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Electrochemical transformation processes involving carbon, hydrogen, oxygen, nitrogen, and small-molecule chemistries represent a promising means to store renewable energy sources in the form of chemical energy. However, their widespread deployment is hindered by a lack of efficient, selective, durable, and affordable electrocatalysts. Recently, grain boundary (GB) engineering as one category of defect engineering, has emerged as a viable and powerful pathway to achieve improved electrocatalytic performances. This review presents a timely and comprehensive overview of recent advances in GB engineering for efficient electrocatalysis. The beneficial effects of introducing GBs into electrocatalysts are discussed, followed by an overview of the synthesis and characterization of GB-enriched electrocatalysts. Importantly, the latest developments in leveraging GB engineering for enhanced electrocatalysis are thoroughly examined, focusing on the electrochemical utilization cycles of carbon, hydrogen, oxygen, and nitrogen. Future research directions are proposed to further advance the understanding and application of GB engineering for improved electrocatalysis.

Autonomously self-healing, reversible, and soft adhesive microarchitectures and structured electric elements could be important features in stable and versatile bioelectronic devices adhere to complex surfaces of the human body (rough, dry, wet, and vulnerable). In this study, we propose an autonomous self-healing multi-layered adhesive patch inspired by the octopus, which possess self-healing and robust adhesion properties in dry/underwater conditions. To implement autonomously self-healing octopus-inspired architectures, a dynamic polymer reflow model based on structural and material design suggests criteria for three-dimensional patterning self-healing elastomers. In addition, self-healing multi-layered microstructures with different moduli endows efficient self-healing ability, human-friendly reversible bio-adhesion, and stable mechanical deformability. Through programmed molecular behavior of microlevel hybrid multiscale architectures, the bioinspired adhesive patch exhibited robust adhesion against rough skin surface under both dry and underwater conditions while enabling autonomous adhesion restoring performance after damaged (over 95% healing efficiency under both conditions for 24 h at 30°C). Finally, we developed a self-healing skin-mountable adhesive electronics with repeated attachment and minimal skin irritation by laminating thin gold electrodes on octopus-like structures. Based on the robust adhesion and intimate contact with skin, we successfully obtained reliable measurements during dynamic motion under dry, wet, and damaged conditions.

Photothermoelectric (PTE) detectors combine photothermal and thermoelectric conversion, surmounting material band gap restrictions and limitations related to matching light wavelengths, have been widely used in telecommunication band detection. Two-dimensional (2D) materials with gate-tunable Seebeck coefficient can induce the generation of photothermal currents under illumination by the asymmetric Seebeck coefficient, making them promising candidate for PTE detectors in the telecommunication band. In this work, we report that a newly explored van der Waals (vdW) layered material, SnP₂Se₆, possessing excellent field regulation capabilities and behaviors as an ideal candidate for PTE detector implementation. With the assistance of temperature-dependent Raman characterization, the suspended atomic thin SnP₂Se₆ nanosheets reveal thickness-dependent thermal conductivity of 1.4–5.7 W m⁻¹ K⁻¹ at room temperature. The 2D SnP₂Se₆ demonstrates high Seebeck coefficient (S) and power factor (PF), which are estimated to be −506 μV K⁻¹ and 207 μW m⁻¹ K⁻², respectively. By effectively modulating the SnP₂Se₆ localized carrier concentration, which in turn leads to inhomogeneous Seebeck coefficients, the designed dual-gate PTE detector with 2D SnP₂Se₆ channel demonstrates wide spectral photoresponse in telecommunication bands, yielding high responsivity (R = 1.2 mA W⁻¹) and detectivity (D* = 6 × 10⁹ Jones) under 1550 nm light illumination. Our findings provide a new material platform and device configuration for the telecommunication band detection.

