Binary and Ternary Colloidal Cu-Sn-Te Nanocrystals for Thermoelectric Thin Films.

Recent advances in copper chalcogenide-based nanocrystals (NCs), copper sulfide, and copper selenide derived nanostructures, have drawn considerable attention. However, reports of crystal phase and shape engineering of binary or ternary copper telluride NCs remain rare. Here, a colloidal hot-injection approach for producing binary copper/tin telluride, and ternary copper tin telluride NCs with controllable compositions, crystal structures, and morphologies is reported. The crystal phase and growth behavior of these tellurides are systematically studied from both experimental and theoretical perspectives. The morphology of Cu1.29 Te NCs is modified from 1D nanorods with different aspect ratios to 2D nanosheets and 3D nanocubes, by controlling the preferential growth of specific crystalline facets. A controllable phase transition from Cu1.29 Te to Cu1.43 Te NCs is also demonstrated. The latter can be further converted into Cu2 SnTe3 and SnTe through Sn incorporation. Temperature dependent thermoelectric properties of metal (Cu and Sn) telluride nanostructure thin films are also studied, including Cu1.29 Te, Cu1.43 Te, Cu2 SnTe3 , and SnTe. Cu2 SnTe3 is a low carrier density semimetal with compensating electron and hole Fermi surface pockets. The engineering of crystal phase and morphology control of colloidal copper tin telluride NCs opens a path to explore and design new classes of copper telluride-based nanomaterials for thermoelectrics and other applications.

Controllable Colloidal Synthesis of Tin(II) Chalcogenide Nanocrystals and Their Solution-Processed Flexible Thermoelectric Thin Films.

A systematic colloidal synthesis approach to prepare tin(II, IV) chalcogenide nanocrystals with controllable valence and morphology is reported, and the preparation of solution-processed nanostructured thermoelectric thin films from them is then demonstrated. Triangular SnS nanoplates with a recently-reported π-cubic structure, SnSe with various shapes (nanostars and both rectangular and hexagonal nanoplates), SnTe nanorods, and previously reported Sn(IV) chalcogenides, are obtained using different combinations of solvents and ligands with an Sn4+ precursor. These unique nanostructures and the lattice defects associated with their Sn-rich composition allow the production of flexible thin films with competitive thermoelectric performance, exhibiting room temperature Seebeck coefficients of 115, 81, and 153 µV K-1 for SnS, SnSe, and SnTe films, respectively. Interestingly, a p-type to n-type transition is observed in SnS and SnSe due to partial anion loss during post-synthesis annealing at 500 °C. A maximum figure of merit (ZT) value of 0.183 is achieved for an SnTe thin film at 500 K, exceeding ZT values from previous reports on SnTe at this temperature. Thus, a general strategy to prepare tin(II) chalcogenide nanocrystals is provided, and their potential for use in high-performance flexible thin film thermoelectric generators is demonstrated.

Ultrathin, Washable, and Large-Area Graphene Papers for Personal Thermal Management.

Freestanding, flexible/foldable, and wearable bifuctional ultrathin graphene paper for heating and cooling is fabricated as an active material in personal thermal management (PTM). The promising electrical conductivity grants the superior Joule heating for extra warmth of 42 °C using a low supply voltage around 3.2 V. Besides, based on its high out-of-plane thermal conductivity, the graphene paper provides passive cooling via thermal transmission from the human body to the environment within 7 s. The cooling effect of graphene paper is superior compared with that of the normal cotton fiber, and this advantage will become more prominent with the increased thickness difference. The present bifunctional graphene paper possesses high durability against bending cycles over 500 times and wash time over 1500 min, suggesting its great potential in wearable PTM.

Flexible thermoelectric fabrics based on self-assembled tellurium nanorods with a large power factor.

Highly-flexible thermoelectric fabrics were fabricated based on a layered structure, composed of a thin active layer of self-assembled tellurium nanorods and a substrate layer of polyvinylidene fluoride. The resulting thermoelectric fabrics show a high room temperature power factor of 45.8 µW m(-1) K(-2), which opens a new avenue to fabricate highly-flexible sustainable energy sources.

Seedless synthesis of layered ZnO nanowall networks on Al substrate for white light electroluminescence.

