance the adsorption of intermediate...

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The integration of two-dimensional van der Waals (vdW) heterostructures breaks through the constraints of lattice matching and symmetry, offering substantial opportunities in the development of advanced materials. After the width is reduced, one-dimensional vdW heterostructures show rich band structures and strong spin–orbit coupling behaviors, widening the applications in optoelectronics and spintronics. However, the synthesis of one-dimensional vdW heterostructure nanoribbons has rarely been reported yet. Herein, we report a general approach to realizing transition metal dichalcogenide (TMD) heterostructure nanoribbons for the first time by unzipping self-assembled TMD heterostructure nanoscrolls. As demonstrated by MoS2/WS2 nanoribbons, the obtained TMD heterostructure nanoribbons with alternating stacked layers possess flat edge structures and high quality. Meanwhile, this strategy can be extended to create diverse vdW TMD nanoribbons, demonstrating its versatility. Our work thus shows great potential to prepare TMD heterostructure nanoribbons with various compositions and stacking modes, and new structures can be customized with targeted properties.