Low-dimensional metal halide perovskites exhibit exceptional photoelectronic properties and intrinsic stability, positioning them as a promising class of semiconductor materials for light-emitting devices and photodetectors. In this work, we present a millimeter-scale single crystal of mixed low-dimensional (one-dimensional–zero-dimensional [1D–0D]) organic lead iodide with well-defined crystallinity. The fabricated single-crystal devices demonstrate high-sensitivity photoresponse and x-ray detection performance. By spatially isolating organic molecules to form the mixed 1D–0D crystal structure, ion migrations is effectively suppressed, resulting in a remarkable three orders of magnitude reduction in the dark current (56.4 pA @200 V) of the single-crystal devices. Furthermore, by enhancing the background characteristics, we achieved an impressive low x-ray detection limit of 154.5 nGys⁻¹ in the single-crystal device. These findings highlight that the mixed 1D–0D organic lead iodide configuration efficiently controls ion migration within the crystal structure, offering a promising avenue for realizing high-performance perovskite-based photodetectors and x-ray detectors.

High-temperature stable transparent conductive oxides (TCOs) are highly desirable in optoelectronics but are rarely achieved due to the defect generation that is inevitable during high-temperature air annealing. This work reports unprecedented stability in aluminum and fluorine co-doped ZnO (AFZO) films prepared by pulse laser deposition. The AFZO can retain a mobility of 60 cm² V⁻¹ s⁻¹, an electron concentration of 4.5 × 10²⁰ cm⁻³, and a visible transmittance of 91% after air-annealing at 600°C. Comprehensive defect characterization and first principles calculations have revealed that the offset of substitutional aluminum by zinc vacancy is responsible for the instability observed in aluminum-doped ZnO, and the pairing between fluorine substitution and zinc vacancy ensures the high-temperature stability of AFZO. The utility of AFZO in enabling the epitaxial growth of (Al_xGa_1−x)₂O₃ film within a high-temperature, oxygen-rich environment is demonstrated, facilitating the development of a self-powered solar-blind ultraviolet Schottky photodiode. Furthermore, the high-mobility AFZO transparent electrode enables perovskite solar cells to achieve improved power conversion efficiency by balancing the electron concentration-dependent conductivity and transmittance. These findings settle the long-standing controversy surrounding the instability in TCOs and open up exciting prospects for the advancement of optoelectronics.

Local phase transition in transition metal dichalcogenides (TMDCs) by lithium intercalation enables the fabrication of high-quality contact interfaces in two-dimensional (2D) electronic devices. However, controlling the intercalation of lithium is hitherto challenging in vertically stacked van der Waals heterostructures (vdWHs) due to the random diffusion of lithium ions in the hetero-interface, which hinders their application for contact engineering of 2D vdWHs devices. Herein, a strategy to restrict the lithium intercalation pathway in vdWHs is developed by using surface-permeation assisted intercalation while sealing all edges, based on which a high-performance edge-contact MoS₂ vdWHs floating-gate transistor is demonstrated. Our method avoids intercalation from edges that are prone to be random but intentionally promotes lithium intercalation from the top surface. The derived MoS₂ floating-gate transistor exhibits improved interface quality and significantly reduced subthreshold swing (SS) from >600 to 100 mV dec^–1. In addition, ultrafast program/erase performance together with well-distinguished 32 memory states are demonstrated, making it a promising candidate for low-power artificial synapses. The study on controlling the lithium intercalation pathways in 2D vdWHs offers a viable route toward high-performance 2D electronics for memory and neuromorphic computing purposes.

The relentless pursuit of sustainable and safe energy storage technologies has driven a departure from conventional lithium-based batteries toward other relevant alternatives. Among these, aqueous batteries have emerged as a promising candidate due to their inherent properties of being cost-effective, safe, environmentally friendly, and scalable. However, traditional aqueous systems have faced limitations stemming from water's narrow electrochemical stability window (~1.23 V), severely constraining their energy density and viability in high-demand applications. Recent advancements in decoupling aqueous batteries offer a novel solution to overcome this challenge by separating the anolyte and catholyte, thereby expanding the theoretical operational voltage window to over 3 V. One key component of this innovative system is the ion-selective membrane (ISM), acting as a barrier to prevent undesired crossover between electrolytes. This review provides a comprehensive overview of recent advancements in decoupling aqueous batteries, emphasizing the application of various types of ISMs. Moreover, we summarize different specially designed ISMs and their performance attributes. By addressing the current challenges ISMs face, the review outlines potential pathways for future enhancement and development of aqueous decoupling batteries.