In this paper, layered ZnO nanowall networks were directly grown on Al substrates using a hydrothermal method without predepositing seed layers. The individual ZnO nanowalls with a thickness of several nanometers and a size of several hundred nanometers were (002) surface dominated, in which the preferential growth direction of ZnO was suppressed. White electroluminescence devices were fabricated based on Au/polymethylmethacrylate/ZnO-nanowall (metal-insulator-semiconductor) structures. The chromaticity coordinate of the electroluminescence spectrum for the optimal device was calculated as (0.27, 0.34), which is close to (0.33, 0.33) of standard white light.

Multilayered carbon nanotube/polymer composite based thermoelectric fabrics.

Thermoelectrics are materials capable of the solid-state conversion between thermal and electrical energy. Carbon nanotube/polymer composite thin films are known to exhibit thermoelectric effects, however, have a low figure of merit (ZT) of 0.02. In this work, we demonstrate individual composite films of multiwalled carbon nanotubes (MWNT)/polyvinylidene fluoride (PVDF) that are layered into multiple element modules that resemble a felt fabric. The thermoelectric voltage generated by these fabrics is the sum of contributions from each layer, resulting in increased power output. Since these fabrics have the potential to be cheaper, lighter, and more easily processed than the commonly used thermoelectric bismuth telluride, the overall performance of the fabric shows promise as a realistic alternative in a number of applications such as portable lightweight electronics.

Retraction: Colloidal Cobalt Phosphide Nanocrystals as Trifunctional Electrocatalysts for Overall Water Splitting Powered by a Zinc-Air Battery.

Adv. Mater. 2018, 30, 1705796 https://doi.org/10.1002/adma.201705796 The above article, published online on January 15, 2018, in Wiley Online Library (https://doi.org/10.1002/adma.201705796), has been retracted by agreement between the authors, the journal Editor in Chief Jos Lenders, and Wiley-VCH GmbH. The retraction has been agreed on following concerns raised by a third party and a subsequent investigation at Wake Forest University. Data integrity issues were found in Figures 1a, S2b, and S17. As a result, the authors consider the conclusions of this article invalid.

Long-term survival following a single treatment of kidney tumors with multiwalled carbon nanotubes and near-infrared radiation.

Multiwalled carbon nanotubes (MWCNTs) exhibit physical properties that render them ideal candidates for application as noninvasive mediators of photothermal cancer ablation. Here, we demonstrate that use of MWCNTs to generate heat in response to near-infrared radiation (NIR) results in thermal destruction of kidney cancer in vitro and in vivo. We document the thermal effects of the therapy through magnetic resonance temperature-mapping and heat shock protein-reactive immunohistochemistry. Our results demonstrate that use of MWCNTs enables ablation of tumors with low laser powers (3 W/cm(2)) and very short treatment times (a single 30-sec treatment) with minimal local toxicity and no evident systemic toxicity. These treatment parameters resulted in complete ablation of tumors and a >3.5-month durable remission in 80% of mice treated with 100 microg of MWCNT. Use of MWCNTs with NIR may be effective in anticancer therapy.

Correction: Synthesis of lead-free Cs3Sb2Br9 perovskite alternative nanocrystals with enhanced photocatalytic CO2 reduction activity.

Correction for 'Synthesis of lead-free Cs3Sb2Br9 perovskite alternative nanocrystals with enhanced photocatalytic CO2 reduction activity' by Chang Lu et al., Nanoscale, 2020, 12, 2987-2991, https://doi.org/10.1039/C9NR07722G.

A soluble high molecular weight copolymer of benzo[1,2-b:4,5-b']dithiophene and benzoxadiazole for efficient organic photovoltaics.

The synthesis and characterization of a soluble high molecular weight copolymer based on 4,8-bis(1-pentylhexyloxy)benzo[1,2-b:4,5-b']dithiophene and 2,1,3-benzoxadiazole is presented. High efficiency organic photovoltaic (OPV) devices comprised of this polymer and phenyl-C(71) -butyric acid methyl ester (PC(71) BM) were fabricated by additive processing with 1-chloronapthalene (CN). When the active layer is cast from pristine chlorobenzene (CB), power conversion efficiencies (PCEs) average 1.41%. Our best condition-using 2% chloronapthalene as a solvent additive in CB-results in an average PCE of 5.65%, with a champion efficiency of 6.05%.

