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Abstract Molecular detection is important in biosensing, food safety, and environmental surveillance. The high biocompatibility, superior mechanical stability, and low cost make plasmon-free surface-enhanced Raman scattering (SERS) a promising sensing technique, the ultrahigh sensitivity of which is urgently pursued for realistic applications. As a proof of concept, we report a mechanochemical strategy, which combines the wrinkling and chemical functionalization, to fabricate a plasmon-free SERS platform based on 2D MnPS3 with a sub-attomolar detection limit. In detail, the formation of wrinkles in 2D MnPS3 enables a SERS substrate of the material to detect trace methylene blue molecules. The mechanism is experimentally revealed that the wrinkled structures contribute to the improvement of light-matter coupling. On this basis, decorating a wrinkled MnPS3 which has absorbed methylene blue with histamine dihydrochloride further lowers the detection limit to 10−19 M. Because the amino groups in histamine dihydrochloride molecules are crosslinkers that create more pathways to promote charge transfer between these substances. This work provides a guidance for the design of SERS sensors with single-molecule-level sensitivity.

Abstract The swift progress in wearable technology has accentuated the need for flexible power systems. Such systems are anticipated to exhibit high efficiency, robust durability, consistent power output, and the potential for effortless integration. Integrating ultraflexible energy harvesters and energy storage devices to form an autonomous, efficient, and mechanically compliant power system remains a significant challenge. In this work, we report a 90 µm-thick energy harvesting and storage system (FEHSS) consisting of high-performance organic photovoltaics and zinc-ion batteries within an ultraflexible configuration. With a power conversion efficiency surpassing 16%, power output exceeding 10 mW cm–2, and an energy density beyond 5.82 mWh cm–2, the FEHSS can be tailored to meet the power demands of wearable sensors and gadgets. Without cumbersome and rigid components, FEHSS shows immense potential as a versatile power source to advance wearable electronics and contribute toward a sustainable future.

Abstract In the last decade, laboratory-scale single-junction perovskite solar cells have achieved a remarkable power conversion efficiency exceeding 26.1%. However, the transition to industrial-scale production has unveiled a significant efficiency gap. The central challenge lies in the difficulty of achieving uniform, high-quality perovskite films on a large scale. To tackle this issue, various innovative strategies for manipulating crystallization have emerged in recent years. Based on an in-depth fundamental understanding of the nucleation and growth mechanisms in large-area perovskite films prepared through blade/slot-die coating methods, this review offers a critical examination of crystallization manipulation strategies for large-area perovskite solar modules. Lastly, we explore future avenues aimed at enhancing the efficiency and stability of large-area PSMs, thereby steering the field toward commercially viable applications.

Abstract Two-dimensional semiconductors with high thermal conductivity and charge carrier mobility are of great importance for next-generation electronic and optoelectronic devices. However, constrained by the long-held Slack’s criteria, the reported two-dimensional semiconductors such as monolayers of MoS2, WS2, MoSe2, WSe2 and black phosphorus suffer from much lower thermal conductivity than silicon (~142 W·m–1·K–1) because of the complex crystal structure, large average atomic mass and relatively weak chemical bonds. Despite the more complex crystal structure, the recently emerging monolayer MoSi2N4 semiconductor has been predicted to have high thermal conductivity and charge carrier mobility simultaneously. In this work, using a noncontact optothermal Raman technique, we experimentally measure a high thermal conductivity of ~173 W·m–1·K–1 at room temperature for suspended monolayer MoSi2N4 grown by chemical vapor deposition. First-principles calculations reveal that such unusually high thermal conductivity benefits from the high Debye temperature and small Grüneisen parameter of MoSi2N4, both of which are strongly dependent on the high Young’s modulus induced by the outmost Si-N bilayers. Our study not only establishes monolayer MoSi2N4 as a benchmark 2D semiconductor for next-generation electronic and optoelectronic devices, but also provides an insight into the design of 2D materials for efficient heat conduction.

Abstract Sustainable battery recycling is essential for achieving resource conservation and alleviating environmental issues. Many open/closed-loop strategies for critical metal recycling or direct recovery aim at a single component, and the reuse of mixed cathode materials is a significant challenge. To address this barrier, here we propose an upcycling strategy for spent LiFePO4 and Mn-rich cathodes by structural design and transition metal replacement, for which uses a green deep eutectic solvent to regenerate a high-voltage polyanionic cathode material. This process ensures the complete recycling of all the elements in mixed cathodes and the deep eutectic solvent can be reused. The regenerated LiFe0.5Mn0.5PO4 has an increased mean voltage (3.68 V versus Li/Li+) and energy density (559 Wh kg–1) compared with a commercial LiFePO4 (3.38 V and 524 Wh kg–1). The proposed upcycling strategy can expand at a gram-grade scale and was also applicable for LiFe0.5Mn0.5PO4 recovery, thus achieving a closed-loop recycling between the mixed spent cathodes and the next generation cathode materials. Techno-economic analysis shows that this strategy has potentially high environmental and economic benefits, while providing a sustainable approach for the value-added utilization of waste battery materials.

