A photon-recycling incandescent lighting device.

Energy-efficient, healthy lighting is vital for human beings. Incandescent lighting provides high-fidelity color rendering and ergonomic visual comfort yet is phased out owing to low luminous efficacy (15 lumens per watt) and poor lifetime (2000 hours). Here, we propose and experimentally realize a photon-recycling incandescent lighting device (PRILD) with a luminous efficacy of 173.6 lumens per watt (efficiency of 25.4%) at a power density of 277 watts per square centimeter, a color rendering index (CRI) of 96, and a LT70-rated lifetime of >60,000 hours. The PRILD uses a machine learning-designed 637-nm-thick visible-transparent infrared-reflective filter and a Janus carbon nanotube/hexagonal boron nitride filament to recycle 92% of the infrared radiation. The PRILD has higher luminous efficacy, CRI, and lifetime compared with solid-state lighting and thus is promising for high-power density lighting.

Module-Level Polaritonic Thermophotovoltaic Emitters via Hierarchical Sequential Learning.

Thermophotovoltaic (TPV) generators provide continuous and high-efficiency power output by utilizing local thermal emitters to convert energy from various sources to thermal radiation matching the bandgaps of photovoltaic cells. Lack of effective guidelines for thermal emission control at high temperatures, poor thermal stability, and limited fabrication scalability are the three key challenges for the practical deployment of TPV devices. Here we develop a hierarchical sequential-learning optimization framework and experimentally realize a 6″ module-scale polaritonic thermal emitter with bandwidth-controlled thermal emission as well as excellent thermal stability at 1473 K. The 300 nm bandwidth thermal emission is realized by a complex photon polariton based on the superposition of Tamm plasmon polariton and surface plasmon polariton. We experimentally achieve a spectral efficiency of 65.6% (wavelength range of 0.4-8 µm) with statistical deviation less than 4% over the 6″ emitter, demonstrating industrial-level reliability for module-scale TPV applications.

Multiscale Plasmonic Refractory Nanocomposites for High-Temperature Solar Photothermal Conversion.

Development of a refractory selective solar absorber (RSSA) is the key to unlock high-temperature solar thermal and thermochemical conversion. The fundamental challenge of RSSA is the lack of design and fabrication guidelines to simultaneously achieve omnidirectional, broadband solar absorption and sharp spectral selectivity at the desired cutoff wavelength. Here, we realize a ruthenium-carbon nanotube (Ru-CNT) nanocomposite RSSA with multiscale nanoparticle-on-nanocavity plasmonic modes. Ru conformally coated on the sidewalls of CNTs enables a spoof surface plasmon polariton mode for spectra selectivity; Ru nanoparticles formed at the tips of CNTs enable a localized surface plasmon resonance mode and plasmon hybridization for omnidirectional broadband solar absorption. The fabricated Ru-CNT RSSA has a total solar absorption (TSA) of 96.1% with sharp spectral cutoff at 2.21 µm. The TSA is maintained at over 90% for an incident angle of 56°. Our findings therefore guide full-spectrum optical and thermal control from visible to the far-infrared.

Unzipping Carbon Nanotube Bundles through NH-π Stacking for Enhanced Electrical and Thermal Transport.

