Although two-dimensional (2D) materials have attracted considerable research interest for use in the development of innovative wearable optoelectronic systems, the integrated optoelectronic performance of 2D materials photodetectors, including flexibility, transparency, broadband response and stability in air, remains quite low to date. Here, we demonstrate a flexible, transparent, high-stability and ultra-broadband photodetector made using large-area and highly-crystalline WSe2 films that were prepared by pulsed-laser deposition (PLD). Benefiting from the 2D physics of WSe2 films, this device exhibits excellent average transparency of 72% in the visible range and superior photoresponse characteristics, including an ultra-broadband detection spectral range from 370 to 1064 nm, reversible photoresponsivity approaching 0.92 A W(-1), external quantum efficiency of up to 180% and a relatively fast response time of 0.9 s. The fabricated photodetector also demonstrates outstanding mechanical flexibility and durability in air. Also, because of the wide compatibility of the PLD-grown WSe2 film, we can fabricate various photodetectors on multiple flexible or rigid substrates, and all these devices will exhibit distinctive switching behavior and superior responsivity. These indicate a possible new strategy for the design and integration of flexible, transparent and broadband photodetectors based on large-area WSe2 films, with great potential for practical applications in the wearable optoelectronic devices.

The progress in the field of graphene has aroused a renaissance of keen research interest in layered transition metal dichalcogenides (TMDs). Tungsten disulfide (WS2), a typical TMD with favorable semiconducting band gap and strong light-matter interaction, exhibits great potential for highly-responsive photodetection. However, WS2-based photodetection is currently unsatisfactory due to the low optical absorption (2%-10%) and poor carrier mobility (0.01-0.91 cm(2) V(-1) s(-1)) of the thin WS2 layers grown by chemical vapor deposition (CVD). Here, we introduce pulsed-laser deposition (PLD) to prepare multilayered WS2 films. Large-area WS2 films of the magnitude of cm(2) are achieved. Comparative measurements of a WS2-based photoresistor demonstrate its stable broadband photoresponse from 370 to 1064 nm, the broadest range demonstrated in WS2 photodetectors. Benefiting from the large optical absorbance (40%-85%) and high carrier mobility (31 cm(2) V(-1) s(-1)), the responsivity of the device approaches a high value of 0.51 A W(-1) in an ambient environment. Such a performance far surpasses the CVD-grown WS2-based photodetectors (μA W(-1)). In a vacuum environment, the responsivity is further enhanced to 0.70 A W(-1) along with an external quantum efficiency of 137% and a photodetectivity of 2.7 × 10(9) cm Hz(1/2) W(-1). These findings stress that the PLD-grown WS2 film may constitute a new paradigm for the next-generation stable, broadband and highly-responsive photodetectors.

A facile pathway of the electrocatalytic nitrogen oxidation reaction (NOR) to nitrate is proposed, and Ru‐doped TiO2/RuO2 (abbreviated as Ru/TiO2) as a proof‐of‐concept catalyst is employed accordingly. Density functional theory (DFT) calculations suggest that Ruδ+ can function as the main active center for the NOR process. Remarkably doping Ru into the TiO2 lattice can induce an upshift of the d‐band center of the Ru site, resulting in enhanced activity for accelerating electrochemical conversion of inert N2 to active NO*. Overdoping of Ru ions will lead to the formation of additional RuO2 on the TiO2 surface, which provides oxygen evolution reaction (OER) active sites for promoting the redox transformation of the NO* intermediate to nitrate. However, too much RuO2 in the catalyst is detrimental to both the selectivity of the NOR and the Faradaic efficiency due to the dominant OER process. Experimentally, a considerable nitrate yield rate of 161.9 µmol h−1 gcat−1 (besides, a total nitrate yield of 47.9 µg during 50 h) and a highest nitrate Faradaic efficiency of 26.1% are achieved by the Ru/TiO2 catalyst (with the hybrid composition of RuxTiyO2 and extra RuO2 by 2.79 wt% Ru addition amount) in 0.1 m Na2SO4 electrolyte.

The oxygen evolution reaction (OER) is a key process involved in energy and environment‐related technologies. An ideal OER electrocatalyst should show high exposure of active sites and optimal adsorption energies of oxygenated species. However, earth‐abundant transition‐metal‐based OER electrocatalysts still operate with sluggish OER kinetics. Here, a cation‐exchange route is reported to fabricate cobalt‐vanadium‐iron (oxy)hydroxide (CoV‐Fe0.28) nanosheets with tunable binding energies for the oxygenated intermediates. The formation of an amorphous/crystalline heterostructure in the CoV‐Fe0.28 catalyst boosts the exposure of active sites compared to their crystalline and amorphous counterparts. Furthermore, the synergetic interaction of Co, V, and Fe cations in the CoV‐Fe0.28 catalyst subtly regulates the local coordination environment and electronic structure, resulting in the optimal thermodynamic barrier for this elementary reaction step. As a result, the CoV‐Fe0.28 catalyst exhibits superior electrocatalytic activity toward the OER. A low overpotential of 215 mV is required to afford a current density of 10 mA cm−2 with a small Tafel slope of 39.1 mV dec−1, which outperforms commercial RuO2 (321 mV and 86.2 mV dec−1, respectively).

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