Abstract Two-dimensional materials with ultrahigh in-plane thermal conductivity are ideal for heat spreader applications but cause significant thermal contact resistance in complex interfaces, limiting their use as thermal interface materials. In this study, we present an interfacial phonon bridge strategy to reduce the thermal contact resistance of boron nitride nanosheets-based composites. By using a low-molecular-weight polymer, we are able to manipulate the alignment of boron nitride nanosheets through sequential stacking and cutting, ultimately achieving flexible thin films with a layer of arc-like structure superimposed on perpendicularly aligned ones. Our results suggest that arc-like structure can act as a phonon bridge to lower the contact resistance by 70% through reducing phonon back-reflection and enhancing phonon coupling efficiency at the boundary. The resulting composites exhibit ultralow thermal contact resistance of 0.059 in2 KW−1, demonstrating effective cooling of fast-charging batteries at a thickness 2-5 times thinner than commercial products.

Abstract Bifacial perovskite solar cells have shown great promise for increasing power output by capturing light from both sides. However, the suboptimal optical transmittance of back metal electrodes together with the complex fabrication process associated with front transparent conducting oxides have hindered the development of efficient bifacial PSCs. Here, we present a novel approach for bifacial perovskite devices using single-walled carbon nanotubes as both front and back electrodes. single-walled carbon nanotubes offer high transparency, conductivity, and stability, enabling bifacial PSCs with a bifaciality factor of over 98% and a power generation density of over 36%. We also fabricate flexible, all-carbon-electrode-based devices with a high power-per-weight value of 73.75 W g−1 and excellent mechanical durability. Furthermore, we show that our bifacial devices have a much lower material cost than conventional monofacial PSCs. Our work demonstrates the potential of SWCNT electrodes for efficient, stable, and low-cost bifacial perovskite photovoltaics.

Abstract Developing highly efficient catalysts is significant for Li-CO2 batteries. However, understanding the exact structure of catalysts during battery operation remains a challenge, which hampers knowledge-driven optimization. Here we use X-ray absorption spectroscopy to probe the reconstruction of CoSx (x = 8/9, 1.097, and 2) pre-catalysts and identify the local geometric ligand environment of cobalt during cycling in the Li-CO2 batteries. We find that different oxidized states after reconstruction are decisive to battery performance. Specifically, complete oxidation on CoS1.097 and Co9S8 leads to electrochemical performance deterioration, while oxidation on CoS2 terminates with Co-S4-O2 motifs, leading to improved activity. Density functional theory calculations show that partial oxidation contributes to charge redistributions on cobalt and thus facilitates the catalytic ability. Together, the spectroscopic and electrochemical results provide valuable insight into the structural evolution during cycling and the structure-activity relationship in the electrocatalyst study of Li-CO2 batteries.

Abstract Adding extra raw materials for direct recycling or upcycling is prospective for battery recycling, but overlooks subtracting specific components beforehand can facilitate the recycling to a self-sufficient mode of sustainable production. Here, a subtractive transformation strategy of degraded LiNi0.5Co0.2Mn0.3O2 and LiMn2O4 to a 5 V-class disordered spinel LiNi0.5Mn1.5O4-like cathode material is proposed. Equal amounts of Co and Ni from degraded materials are selectively extracted, and the remaining transition metals are directly converted into Ni0.4Co0.1Mn1.5(CO3)2 precursor for preparing cathode material with in-situ Co doping. The cathode material with improved conductivity and bond strength delivers high-rate (10 C and 20 C) and high-temperature (60 °C) cycling stability. This strategy with no extra precursor input can be generalized to practical degraded black mass and reduces the dependence of current cathode production on rare elements, showing the potential of upcycling from the spent to a next-generation 5 V-class cathode material for the sustainable Li-ion battery industry.