Enhancement of electric oxygen-iodine laser performance using larger mode volume resonators.

Herein the authors report on the demonstration of an 87% enhancement in cw laser power on the 1315 nm transition of atomic iodine via a 100% increase in the resonator mode volume. O(2)(a1Delta) is produced by a single rf-excited electric discharge sustained in an O(2)-He-NO gas mixture flowing through a rectangular geometry, and I(P2(1/2)) is then pumped using energy transferred from O(2)(a1Delta). A total laser output power of 102.5 W was obtained using a Z-pass resonator configuration.

Perovskite Quantum-Dot-in-Host for Detection of Ionizing Radiation.

The concept of quantum-dot-in-perovskite solids pioneered by Ning and co-workers introduces a useful class of solution-processed type I heterostructures for optoelectronics applications. Concurrent searches for solution-processable detectors of ionizing radiation have focused on lead-halide perovskites. As described in this issue of ACS Nano, Cao et al. examined CsPbBr3 nanocrystals imbedded in Cs4PbBr6 as a wider gap host and determined its performance and possibilities as a scintillator for X-ray imaging. In this Perspective, we describe issues and research opportunities on ionizing radiation imaging and spectroscopy based on the CsPbBr3@Cs4PbBr6 composite and other perovskite-dot-in-host combinations in which the dot may be of lower dimensionality than 3, and we explore ionizing radiation detectors using halide perovskites.

Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways.

Despite progress in small scale electrocatalytic production of hydrogen peroxide (H2O2) using a rotating ring-disk electrode, further work is needed to develop a non-toxic, selective, and stable O2-to-H2O2 electrocatalyst for realizing continuous on-site production of neutral hydrogen peroxide. We report ultrasmall and monodisperse colloidal PtP2 nanocrystals that achieve H2O2 production at near zero-overpotential with near unity H2O2 selectivity at 0.27 V vs. RHE. Density functional theory calculations indicate that P promotes hydrogenation of OOH* to H2O2 by weakening the Pt-OOH* bond and suppressing the dissociative OOH* to O* pathway. Atomic layer deposition of Al2O3 prevents NC aggregation and enables application in a polymer electrolyte membrane fuel cell (PEMFC) with a maximum r(H2O2) of 2.26 mmol h-1 cm-2 and a current efficiency of 78.8% even at a high current density of 150 mA cm-2. Catalyst stability enables an accumulated neutral H2O2 concentration in 600 mL of 3.0 wt% (pH = 6.6).

Synthesis of lead-free Cs3Sb2Br9 perovskite alternative nanocrystals with enhanced photocatalytic CO2 reduction activity.

A synthetic method for uniform and pure Cs3Sb2Br9 NCs has been developed. Cs3Sb2Br9 NCs exhibit a 10-fold increase in activity for the photocatalytic CO2 reduction reaction compared to CsPbBr3 NCs, achieving 510 µmol CO g-1 cat. after 4 h. Density functional theory shows that Cs3Sb2Br9 surfaces sufficiently expose Sb to allow reactivity, as opposed to the unreactive CsPbBr3 surface.

Effects of including a diffraction term into Rigrod theory for a continuous-wave laser.

Multimode, low-gain continuous-wave lasers are often subject to having intracavity apertures that create diffractive losses inside the optical resonator. For very low-gain systems with short gain lengths, highly reflective mirrors are required to obtain laser oscillation. The Rigrod theory was modified to include a diffractive loss term and comparisons with experimental data show that the intracavity diffractive losses, while small in magnitude, can play a significant role for these low-gain cases with high mirror reflectivities.

Enhanced absorption in a reverse saturable absorbing dye blended with carbon nanotubes.

Using nonlinear absorption at 532 nm in the nanosecond temporal regime, we have measured the low fluence nonlinear transmittance properties of the reverse saturable absorbing carbocyanine dye, 1,1',3,3,3',3'-hexamethylindotricarbocyanine iodide (HITCI), blended with well dispersed carbon nanotubes. The nonlinear optical properties of the blends are strongly dependent on the ratio of dye to nanotubes in solution. In the case where the nanotubes per dye molecule ratio is large, we see a distinctive enhancement in optical fluence limiting properties of the system, suggesting enhanced absorption of the excited states. However, when the nanotube to dye ratio decreases, the system's response is dominated by the behavior of the dye. We suggest that this can be understood as a two component system in which sensitized dye molecules associated with the nanotubes have an effectively different optical cross-section from the dye molecules far from the nanotubes. From classical antennae considerations, this is expected.