Due to the built-in electric field induced by spontaneous polarization in hybrid perovskite (HP) ferroelectrics, the devices based on them exhibit excellent performance in self-powered photodetection. However, most of the self-powered photodetector are made of lead-based HP ferroelectrics and have a relatively narrow photoresponse waveband. Although lead-free HPs solve the problem of lead toxicity, their optoelectronic performance is inferior to that of lead-based HPs and photoresponse waveband is limited by its optical band gap, which hinders their further application. To solve this problem, herein, a lead-free HP ferroelectric (HDA)BiI₅ (HDA is hexane-1,6-diammonium) with large spontaneous polarization shows an enhanced photocurrent and achieves x-ray-ultraviolet–visible-near-infrared (x-ray-UV–Vis–NIR) photoresponse through the ferro-pyro-phototronic (FPP) effect. The ferroelectric, pyroelectric, and photovoltaic characteristics coupled together in a single-phase (HDA)BiI₅ ferroelectric is an effective way to improve the performance of the devices. What is particularly attractive is that the FPP effect not only improves the optoelectronic performance of (HDA)BiI₅, but also achieves broadband photoresponses beyond its optical absorption range. Especially, the current boosting with an exceptional contrast of ~1100% and 2400% under 520 and 637 nm, respectively, which is associated with FPP effect. Meanwhile, single crystal self-powered photodetector based on (HDA)BiI₅ also exhibit significant FPP effects even under high-energy x-ray, which owns an outstanding sensitivity of 170.7 μC Gy⁻¹ cm⁻² and a lower detection limit of 266 nGy s⁻¹ at 0 V bias. Therefore, it is of great significance to study the coupling of multiple physical effects and improve device performance based on lead-free HP ferroelectrics.

Crystallization speed of phase change material is one of the main obstacles for the application of phase change memory (PCM) as storage class memory in computing systems, which requires the combination of nonvolatility with ultra-fast operation speed in nanoseconds. Here, we propose a novel approach to speed up crystallization process of the only commercial phase change chalcogenide Ge₂Sb₂Te₅ (GST). By employing TiO₂ as the dielectric layer in phase change device, operation speed of 650 ps has been achieved, which is the fastest among existing representative PCM, and is comparable to the programing speed of commercial dynamic random access memory (DRAM). Because of its octahedral atomic configuration, TiO₂ can provide nucleation interfaces for GST, thus facilitating the crystal growth at the determinate interface area. Ti–O–Ti–O four-fold rings on the (110) plane of tetragonal TiO₂ is critical for the fast-atomic rearrangement in the amorphous matrix of GST that enables ultra-fast operation speed. The significant improvement of operation speed in PCM through incorporating standard dielectric material TiO₂ in DRAM paves the way for the application of phase change memory in high performance cache-type data storage.

Flexible perovskite photodetectors (FPDs) are promising for novel wearable devices in bionics, robotics and health care. However, their performance degradation and instability during operations remain a grand challenge. Superior flexibility and spontaneous functional repair of devices without the need for any external drive or intervention are ideal goals for FPDs. Herein, by using phenyl disulfide instead of alkyl disulfide as a crosslinking agent, disulfide bonds with lower bond energy are introduced, thus endowing the polyurethane network (SCPU) with the ability of self-healing at room temperature. SCPU is filled to the grain boundary of perovskite film, which not only improves the crystal quality of perovskite and mechanical stability of FPD but also enables FPD to self-heal at room temperature. As a result, the as-prepared FPD exhibits a superior responsivity of 0.4 A W⁻¹, a high specific detectivity of 2.5 × 10¹¹ Jones and 2 μs fast response time in a self-powered mode. More importantly, the FPD still retained 91% of the initial photo responsivity after 9000 times of bending upon cyclic healing. This polymer doping strategy provides an effective solution for stable operation and room-temperature self-healing for FPDs.