Zhenghui Pan

Wrapping Aligned Carbon Nanotube Composite Sheets around Vanadium Nitride Nanowire Arrays for Asymmetric Coaxial Fiber-Shaped Supercapacitors with Ultrahigh Energy Density

The emergence of fiber-shaped supercapacitors (FSSs) has led to a revolution in portable and wearable electronic devices. However, obtaining high energy density FSSs for practical applications is still a key challenge. This article exhibits a facile and effective approach to directly grow well-aligned three-dimensional vanadium nitride (VN) nanowire arrays (NWAs) on carbon nanotube (CNT) fiber with an ultrahigh specific capacitance of 715 mF/cm2 in a three-electrode system. Benefiting from their intriguing structural features, we successfully fabricated a prototype asymmetric coaxial FSS (ACFSS) with a maximum operating voltage of 1.8 V. From core to shell, this ACFSS consists of a CNT fiber core coated with VN@C NWAs as the negative electrode, Na2SO4 poly(vinyl alcohol) (PVA) as the solid electrolyte, and MnO2/conducting polymer/CNT sheets as the positive electrode. The novel coaxial architecture not only fully enables utilization of the effective surface area and decreases the contact resistance between the two electrodes but also, more importantly, provides a short pathway for the ultrafast transport of axial electrons and ions. The electrochemical results show that the optimized ACFSS exhibits a remarkable specific capacitance of 213.5 mF/cm2 and an exceptional energy density of 96.07 μWh/cm2, the highest areal capacitance and areal energy density yet reported in FSSs. Furthermore, the device possesses excellent flexibility in that its capacitance retention reaches 96.8% after bending 5000 times, which further allows it to be woven into flexible electronic clothes with conventional weaving techniques. Therefore, the asymmetric coaxial architectural design allows new opportunities to fabricate high-performance flexible FSSs for future portable and wearable electronic devices.

All-Solid-State High-Energy Asymmetric Supercapacitors Enabled by Three-Dimensional Mixed-Valent MnOx Nanospike and Graphene Electrodes

Three-dimensional (3D) nanostructures enable high-energy storage devices. Here we report a 3D manganese oxide nanospike (NSP) array electrode fabricated by anodization and subsequent electrodeposition. All-solid-state asymmetric supercapacitors were assembled with the 3D Al@Ni@MnOx NSP as the positive electrode, chemically converted graphene (CCG) as the negative electrode, and Na2SO4/poly(vinyl alcohol) (PVA) as the polymer gel electrolyte. Taking advantage of the different potential windows of Al@Ni@MnOx NSP and CCG electrodes, the asymmetric supercapacitor showed an ideal capacitive behavior with a cell voltage up to 1.8 V, capable of lighting up a red LED indicator (nominal voltage of 1.8 V). The device could deliver an energy density of 23.02 W h kg(-1) at a current density of 1 A g(-1). It could also preserve 96.3% of its initial capacitance at a current density of 2 A g(-1) after 10000 charging/discharging cycles. The remarkable performance is attributed to the unique 3D NSP array structure that could play an important role in increasing the effective electrode surface area, facilitating electrolyte permeation, and shortening the electron pathway in the active materials.

Tuning plasmonic and chemical enhancement for SERS detection on graphene-based Au hybrids

Various graphene-based Au nanocomposites have been developed as surface-enhanced Raman scattering (SERS) substrates recently. However, efficient use of SERS has been impeded by the difficulty of tuning SERS enhancement effects induced from chemical and plasmonic enhancement by different preparation methods of graphene. Herein, we developed graphene-based Au hybrids through physical sputtering gold NPs on monolayer graphene prepared by chemical vapor deposition (CVD) as a CVD-G/Au hybrid, as well as graphene oxide-gold (GO/Au) and reduced-graphene oxide (rGO/Au) hybrids prepared using the chemical in situ crystallization growth method. Plasmonic and chemical enhancements were tuned effectively by simple methods in these as-prepared graphene-based Au systems. SERS performances of CVD-G/Au, rGO/Au and GO/Au showed a gradually monotonic increasing tendency of enhancement factors (EFs) for adsorbed Rhodamine 6G (R6G) molecules, which show clear dependence on chemical bonds between graphene and Au, indicating that the chemical enhancement can be steadily controlled by chemical groups in a graphene-based Au hybrid system. Most notably, we demonstrate that the optimized GO/Au was able to detect biomolecules of adenine, which displayed high sensitivity with a detection limit of 10(-7) M as well as good reproducibility and uniformity.