Abstract The practical applications of solar-driven water splitting pivot on significant advances that enable scalable production of robust photoactive films. Here, we propose a proof-of-concept for fabricating robust photoactive films by a particle-implanting technique (PiP) which embeds semiconductor photoabsorbers in the liquid metal. The strong semiconductor/metal interaction enables resulting films efficient collection of photogenerated charges and superior photoactivity. A photoanode of liquid-metal embraced BiVO4 can stably operate over 120 h and retain ~ 70% of activity when scaled from 1 to 64 cm2. Furthermore, a Z-scheme photocatalyst film of liquid-metal embraced BiVO4 and Rh-doped SrTiO3 particles can drive overall water splitting under visible light, delivering an activity 2.9 times higher than that of the control film with gold support and a 110 h stability. These results demonstrate the advantages of the PiP technique in constructing robust and efficient photoactive films for artificial photosynthesis.

Abstract Although zinc‒air batteries (ZABs) are regarded as one of the most prospective energy storage devices, their practical application has been restricted by poor air electrode performance. Herein, we developed a free‐standing air electrode that is fabricated on the basis of a multifunctional three‐dimensional interconnected graphene network. Specifically, a three‐dimensional interconnected graphene network with fast mass and electron transport ability, prepared by catalyzing growth of graphene foam on nickel foam and then filling reduced graphene oxide into the pores of graphene foam, is used to anchor iron phthalocyanine molecules with atomic Fe‒N4 sites for boosting the oxygen reduction during discharging and nanosized FeNi hydroxides for accelerating the oxygen evolution during charging. As a result, the obtained air electrode exhibited an ultra‐small electrocatalytic overpotential of 0.603 V for oxygen reactions, a high peak power density of 220.2 mW cm‒2, and a small and stable charge‒discharge voltage gap of 0.70 V at 10 mA cm‒2 after 1136 cycles. Furthermore, in situ Raman spectroscopy together with theoretical calculations confirmed that phase transformation of FeNi hydroxides takes place from α‐Ni(OH)x to β‐Ni(OH)x to γ‐Ni(3+δ)+OOH for the oxygen evolution reaction and Ni is the active center while Fe enhances the activity of Ni active sites.

Abstract Advancing fast‐charging technology is an important strategy for the development of alkali metal ion batteries (AMIBs). The exploitation of a new generation of anode material system with high‐rate performance, high capacity, and low risk of lithium/sodium/potassium plating is critical to realize fast‐charging capability of AMIBs while maintaining high energy density and safety. Among them, phosphorus‐based anodes including phosphorus anodes and metal phosphide anodes have attracted wide attention, due to their high theoretical capacities, safe reaction voltages, and natural abundance. In this review, we summarize the research progress of different phosphorus‐based anodes for fast‐charging AMIBs, including material properties, mechanisms for storing alkali metal ions, key challenges and solution strategies for achieving fast‐charging capability. Moreover, the future development directions of phosphorus‐based anodes in fast‐charging AMIBs are highlighted.

Abstract Bi3TiNbO9, a layered ferroelectric photocatalyst, exhibits great potential for overall water splitting through efficient intralayer separation of photogenerated carriers motivated by a depolarization field along the in-plane a-axis. However, the poor interlayer transport of carriers along the out-of-plane c-axis, caused by the significant potential barrier between layers, leads to a high probability of carrier recombination and consequently results in low photocatalytic activity. Here, we have developed an efficient photocatalyst consisting of Bi3TiNbO9 nanosheets with a gradient tungsten (W) doping along the c-axis. This results in the generation of an additional electric field along the c-axis and simultaneously enhances the magnitude of depolarization field within the layers along the a-axis due to strengthened structural distortion. The combination of the built-in field along the c-axis and polarization along the a-axis can effectively facilitate the anisotropic migration of photogenerated electrons and holes to the basal {001} surface and lateral {110} surface of the nanosheets, respectively, enabling desirable spatial separation of carriers. Hence, the W-doped Bi3TiNbO9 ferroelectric photocatalyst with Rh/Cr2O3 cocatalyst achieves an efficient and durable overall water splitting feature, thereby providing an effective pathway for designing excellent layered ferroelectric photocatalysts.

Abstract Low-dimensional materials exhibit unique quantum confinement effects and morphologies as a result of their nanoscale size in one or more dimensions, making them exhibit distinctive physical properties compared to bulk counterparts. Among all low-dimensional materials, due to their atomic level thickness, two-dimensional materials possess extremely large shape anisotropy and consequently are speculated to have large optically anisotropic absorption. In this work, we demonstrate an optoelectronic device based on the combination of two-dimensional material and carbon dot with wide bandgap. High-efficient luminescence of carbon dot and extremely large shape anisotropy (>1500) of two-dimensional material with the wide bandgap of >4 eV cooperatively endow the optoelectronic device with multi-functions of optically anisotropic blue-light emission, visible light modulation, wavelength-dependent ultraviolet-light detection as well as blue fluorescent film assemble. This research opens new avenues for constructing multi-function-integrated optoelectronic devices via the combination of nanomaterials with different dimensions.

