Interdigitated and square laser-induced graphene (LIG) electrodes were successfully fabricated by direct laser writing of common natural cork bottle stoppers. The laser graphitization process was performed with a low-cost hobbyist visible laser in a simple, fast, and one-step process under ambient conditions. The formation of LIG material was revealed by extensive characterization using Raman, attenuated total reflection-Fourier transform infrared (ATR-FTIR), and X-ray photoelectron (XPS) spectroscopies. Electron microscopy investigation showed that the formed LIG structure maintained the hierarchical alveolar structure of the pristine cork but displayed increased surface area, disorder, and electrical conductivity, promising for electrochemical applications. Open planar and sandwich supercapacitors, assembled from fabricated electrodes using poly(vinyl alcohol) PVA/H + as an electrolyte, exhibited a maximum areal capacitance of 1.56 mF/cm 2 and 3.77 mF/cm 2 at a current density 0.1 mA/cm 2 , respectively. Upon treatment with boric acid (H 3 BO 3 ), the areal capacitance of the resulting boron-doped LIG devices increased by ca. three times, reaching 4.67 mF/cm 2 and 11.24 mF/cm 2 at 0.1 mA/cm 2 current density for planar and sandwich configurations, respectively. Supercapacitor devices showed excellent stability over time with only a 14% loss after >10 000 charge/discharge cycles. The easy, fast, scalable, and energy-efficient method of fabrication illustrated in this work, combined with the use of natural and abundant materials, opens avenues for future large-scale production of "green" supercapacitor devices.
A reagent-less pH sensor based on disposable and low cost carbon fibre cloth (CFC) is demonstrated for the first time, where tungsten oxide nanoparticles were grown directly onto the CFC substrate. For comparison purpose, tungsten oxide nanoparticle modified glassy carbon electrode (GCE) was also fabricated as a pH sensor, where hydrothermally synthesized tungsten oxide nanoparticles were drop casted onto the GCE surface. The corresponding equilibrium potential using tungsten oxide/CFC as a pH sensor was measured using open circuit potential (OCP), and was found to be linear over the pH range of 3–10, with a sensitivity of 41.38 mVpH−1, and response time of 150 s. In the case of tungsten oxide/GCE as a pH sensor, square wave voltammetry (SWV) was used to measure the shifts in peak potential and was found to be linear with a pH range of 3–11, and a sensitivity of 60 mVpH−1 with a potential drift of 2.4–5.0% after 3 hour of continuous use. The advantages of tungsten oxide/CFC and tungsten oxide/GCE as pH sensing electrode have been directly compared with the commercial glass probe based electrode, and validated in real un-buffered samples. Thereby, tungsten oxide nanoparticles with good sensitivity and long term stability could be potentially implemented as a low cost and robust pH sensor in numerous applications for the Internet of Things (IoT).
Single crystals of organolead halide perovskites attract much attention to electrooptical and photovoltaic applications. They are usually prepared in precursor solutions incubated at controlled temperatures or under optimized vapor atmosphere conditions, and thus, multiple perovskite crystals are nucleated all over the solution. Multiple nucleation of crystals prevents efficient use of precursors in the preferential growth of large single crystals. An innovative approach is presented for spatiotemporally controlled, selective nucleation and growth of single crystals of lead halide perovskites by optical trapping with a focused laser beam. Upon such trapping in unsaturated precursor solutions, nucleation of MAPbX (MA=CH NH ; X=Cl , Br , or I ) is induced at the focal spot through increase in the concentration of perovskite precursors in the focal volume. The rate at which the nucleated crystal grows depends upon whether the perovskite absorbs the trapping laser or not. These findings suggest that optical trapping would be useful to prepare various perovskite single crystals and modify their optical and electronic properties; thereby, offering new methods for engineering of perovskite crystals.
Local halide exchange reactions enable one to fabricate heterojunction perovskites; however, it is particularly challenging to deliver reactive halide precursors at the desired position. Here, we report an innovative approach for the fabrication of heterojunction perovskites by the localized halide exchange. We demonstrate the tuning of bandgap and the emission color of the desired domain in a lead halide perovskite microrod, which is realized by increasing the local concentration of the halide precursor under optical trapping using a nonresonant near-infrared laser beam. Similarly, the bandgap and the emission color of a crystal among several crystals are temporally tuned by a locally induced halide exchange reaction. Using this method, we overcome spontaneous halide exchange at undesired locations or crystals. We minimize photothermal and photochemical effects on halide exchange and photoinduced damage to the crystals by optical trapping using a 1064 nm continuous wave laser beam. The site-specific halide exchange offers flexible spatial control of bandgap and photoluminescence for designing perovskite-based heterojunction structures by laser scanning.
The development of new methods to engineer lead halide perovskite crystals with a controlled band gap and emission properties is an active subject in materials science and chemistry. We present the preparation of mixed-halide lead perovskites by spatially-and temporally-controlled chemical reactions and crystal growth under an optical potential in unsaturated precursor solutions. The crystals are characterized by transmission and photoluminescence spectral measurements and X-ray diffraction analysis. When compared with the spontaneous formation of multiple crystals in saturated precursor solutions, the optical potential creates large single crystals with a high chloride composition, providing distinct blue and green fluorescent crystals of chloride-bromide lead perovskites. We discuss the formation of mixed-halide perovskites from the viewpoints of an increased rate of chemical reaction via the formation and desolvation of precursor complexes and a decreased free energy potential.
This paper reports chiral mixed Eu(iii)–Ln(iii) coordination polymers (Ln = Gd and Sm) for the enhancement of the emission quantum yield (Φtot ≥ 50%), achieved via control of 4f electronic structures.
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