Synthesis of three-dimensional hyperbranched TiO2 nanowire arrays with significantly enhanced photoelectrochemical hydrogen production

The three-dimensional (3D) hierarchical nanostructure is one of the promising candidates for high performance photoelectrochemical (PEC) water splitting electrodes due to the reduced carrier diffusion distance, improved light absorption efficiency and charge collection efficiency. Here, by growing omnidirectional, densely packed branches on TiO2 nanowires, we demonstrated a 3D hyperbranched hierarchical TiO2 nanowire (HHNW) architecture that could significantly enhance the performance of PEC water splitting. Under a solar simulator with chopped AM 1.5G light of 100 mW cm−2 intensity, the HHNW electrode yielded a photocurrent density of 1.21 mA cm−2 at 1.23 V with respect to the reversible hydrogen electrode (RHE), which was about four times higher than that of TiO2 nanowires (NWs) (0.34 mA cm−2). The highest incident photon-to-current conversion efficiency (IPCE) obtained from our HHNWs was 77% at 365–425 nm. This greatly improved PEC performance can be attributed to the improved light absorption efficiency and the increased contact surface areas at the TiO2/electrolyte interface.

Constructing Ultrahigh-Capacity Zinc–Nickel–Cobalt Oxide@Ni(OH)2 Core–Shell Nanowire Arrays for High-Performance Coaxial Fiber-Shaped Asymmetric Supercapacitors

Increased efforts have recently been devoted to developing high-energy-density flexible supercapacitors for their practical applications in portable and wearable electronics. Although high operating voltages have been achieved in fiber-shaped asymmetric supercapacitors (FASCs), low specific capacitance still restricts the further enhancement of their energy density. This article specifies a facile and cost-effective method to directly grow three-dimensionally well-aligned zinc-nickel-cobalt oxide (ZNCO)@Ni(OH)2 nanowire arrays (NWAs) on a carbon nanotube fiber (CNTF) with an ultrahigh specific capacitance of 2847.5 F/cm3 (10.678 F/cm2) at a current density of 1 mA/cm2, These levels are approximately five times higher than those of ZNCO NWAs/CNTF electrodes (2.10 F/cm2) and four times higher than Ni(OH)2/CNTF electrodes (2.55 F/cm2). Benefiting from their unique features, we successfully fabricated a prototype coaxial FASC (CFASC) with a maximum operating voltage of 1.6 V, which was assembled by adopting ZNCO@Ni(OH)2 NWAs/CNTF as the core electrode and a thin layer of carbon coated vanadium nitride (VN@C) NWAs on a carbon nanotube strip (CNTS) as the outer electrode with KOH poly(vinyl alcohol) (PVA) as the gel electrolyte. A high specific capacitance of 94.67 F/cm3 (573.75 mF/cm2) and an exceptional energy density of 33.66 mWh/cm3 (204.02 μWh/cm2) were achieved for our CFASC device, which represent the highest levels of fiber-shaped supercapacitors to date. More importantly, the fiber-shaped ZnO-based photodetector is powered by the integrated CFASC, and it demonstrates excellent sensitivity in detecting UV light. Thus, this work paves the way to the construction of ultrahigh-capacity electrode materials for next-generation wearable energy-storage devices.