Abstract Hydrogen production coupled with biomass upgrading is vital for future sustainable energy developments. However, most biomass electrooxidation reactions suffer from high working voltage and low current density, which substantially hinder large-scale industrial applications. Herein, we report an acidic hydrogen production system that combined anodic ascorbic acid electrooxidation with cathodic hydrogen evolution. Unlike C-H and O-H bonds cleavage with slow kinetics in conventional organic oxidation, the highly active enol structure in ascorbic acid allows for an ultralow overpotential of only 12 mV@10 mA/cm2 using Fe single-atom catalysts, and reaches 1 A/cm2 at only 0.75 V (versus reversible hydrogen electrode) with approximately 100% Faraday efficiency for hydrogen production. Furthermore, the fabricated two-electrode membrane-free electrolyser delivers an industrial current density of 2 A/cm2@1.1 V at 60 °C (2.63 kWh/Nm3 H2), which requires half of the electricity consumption in conventional water electrolysis (~5 kWh/Nm3 H2). This work provides a new avenue for achieving industrial-scale hydrogen production from biomass.

Abstract Recycling cathode materials from spent lithium‐ion batteries (LIBs) is critical to a sustainable society as it will relief valuable but scarce recourse crises and reduce environment burdens simultaneously. Different from conventional hydrometallurgical and pyrometallurgical recycling methods, direct regeneration relies on non‐destructive cathode‐to‐cathode mode, and therefore, more time and energy‐saving along with an increased economic return and reduced CO2 footprint. This review retrospects the history of direct regeneration and discusses state‐of‐the‐art development. The reported methods, including high‐temperature solid‐state, hydrothermal/ionothermal, molten salt thermochemistry, and electrochemical method, are comparatively introduced, targeting at illustrating their underlying regeneration mechanism and applicability. Further, representative repairing and upcycling studies on wide‐applied cathodes, including LiCoO2 (LCO), ternary oxides, LiFePO4 (LFP), and LiMn2O4 (LMO), are presented, with an emphasis on milestone cases. Despite these achievements, there remain several critical issues that shall be addressed before the commercialization of the mentioned direct regeneration methods.

Abstract Direct seawater electrolysis is promising for sustainable hydrogen gas (H2) production. However, the chloride ions in seawater lead to side reactions and corrosion, which result in a low efficiency and poor stability of the electrocatalyst and hinder the use of seawater electrolysis technology. Here we report a corrosion-resistant RuMoNi electrocatalyst, in which the in situ-formed molybdate ions on its surface repel chloride ions. The electrocatalyst works stably for over 3000 h at a high current density of 500 mA cm−2 in alkaline seawater electrolytes. Using the RuMoNi catalyst in an anion exchange membrane electrolyzer, we report an energy conversion efficiency of 77.9% and a current density of 1000 mA cm−2 at 1.72 V. The calculated price per gallon of gasoline equivalent (GGE) of the H2 produced is $ 0.85, which is lower than the 2026 technical target of $ 2.0/GGE set by the United Stated Department of Energy, thus, suggesting practicability of the technology.

Abstract Developing efficient noble-metal-free surface-enhanced Raman scattering (SERS) substrates and unveiling the underlying mechanism is crucial for ultrasensitive molecular sensing. Herein, we report a facile synthesis of mixed-dimensional heterostructures via oxygen plasma treatments of two-dimensional (2D) materials. As a proof-of-concept, 1D/2D WO3-x /WSe2 heterostructures with good controllability and reproducibility are synthesized, in which 1D WO3-x nanowire patterns are laterally arranged along the three-fold symmetric directions of 2D WSe2. The WO3-x/WSe2 heterostructures exhibited high molecular sensitivity, with a limit of detection of 5 × 10−18 M and an enhancement factor of 5.0 × 1011 for methylene blue molecules, even in mixed solutions. We associate the ultrasensitive performance to the efficient charge transfer induced by the unique structures of 1D WO3-x nanowires and the effective interlayer coupling of the heterostructures. We observed a charge transfer timescale of around 1.0 picosecond via ultrafast transient spectroscopy. Our work provides an alternative strategy for the synthesis of 1D nanostructures from 2D materials and offers insights on the role of ultrafast charge transfer mechanisms in plasmon-free SERS-based molecular sensing.