Controllable colloidal synthesis of anisotropic tin dichalcogenide nanocrystals for thin film thermoelectrics.

Tin chalcogenides have shown promise in applications including energy storage, optoelectronics, photovoltaics, and thermoelectrics. Here, we present a colloidal synthesis strategy to produce tin dichalcogenide nanocrystals (NCs) with controllable stoichiometry, vacancies, shape, and crystal structure. Compared with previously reported methods, we use less expensive precursors, such as tin(iv) chloride and sulfur or selenium powder, to produce tin(iv) chalcogenide NCs. SnS2 and SnSe2 NCs with novel NC morphologies including SnS2 nanoflowers/nanoflakes, SnSe2 nanosheets with circular and hexagonal shapes, as well as mixtures of nanospheres and nanoflakes were prepared by varying the solvents and anion precursors. We were also able to reduce tin(iv) to tin(ii) to produce tin(ii) chalcogenide NCs. The corresponding thin films were prepared by spin-coating, followed by post-treatment to study their thermoelectric properties. Room temperature Seebeck coefficients of -150 µV K-1 and -126 µV K-1 were measured for SnS2 and SnSe2 films, demonstrating their promise as thin film thermoelectric materials.

Highly robust and flexible n-type thermoelectric film based on Ag2Te nanoshuttle/polyvinylidene fluoride hybrids.

Highly robust and flexible n-type thermoelectric (TE) films based on Ag2Te nanoshuttle/polyvinylidene fluoride were prepared by a solution-processable method without a surfactant. A good power performance of over 30 µW (m K2)-1 at room temperature was achieved. Moreover, the synthesized fabrics also exhibited potential for application in flexible electronic devices with negligible performance change after 1000 bending cycles.

Wearable Thermoelectric Devices Based on Au-Decorated Two-Dimensional MoS2.

Two-dimensional (2D) materials have recently opened a new avenue to flexible thermoelectric materials with enhanced performance because of their unique electronic transport properties. Here, we report a feasible approach to improve the thermoelectric performance of transition-metal dichalcogenides by effectively decorating 2D MoS2 with Au nanoparticles using in situ growth. The present Au-decorated MoS2-assembled heterojunction system shows a certain decoupled phenomenon, that is, the Seebeck coefficient and conductivity increased simultaneously. This is due to the occurrence of p-type doping of the MoS2 2H phase and injection energy filtering of dopant-originated carriers around the local band bending at the interface. The composite flexible films can achieve a power factor value of 166.3 µW m-1 K-2 at room temperature, which have great potential for harvesting human body heat.

Tailoring spin mixtures by ion-enhanced Maxwell magnetic coupling in color-tunable organic electroluminescent devices.

In this work, we show that the spin dynamics of excitons can be dramatically altered by Maxwell magnetic field coupling, together with an ion-enhanced, low-internal-splitting-energy organic semiconducting emitter. By employing a unique, alternating current (AC)-driven organic electroluminescent (OEL) device architecture that optimizes this magnetic field coupling, almost complete control over the singlet-to-triplet ratio (from fluorescent to phosphorescent emission in a single device) is realized. We attribute this spin population control to magnetically sensitive polaron-spin pair intersystem crossings (ISCs) that can be directly manipulated through external driving conditions. As an illustration of the utility of this approach to spin-tailoring, we demonstrate a simple hybrid (double-layer) fluorescence-phosphorescence (F-P) device using a polyfluorene-based emitter with a strong external Zeeman effect and ion-induced long carrier diffusion. Remarkable control over de-excitation pathways is achieved by controlling the device-driving frequency, resulting in complete emission blue-red color tunability. Picosecond photoluminescence (PL) spectroscopy directly confirms that this color control derives from the magnetic manipulation of the singlet-to-triplet ratios. These results may pave the way to far more exotic organic devices with magnetic-field-coupled organic systems that are poised to usher in an era of dynamic spintronics at room temperature.