Active Manipulation of NIR Plasmonics: the Case of Cu2–xSe through Electrochemistry

Active control of nanocrystal optical and electrical properties is crucial for many of their applications. By electrochemical (de)lithiation of Cu2-xSe, a highly doped semiconductor, dynamic and reversible manipulation of its NIR plasmonics has been achieved. Spectroelectrochemistry results show that NIR plasmon red-shifted and reduced in intensity during lithiation, which can be reversed with perfect on-off switching over 100 cycles. Electrochemical impedance spectroscopy reveals that a Faradaic redox process during Cu2-xSe (de)lithiation is responsible for the optical modulation, rather than simple capacitive charging. XPS analysis identifies a reversible change in the redox state of selenide anion but not copper cation, consistent with DFT calculations. Our findings open up new possibilities for dynamical manipulation of vacancy-induced surface plasmon resonances and have important implications for their use in NIR optical switching and functional circuits.

Interfacial Energy-Level Alignment for High-Performance All-Inorganic Perovskite CsPbBr3 Quantum Dot-Based Inverted Light-Emitting Diodes

All-inorganic perovskite light-emitting diode (PeLED) has a high stability in ambient atmosphere, but it is a big challenge to achieve high performance of the device. Basically, device design, control of energy-level alignment, and reducing the energy barrier between adjacent layers in the architecture of PeLED are important factors to achieve high efficiency. In this study, we report a CsPbBr3-based PeLED with an inverted architecture using lithium-doped TiO2 nanoparticles as the electron transport layer (ETL). The optimal lithium doping balances the charge carrier injection between the hole transport layer and ETL, leading to superior device performance. The device exhibits a current efficiency of 3 cd A-1, a luminance efficiency of 2210 cd m-2, and a low turn-on voltage of 2.3 V. The turn-on voltage is one of the lowest values among reported CsPbBr3-based PeLEDs. A 7-fold increase in device efficiencies has been obtained for lithium-doped TiO2 compared to that for undoped TiO2-based devices.

Ultra-Broadband Flexible Photodetector Based on Topological Crystalline Insulator SnTe with High Responsivity

Topological crystalline insulators (TCIs) are predicted to be a promising candidate material for ultra-broadband photodetectors ranging from ultraviolet (UV) to terahertz (THz) due to its gapless surface state and narrow bulk bandgap. However, the low responsivity of TCIs-based photodetectors limits their further applications. In this regard, a high-performance photodetector based on SnTe, a recently developed TCI, working in a broadband wavelength range from deep UV to mid-IR with high responsivity is reported. By taking advantage of the strong light absorption and small bandgap of SnTe, photodetectors based on the as-grown SnTe crystalline nanoflakes as well as specific short channel length achieve a high responsivity (71.11 A W-1 at 254 nm, 49.03 A W-1 at 635 nm, 10.91 A W-1 at 1550 nm, and 4.17 A W-1 at 4650 nm) and an ultra-broad spectral response (254-4650 nm) simultaneously. Moreover, for the first time, a durable flexible SnTe photodetector fabricated directly on a polyethylene terephthalate film is demonstrated. These results prove the great potential of TCIs as a promising material for integrated and flexible optoelectronic devices.

All-Metal-Organic Framework-Derived Battery Materials on Carbon Nanotube Fibers for Wearable Energy-Storage Device

The ever-increasing demands for portable and wearable electronics continue to drive the development of high-performance fiber-shaped energy-storage devices. Metal-organic frameworks (MOFs) with well-tunable structures and large surface areas hold great potential as precursors and templates to form porous battery materials. However, to date, there are no available reports about fabrication of wearable energy-storage devices on the utilization of all-MOF-derived battery materials directly grown on current collectors. Here, MOF-derived NiZnCoP nanosheet arrays and spindle-like α-Fe2O3 on carbon nanotube fibers are successfully fabricated with impressive electrochemical performance. Furthermore, the resulting all-solid-state fiber-shape aqueous rechargeable batteries take advantage of large specific surface area and abundant reaction sites of well-designed MOF-derived electrode materials to yield a remarkable capacity of 0.092 mAh cm-2 and admirable energy density of 30.61 mWh cm-3, as well as superior mechanical flexibility. Thus, this research may open up exciting opportunities for the development of new-generation wearable aqueous rechargeable batteries.