Abstract The asymmetrical growth of a single‐wall carbon nanotube (SWCNT) by introducing a change of a local atomic structure, is usually inevitable and supposed to have a profound effect on the chirality control and property tailor. However, the breaking of the symmetry during SWCNT growth remains unexplored and its origins at the atomic‐scale are elusive. Here, environmental transmission electron microscopy is used to capture the process of breaking the symmetry of a growing SWCNT from a sub‐2‐nm platinum catalyst nanoparticle in real‐time, demonstrating that topological defects formed on the side of a SWCNT can serve as a buffer for stress release and inherently break its axis‐symmetrical growth. Atomic‐level details reveal the importance of the tube‐catalyst interface and how the atom rearrangement of the solid‐state platinum catalyst around the interface influences the final tubular structure. The active sites responsible for trapping carbon dimers and providing enough driving force for carbon incorporation and asymmetric growth are shown to be low‐coordination step edges, as confirmed by theoretical simulations.

Abstract In the fast‐evolving landscape of decentralized and personalized healthcare, the need for multimodal biosensing systems that integrate seamlessly with the human body is growing rapidly. This presents a significant challenge in devising ultraflexible configurations that can accommodate multiple sensors and designing high‐performance sensing components that remain stable over long periods. To overcome these challenges, ultraflexible organic photodetectors (OPDs) that exhibit exceptional performance under near‐infrared illumination while maintaining long‐term stability are developed. These ultraflexible OPDs demonstrate a photoresponsivity of 0.53 A W−1 under 940 nm, shot‐noise‐limited specific detectivity of 3.4 × 1013 Jones, and cut‐off response frequency beyond 1 MHz at −3 dB. As a result, the flexible photoplethysmography sensor boasts a high signal‐to‐noise ratio and stable peak‐to‐peak amplitude under hypoxic and hypoperfusion conditions, outperforming commercial finger pulse oximeters. This ensures precise extraction of blood oxygen saturation in dynamic working conditions. Ultraflexible OPDs are further integrated with conductive polymer electrodes on an ultrathin hydrogel substrate, allowing for direct interface with soft and dynamic skin. This skin‐integrated sensing platform provides accurate measurement of photoelectric and biopotential signals in a time‐synchronized manner, reproducing the functionality of conventional technologies without their inherent limitations.

Abstract For the process of photovoltaic conversion in organic solar cells (OSCs) and quantum‐dot solar cells (QDSCs), three of four steps are determined by exciton behavior, namely, exciton generation, exciton diffusion, and exciton dissociation. Therefore, it is of great importance to regulate exciton behavior in OSCs and QDSCs for achieving high power conversion efficiency. Due to the rapid development in materials and device fabrication, great progress has been made to manage the exciton behavior to achieve prolonged exciton diffusion length and improved exciton dissociation in recent years. In this review, we first introduce the parameters that affect exciton behavior, followed by the methods to measure exciton diffusion length. Then, we provide an overview of the recent advances with regard to exciton behavior investigation in OSCs and QDSCs, including exciton lifetime, exciton diffusion coefficient, and exciton dissociation. Finally, we propose future directions in deepening the understanding of exciton behavior and boosting the performance of OSCs and QDSCs.

Abstract The development of low-cost, high-activity, and durable integrated bifunctional flexible air electrodes for use in Zn-air batteries is both challenging and important. We report a simple and scalable electropolymerization method used to prepare an electrode material comprising heavily N-doped carbon covering single-walled carbon nanotube (N/C-SWCNT) networks. The resulting core/shell structure of the hybrid electrode enabled the flexibility, mechanics, and three-dimensional interconnected porous structure of SWCNT films while containing abundant pyridinic N, which provided excellent catalytic activity for both the oxygen reduction and evolution reactions (overpotential gap = 0.76 V). A binder-free Zn-air battery using the N/C-SWCNT film as an oxygen electrode was assembled and showed a high peak power density of 181 mW/cm2, a high specific capacity of 810 mAh/g and stable discharge‒charge cycling performance. We also constructed a flexible solid-state Zn-air battery featuring not only a high power density of 22 mW/cm2 but also good flexibility and stability.

Sustainable recycle of spent Li ion batteries is an effective strategy to alleviate environmental concerns and support resource conservation. Here, authors report the direct regeneration of LiFePO4 cathode using multifunctional organic lithium salts, leading to high environmental and economic benefits.

New birefringent element which can stably and continuously modulate DUV light by mechanical stimuli (compressing or stretching).

High extraction capacity with precise selectivity to trace amounts of gold over a wide range of co-existing elements remains a challenge for effective e-waste recycling. Here, authors demonstrate the excellent performance of rGO for gold extraction from e-waste leachate, even at minute concentrations.