Bundling of single-walled carbon nanotubes (SWCNTs) significantly undermines their superior thermal and electrical properties. Realizing stable, homogeneous, and surfactant-free dispersion of SWCNTs in solvents and composites has long been regarded as a key challenge. Here, we report amine-containing aromatic and cyclohexane molecules, which are common chain extenders (CEs) for epoxy curing in industry, can be used to effectively disperse CNTs. We achieve single-tube-level dispersion of SWCNTs in CE solvents, as demonstrated by the strong chirality-dependent absorption and photoluminescence emission. The SWCNT-CE dispersion remains stable under ambient conditions for months. The excellent dispersibility and stability are attributed to the formation of an n-type charge-transfer complex through the NH-π interaction between the amine group of CEs and the delocalized π bond of SWCNTs, which is confirmed by the negative Seebeck coefficient of the CE-functionalized SWCNT films, the red shift of the G band in the Raman spectra, and the NH-π peak in X-ray photoelectron spectroscopy. The high dispersibility of CEs significantly improves the electrical and thermal transport of macroscale CNT assemblies. The sheet resistance of the CE-dispersed SWCNT thin films reaches 161 Ω sq-1 at 80.8% optical transmittance after functional modification by HNO3. Moreover, the CEs cross-link CNTs and epoxy molecules, forming a pathway for phonon transport in CNT/epoxy nanocomposites. The thermal conductivity of the CE-CNT-epoxy composite is enhanced by 1850% compared with the original epoxy, which is the highest enhancement reported to date for CNT/epoxy nanocomposites. The CE-based NH-π interaction provides a new paradigm for the effective and stable dispersion of SWCNTs in a facile and scalable process.

Light-Driven Nanodroplet Generation Using Porous Membranes.

A simple, fast, and contactless alternative for the generation of nanodroplets in solution is to apply light to stimulate their formation at a surface. In this work, a light-driven mechanism for the generation of nanodroplets is demonstrated by using a porous membrane. The membrane is placed at the interface between oil and water during the nanodroplet generation process. As light illuminates the membrane a photothermal conversion process induces the growth and release of water vapor bubbles into the aqueous phase. This release leads to the fluctuation of local pressure around the pores and enables the generation of oil nanodroplets. A computational simulation of the fluid dynamics provides insight into the underlying mechanism and the extent to which it is possible to increase nanodroplet concentrations. The ability to form nanodroplets in solutions without the need for mechanical moving parts is significant for the diverse biomedical and chemical applications of these materials.

Breakdown of Native Oxide Enables Multifunctional, Free-Form Carbon Nanotube-Metal Hierarchical Architectures.

Passive oxide layers on metal substrates impose remarkable interfacial resistance for electron and phonon transport. Here, a scalable surface activation process is presented for the breakdown of the passive oxide layer and the formation of nanowire/nanopyramid structured surfaces on metal substrates, which enables high-efficiency catalysis of high-crystallinity carbon nanotubes (CNTs) and the direct integration of the CNT-metal hierarchical architectures with flexible free-form configurations. The CNT-metal hierarchical architecture facilitates a dielectric free-energy-carrier transport pathway and blocks the reformation of passive oxide layer, and thus demonstrates a 5-fold decrease in interfacial electrical resistance with 66% increase in specific surface area compared with those without surface activation. Moreover, the CNT-metal hierarchical architectures demonstrate omnidirectional blackbody photoabsorption with the reflectance of 1 × 10-5 over the range from ultraviolet to terahertz region, which is 1 order of magnitude lower than that of any previously reported broadband absorber material. The synergistically incorporated CNT-metal hierarchical architectures offer record-high broadband optical absorption with excellent electrical and structural properties as well as industrial-scale producibility.

Low-Temperature Growth of Carbon Nanotubes Catalyzed by Sodium-Based Ingredients.

Synthesis of low-dimensional carbon nanomaterials such as carbon nanotubes (CNTs) is a key driver for achieving advances in energy storage, computing, and multifunctional composites, among other applications. Here, we report high-yield thermal chemical vapor deposition (CVD) synthesis of CNTs catalyzed by reagent-grade common sodium-containing compounds, including NaCl, NaHCO3 , Na2 CO3 , and NaOH, found in table salt, baking soda, and detergents, respectively. Coupled with an oxidative dehydrogenation reaction to crack acetylene at reduced temperatures, Na-based nanoparticles have been observed to catalyze CNT growth at temperatures below 400 °C. Ex situ and in situ transmission electron microscopy (TEM) reveal unique CNT morphologies and growth characteristics, including a vaporizing Na catalyst phenomenon that we leverage to create CNTs without residual catalyst particles for applications that require metal-free CNTs. Na is shown to synthesize CNTs on numerous substrates, and as the first alkali group metal catalyst demonstrated for CNT growth, holds great promise for expanding the understanding of nanocarbon synthesis.

