Surface Stoichiometry Control of Colloidal Heterostructured Quantum Dots for High-Performance Photoelectrochemical Hydrogen Generation.

Manipulating the separation and transfer behaviors of charges has long been pursued for promoting the photoelectrochemical (PEC) hydrogen generation based on II-VI quantum dot (QDs), but remains challenging due to the lack of effective strategies. Herein, a facile strategy is reported to regulate the recombination and transfer of interfacial charges through tuning the surface stoichiometry of heterostructured QDs. Using this method, it is demonstrated that the PEC cells based on CdSe-(Sex S1- x )4 -(CdS)2 core/shell QDs with a proper Ssurface /Cdsurface ratio exhibits a remarkably improved photocurrent density (≈18.4 mA cm-2 under one sun illumination), superior to the PEC cells based on QDs with Cd-rich or excessive S-rich surface. In-depth electrochemical and spectroscopic characterizations reveal the critical role (hole traps) of surface S atoms in suppressing the recombination of photogenerated charges, and further attribute the inferior performance of excessive S-rich QDs to the impeded charge transfer from QDs to TiO2 and electrolyte. This work puts forward a simple surface engineering strategy for improving the performance of QDs PEC cells, providing an efficient method to guide the surface design of QDs for their applications in other optoelectronic devices.

Room-Temperature Direct Synthesis of PbSe Quantum Dot Inks for High-Detectivity Near-Infrared Photodetectors.

A PbSe colloidal quantum dot (QD) is typically a solution-processed semiconductor for near-infrared (NIR) optoelectronic applications. However, the wide application of PbSe QDs has been restricted due to their instability, which requires tedious synthesis and complicated treatments before being applied in devices. Here, we demonstrate efficient NIR photodetectors based on the room-temperature, direct synthesis of semiconducting PbSe QD inks. The in-situ passivation and the avoidance of ligand exchange endow PbSe QD photodetectors with high efficiency and low cost. By further constructing the PbSe QDs/ZnO heterostructure, the photodetectors exhibit the NIR responsivity up to 970 mA/W and a detectivity of 1.86 × 1011 Jones at 808 nm. The obtained performance is comparable to that of the state-of-the-art PbSe QD photodetectors using a complex ligand exchange strategy. Our work may pave a new way for fabricating efficient and low-cost colloidal QD photodetectors.

Flexible Self-Powered Real-Time Ultraviolet Photodetector by Coupling Triboelectric and Photoelectric Effects.

The portable UV photodetector is used to timely remind humans of overexposure to UV radiation. However, the traditional UV photodetector cannot meet the practical demands, and the power supply problem hinders its further development. In this work, we demonstrated a flexible, transparent, and self-powered UV photodetector by coupling of triboelectric and photoelectric effects. The device integrates a flexible ZnO nanoparticle (NP) UV photodetector, a transparent- and flexible-film-based TENG (TFF-TENG), commercial chip resistors, and LEDs on the PET thin film. The TFF-TENG could harvest mechanical energy from finger tapping and sliding motion and power the ZnO NP UV photodetector to realize self-powered detection. The voltage of the constant resistors connected with the UV photodetector in series changes from 0.5 to 19 V under the UV light with power intensities increasing from 0.46 to 21.8 mW/cm2, and the voltage variation is reflected by the number of LEDs directly. The excellent flexibility and transparency of the device could extend its application scenarios; for example, such a portable device could be applied to real-time monitoring of the UV radiation to remind humans of intense UV light.

A liquid PEDOT:PSS electrode-based stretchable triboelectric nanogenerator for a portable self-charging power source.

The rapid development of wearable electronics has led to an enormous demand for power sources that are wearable, small-scale, flexible and compatible. In this work, poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) as the liquid electrode and silicone rubber as the triboelectric/encapsulation layer were introduced to design a stretchable PEDOT:PSS liquid electrode-based triboelectric nanogenerator (PL-TENG). The elastic silicone rubber and PEDOT:PSS liquid electrode with a special macromolecular structure endowed PL-TENG with extraordinary flexibility and conductivity simultaneously. Working under the single-electrode mode with different motion frequencies from 0.5 to 2.5 Hz, PL-TENG generated open-circuit voltage of 265 V, short-circuit current of 24.9 µA and short-circuit charge quantity of 85 nC. The output performances still maintained the original values after washing in saline, storing for one month and stretching 10 000 times. At the same time, PL-TENG could also produce stable electrical outputs even when deformed into a variety of shapes including stretching in different directions, bending and twisting. All of these features demonstrated the excellent resistance of PL-TENG to sweat, time and deformation. When attached to a human body, PL-TENG could provide a sufficiently stable power output to drive wearable electronics sustainably.

Spiral Steel Wire Based Fiber-Shaped Stretchable and Tailorable Triboelectric Nanogenerator for Wearable Power Source and Active Gesture Sensor.

Continuous deforming always leads to the performance degradation of a flexible triboelectric nanogenerator due to the Young's modulus mismatch of different functional layers. In this work, we fabricated a fiber-shaped stretchable and tailorable triboelectric nanogenerator (FST-TENG) based on the geometric construction of a steel wire as electrode and ingenious selection of silicone rubber as triboelectric layer. Owing to the great robustness and continuous conductivity, the FST-TENGs demonstrate high stability, stretchability, and even tailorability. For a single device with ~ 6 cm in length and ~ 3 mm in diameter, the open-circuit voltage of ~ 59.7 V, transferred charge of ~ 23.7 nC, short-circuit current of ~ 2.67 µA and average power of ~ 2.13 µW can be obtained at 2.5 Hz. By knitting several FST-TENGs to be a fabric or a bracelet, it enables to harvest human motion energy and then to drive a wearable electronic device. Finally, it can also be woven on dorsum of glove to monitor the movements of gesture, which can recognize every single finger, different bending angle, and numbers of bent finger by analyzing voltage signals.

PbS Quantum Dots/2D Nonlayered CdS xSe1- x Nanosheet Hybrid Nanostructure for High-Performance Broadband Photodetectors.

Two-dimensional (2D) nonlayered nanomaterials have attracted extensive attention for electronic and optoelectronic applications recently because of their distinct properties. In this work, we first employed a facile one-step method to synthesize 2D nonlayered cadmium sulfide selenide (CdS xSe1- x, x = 0.33) nanosheets with a highly crystalline structure and then we introduced a generic spin-coating approach to fabricate hybrid nanomaterials composed of PbS quantum dots (QDs) and 2D CdS xSe1- x nanosheets and demonstrated their potential for high-performance broadband photodetectors. Compared with pure 2D CdS xSe1- x nanosheet photodetectors, the photoelectric performance of the PbS/CdS xSe1- x hybrid nanostructure is enhanced by 3 orders of magnitude under near-infrared (NIR) light illumination and maintains its performance in the visible (Vis) range. The photodetector exhibits a broadband response range from Vis to NIR with an ultrahigh light-to-dark current ratio (3.45 × 106), a high spectral responsivity (1.45 × 103 A/W), and high detectivity (1.05 × 1015 Jones). The proposed QDs/2D nonlayered hybrid nanostructure-based photodetector paves a promising way for next-generation high-performance broadband optoelectronic devices.