Ambient-stable solution-processed conductive materials with a low work function are essential to facilitate electron injection. Here, the authors design and synthesise polymer electrolyte with work function down to 2.2 eV for applications in high-performance light-emitting diodes and solar cells.

Abstract The keen interest in fuel cells and metal‐air batteries stimulates a great deal of research on the development of a cost‐efficient and high‐performance catalyst as an alternative to traditional Pt to boost the sluggish oxygen reduction reaction (ORR) at the cathode. Herein, we report a facile and scalable strategy for the large‐scale preparation of a free‐standing and flexible porous atomically dispersed Fe–N‐doped carbon microtube (FeSAC/PCMT) sponge. Benefiting from its unique structure that greatly facilitates the catalytic kinetics, mass transport, and electron transfer, our FeSAC/PCMT electrode exhibits excellent performance with an ORR potential of 0.942 V at −3 mA cm−2. When the FeSAC/PCMT sponge was directly used as an oxygen electrode for liquid‐state and flexible solid‐state zinc‐air batteries, high peak power densities of 183.1 and 58.0 mW cm−2 were respectively achieved, better than its powdery counterpart and commercial Pt/C catalyst. Experimental and theoretical investigation results demonstrate that such ultrahigh ORR performance can be attributed to atomically dispersed Fe–N5 species in FeSAC/PCMT. This study presents a cost‐effective and scalable strategy for the fabrication of highly efficient and flexible oxygen electrodes, provides a significant new insight into the catalytic mechanisms, and helps to realize significant advances in energy devices.

Though transparent hydrogels with tunable optical anisotropy are attractive for soft robotics, wearable devices and optical applications, achieving large birefringence has been a challenge. Here, the authors report a transparent hydrogel with large, uniform and magnetically tunable birefringence.

Abstract The domains and domain boundaries in 2D materials are known to play essential roles in investigating intriguing physical properties and have potential applications in nanoscale devices. Understanding the influence of individual domains on the superconducting properties of ultrathin 2D superconductors is of crucial importance for fundamental studies on mesoscopic superconductivity as well as applications in superconducting nanoelectronics. Here, low‐temperature electronic transport measurements of high quality ultrathin Mo2C crystals are presented that show clear evidence for the presence of multiple superconducting phase induced by the nanoscale domain structures. In particular, the observation of an anomalous resistance peak in the vicinity of the onset of the superconducting transition is reported. This resistive anomaly is interpreted as a consequence of nonequilibrium charge imbalance near the domain boundaries, which could induce effective normal‐superconducting interfaces in 2D Mo2C crystals. Moreover, the magnetic field‐tuned superconductor‐metal transition for ultrathin Mo2C crystals is examined. The observed scaling behavior is consistent with the appearance of quantum Griffiths singularity in 2D superconducting systems. This study sheds light on the understanding of the domain boundaries and their role on the transport properties of highly crystalline 2D superconductors, which may open potential application of domain structure in functional superconducting nanodevices.

Layered materials with unique structures and symmetries have attracted tremendous interest for constructing 2-dimensional (2D) structures. The weak interlayer interaction renders them to be readily isolated into various ultrathin nanosheets with exotic properties and diverse applications. In order to enrich the library of 2D materials, extensive progress has been made in the field of ternary layered materials. Consequently, many brand-new materials are derived, which greatly extend the members of 2D realm. In this review, we emphasize the recent progress made in synthesis and exploration of ternary layered materials. We first classify them in terms of stoichiometric ratio and summarize their difference in interlayer interaction, which is of great importance to produce corresponding 2D materials. The compositional and structural characteristics of resultant 2D ternary materials are then discussed so as to realize desired structures and properties. As a new family of 2D materials, we overview the layer-dependent properties and related applications in the fields of electronics, optoelectronics, and energy storage and conversion. The review finally provides a perspective for this rapidly developing field.

Abstract Gradient heterostructure is one of fundamental interfaces and provides an effective platform to achieve gradually changed properties in mechanics, optics, and electronics. Among different types of heterostructures, the gradient one may provide multiple resistive states and immobilized conductive filaments, offering great prospect for fabricating memristors with both high neuromorphic computation capability and repeatability. Here, we invent a memristor based on a homologous gradient heterostructure (HGHS), comprising a conductive transition metal dichalcogenide and an insulating homologous metal oxide. Memristor made of Ta–TaSxOy–TaS2 HGHS exhibits continuous potentiation/depression behavior and repeatable forward/backward scanning in the read‐voltage range, which are dominated by multiple resistive states and immobilized conductive filaments in HGHS, respectively. Moreover, the continuous potentiation/depression behavior makes the memristor serve as a synapse, featuring broad‐frequency response (10−1–105 Hz, covering 106 frequency range) and multiple‐mode learning (enhanced, depressed, and random‐level modes) based on its natural and motivated forgetting behaviors. Such HGHS‐based memristor also shows good uniformity for 5 × 7 device arrays. Our work paves a way to achieve high‐performance integrated memristors for future artificial neuromorphic computation.