Process-morphology scaling relations quantify self-organization in capillary densified nanofiber arrays.

Capillary-mediated densification is an inexpensive and versatile approach to tune the application-specific properties and packing morphology of bulk nanofiber (NF) arrays, such as aligned carbon nanotubes. While NF length governs elasto-capillary self-assembly, the geometry of cellular patterns formed by capillary densified NFs cannot be precisely predicted by existing theories. This originates from the recently quantified orders of magnitude lower than expected NF array effective axial elastic modulus (E), and here we show via parametric experimentation and modeling that E determines the width, area, and wall thickness of the resulting cellular pattern. Both experiments and models show that further tuning of the cellular pattern is possible by altering the NF-substrate adhesion strength, which could enable the broad use of this facile approach to predictably pattern NF arrays for high value applications.

Synthesis of subnanometer-diameter vertically aligned single-walled carbon nanotubes with copper-anchored cobalt catalysts.

We synthesize vertically aligned single-walled carbon nanotubes (VA-SWNTs) with subnanometer diameters on quartz (and SiO2/Si) substrates by alcohol CVD using Cu-anchored Co catalysts. The uniform VA-SWNTs with a nanotube diameter of 1 nm are synthesized at a CVD temperature of 800 °C and have a thickness of several tens of µm. The diameter of SWNTs was reduced to 0.75 nm at 650 °C with the G/D ratio maintained above 24. Scanning transmission electron microscopy energy-dispersive X-ray spectroscopy (EDS-STEM) and high angle annular dark field (HAADF-STEM) imaging of the Co/Cu bimetallic catalyst system showed that Co catalysts were captured and anchored by adjacent Cu nanoparticles, and thus were prevented from coalescing into a larger size, which contributed to the small diameter of SWNTs. The correlation between the catalyst size and the SWNT diameter was experimentally clarified. The subnanometer-diameter and high-quality SWNTs are expected to pave the way to replace silicon for next-generation optoelectronic and photovoltaic devices.

Structured Single-Walled Carbon Nanotubes and Graphene for Solar Cells.

We propose the concept of structured single-walled carbon nanotubes (SWNTs) for the applications of heterojunction solar cells and dye-sensitized solar cells (DSSCs). The structure of SWNTs was controlled and modified by a simple water vapor treatment, which was originally developed by our group. Compared with the graphene-Si solar cell and the SWNT-Si solar cell using the random-oriented SWNT film, the pristine micro-honeycomb structured SWNT-Si solar cell shows a significant improvement in terms of fill factor and the greater potential to obtain high power conversion efficiency (PCE). Moreover, the performance of the pristine micro-honeycomb structured SWNT-Si solar cells is stable in ambient condition. In addition, the PCE and fill factor of the DSSC with the micro-honeycomb structured SWNT counter electrode are 3.90% and 0.61, respectively, which are comparable to those of the DSSC with Pt as the counter electrode. This result shows that the micro-honeycomb networked SWNTs provide a low-cost alternative to replace Pt in DSSCs.

Direct and Dry Deposited Single-Walled Carbon Nanotube Films Doped with MoO(x) as Electron-Blocking Transparent Electrodes for Flexible Organic Solar Cells.

Organic solar cells have been regarded as a promising electrical energy source. Transparent and conductive carbon nanotube film offers an alternative to commonly used ITO in photovoltaics with superior flexibility. This communication reports carbon nanotube-based indium-free organic solar cells and their flexible application. Direct and dry deposited carbon nanotube film doped with MoO(x) functions as an electron-blocking transparent electrode, and its performance is enhanced further by overcoating with PEDOT: PSS. The single-walled carbon nanotube organic solar cell in this work shows a power conversion efficiency of 6.04%. This value is 83% of the leading ITO-based device performance (7.48%). Flexible application shows 3.91% efficiency and is capable of withstanding a severe cyclic flex test.