Water electrolysis is a promising hydrogen production technique but is restricted from large-scale application due to poor performance and high cost. Here, the authors report a mechanically stable monolith electrocatalyst that achieves superior hydrogen evolution at large current densities.

Semiconducting single-walled carbon nanotubes (s-SWCNTs) with large diameters are highly desired in the construction of high performance optoelectronic devices. However, it is difficult to selectively prepare large-diameter s-SWCNTs since their structure and chemical stability are quite similar with their metallic counterparts. In this work, we use SWCNTs with large diameter as a raw material, conjugated polymer of regioregular poly-(3-dodecylthiophene) (rr-P3DDT) with long side chain as a wrapping agent to selectively separate large-diameter s-SWCNTs. It is found that s-SWCNTs with a diameter of ~1.9 nm are effectively enriched, which shows a clean surface. By using the sorted s-SWCNTs as a channel material, we constructed thin-film transistors showing charge-carrier mobilities higher than 10 cm2 V−1 s−1 and on/off ratios higher than 103.

Here, the authors exploit a photo-induced barrier-lowering mechanism in MoS2/ α-MoO3-x heterojunctions to realize two-dimensional phototransistors with enhanced performance and fast response at low bias voltage.

Abstract The realization of high‐quality heterostructures or hybrids of graphene and superconductor is crucial for exploring various novel quantum phenomena and devices engineering. Here, the electronic transport on directly grown high‐quality graphene/Mo2C vertical heterostructures with clean and sharp interface is comprehensively investigated. Owing to the strong interface coupling, the graphene layer feels an effective confinement potential well imposed by two‐dimensional (2D) Mo2C crystal. Employing cross junction device geometry, a series of resonance‐like magnetoresistance peaks are observed at low temperatures. The temperature and gate voltage dependences of the observed resonance peaks give evidence for geometric resonance of electron cyclotron orbits with the formed potential well. Moreover, it is found that both the amplitude of resonance peaks and conductance fluctuation exhibit different temperature‐dependent behaviors below the superconducting transition temperature of 2D Mo2C, indicating the correlation of quantum fluctuations and superconductivity. This study offers a promising route toward integrating graphene with 2D superconducting materials, and establishes a new way to investigate the interplay of massless Dirac fermion and superconductivity based on graphene/2D superconductor vertical heterostructures.

Twisted phosphorene offers another attractive system to explore moiré physics. Here, the authors report emerging anisotropic moiré optical resonances in twisted monolayer/bilayer phosphorene, exhibiting strong twist dependence for angles as large as 19°.

The discovery of a new two-dimensional van der Waals layered MoSi2N4 material inspires many attentions. Here, the authors report intercalation strategies to explore a much wider range of MA2Z4 family and predict amount of materials accessible to experimental verifications with emergent topological, magnetic or Ising superconductivity properties.

To emulate nature biological processing, highly-integrated ultra-sensitive artificial neuromorphic system is highly desirable. Here, the authors report flexible sensor array of 1024 pixels using combination of carbon nanotubes and perovskite QDs as active matetials, achieving highly responsive device for reinforcement learning.

Abstract Deteriorating interfacial contact under mechanical deformation induces large cracks and high charge transfer resistance, resulting in a severe capacity fading of flexible lithium‐ion batteries (LIBs). Herein, an oxygen plasma treatment on a polymer separator combined with high‐speed centrifugal spraying to construct ultrastable interfacial contacts is reported. With the treatment, abundant hydrophilic oxygen‐containing functional groups are produced and ensure strong chemical adhesion between the separator and the active materials. With single walled carbon nanotubes (SWCNTs) sprayed onto the active materials, a dense thin film is formed as the current collector. Meanwhile, the centrifugal force caused by high‐speed rotation together with van der Waals forces under fast evaporation produces a much closer interface between the current collector and the active materials. As a result of this ultrastable interfacial interaction, the integrated electrode shows no structural failure after 5000 bending cycles with the charge‐transfer resistance as low as 35.8% and a Li‐ion diffusion coefficient nearly 19 times of the untreated electrode. Flexible LIBs assembled with these integrated electrodes show excellent structural and electrochemical stability, and can work steadily under various deformed states and repeated bending. This work provides a new technique toward rational design of electrode configuration for flexible LIBs.

The large-scale implementation of electrochemical technologies will require the high-throughput production of high-performance, inexpensive catalysts. Here, authors demonstrate earth abundant molybdenite as raw materials to produce efficient MoS2 catalysts for high current density H2 evolution.

Materials with tunable transmitted colours are sought after for a range of applications. The authors here present magnetic-field-controlled color tuning in a transparent suspension of 2D crystals with unusually large magneto-birefringence.

The abundance and low cost of potassium makes potassium batteries a promising technology for large scale energy storage. Here the authors apply a previously known frustrated magnet, KFeC2O4F, as the cathode in which the unique structure and Fe2+/Fe3+ redox enable excellent cycling stability.

Carbon nanotubes (CNTs) are considered a promising candidate for the detection of toxic gases because of their high specific surface area and excellent electrical and mechanical properties. However, the detecting performance of CNT-based detectors needs to be improved because covalently bonded CNTs are usually chemically inert. We prepared a nitrogen-doped single-wall CNT (SWCNT) film by means of gas-phase fluorination followed by thermal annealing in NH3. The doped nitrogen content could be changed in the range of 2.9–9.9 at%. The N-doped SWCNT films were directly used to construct flexible and transparent gas sensors, which can work at a low voltage of 0.01 V. It was found that their NO2 detection performance was closely related to their nitrogen content. With an optimum nitrogen content of 9.8 at%, a flexible sensor had a detection limit of 500 ppb at room temperature with good cycling ability and stability during bending.

With an aim to enhance the photocatalytic activity, Pt loaded TiO2–Al-MCM-41 catalysts with high surface area were synthesized by a multistep route. The waste of the rice processing, rice husk (RH), was used as the precursor for the extraction of silica. The diffuse reflectance and photoluminescence spectroscopy revealed the extension of the absorption edge in the visible region and exciton trapping nature of the dispersed platinum. The structural analysis was carried out by XRD, whereas X-ray photoelectron spectroscopy identified the chemical states of the components of the synthesized powders. The BET surface area measurements revealed the reduction in the surface area and pore volume with the increasing platinum loading. TEM micrographs showed the uniform distribution of TiO2 and Pt nanoparticles at the surface of Al-MCM-41. The photocatalytic efficiency of the synthesized powders as photocatalysts was obtained for the removal of 100 ppm CN− from aqueous solution in fluorescent blue light exposure. Compared to unsupported TiO2, the Pt-loaded catalysts exhibited substantially high activity for the removal of CN−. A plausible mechanism for the removal of cyanide ions was proposed. The catalysts showed excellent stability and reproducibility in the successive use. Keywords: Al-MCM-41, Rice Husk, Pt loading, TiO2 loaded Al-MCM-41, Cyanide

Nano-crystallization is essential to tune different properties of materials. Here, the authors report a synthesis strategy that involves quenching of a hot metal foil for few seconds in liquid carbon source to form graphene films of 3.6 nm grain size, showing mechanical strength of 101 GPa and semiconducting behaviour.

Polyoxyanion compounds are alternative cathodes to conventional oxides, but their reliance on the transition metal redox limits the performance. Here the authors report an oxalate system which possesses additional polyanionic redox reactivity, suggesting a new direction for cathode materials design.

Specific stacking sequence of graphene can enable observation of unusual properties however it has been difficult to obtain this over wider areas. Here, the authors report wafer-scale growth of 100% AB-stacked bilayer graphene films by CVD on liquid Pt3Si/solid Pt substrates showing high quality and improved mechanical properties comparable to the mechanically exfoliated flakes.

Hydrogen production from water provides one avenue toward harnessing renewable energy, although large-scale implementation remains a challenge. Here, authors explore roles of morphology and surface chemistry, and develop efficient catalysts for hydrogen evolution at high current densities.

Single-wall carbon nanotubes (SWCNTs) have a high aspect ratio, large surface area, good stability and unique metallic or semiconducting electrical conductivity, they are therefore considered a promising candidate for the fabrication of flexible gas sensors that are expected to be used in the Internet of Things and various portable and wearable electronics. In this review, we first introduce the sensing mechanism of SWCNTs and the typical structure and key parameters of SWCNT-based gas sensors. We then summarize research progress on the design, fabrication, and performance of SWCNT-based gas sensors. Finally, the principles and possible approaches to further improving the performance of SWCNT-based gas sensors are discussed.

Aligning 2D nanosheets to form a compact layered structure can maximize the in-plane properties. Here the authors report an efficient and scalable continuous centrifugal casting method to produce highly compact and well-aligned films of GO nanosheets that show record performances in some applications.