skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Laser Photoreduction of Graphene Aerogel Microfibers: Dynamic Electrical and Thermal Behaviors
Abstract This work reports the dynamic behaviors of graphene aerogel (GA) microfibers during and after continuous wave (CW) laser photoreduction. The reduction results in one‐order of magnitude increase in the electrical conductivity. The experimental results reveal the exact mechanisms of photoreduction as it occurs: immediate photochemical removal of oxygen functional groups causing a sharp decrease in electrical resistance and subsequent laser heating that facilitates thermal rearrangement of GO sheets towards more graphene‐like domains. X‐ray and Raman spectroscopy analysis confirm that photoreduction removes virtually all oxygen and nitrogen containing functional groups. Interestingly, a dynamic period immediately following the end of laser exposure shows a slow, gradual increase in electrical resistance, suggesting that a proportion of the electrical conductivity enhancement from photoreduction is not permanent. A two‐part experiment monitoring the resistance changes in real‐time before and after photoreduction is conducted to investigate this critical period. The thermal diffusivity evolution of the microfiber is tracked and shows an improvement of 277 % after all photoreduction experiments. A strong linear coherency between thermal diffusivity and electrical conductivity is also uncovered. This is the first known work to explore both the dynamic electrical and thermal evolution of a GO‐based aerogel during and after photoreduction.  more » « less
Award ID(s):
2032464 1930866
PAR ID:
10419350
Author(s) / Creator(s):
 ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
ChemPhysChem
Volume:
23
Issue:
23
ISSN:
1439-4235
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. null (Ed.)
    Laser photoreduction of metal ions onto graphene oxide (GO) is a facile, environmentally friendly method to produce functional metal–GO nanocomposites for a variety of applications. This work compares Au–GO nanocomposites prepared by photoreduction of [AuCl 4 ] − in aqueous GO solution using laser pulses of nanosecond (ns) and femtosecond (fs) duration. The presence of GO significantly accelerates the [AuCl 4 ] − photoreduction rate, with a more pronounced effect using ns laser pulses. This difference is rationalized in terms of the stronger interaction of the 532 nm laser wavelength and long pulse duration with the GO. Both the ns and fs lasers produce significant yields of sub-4 nm Au nanoparticles attached to GO, albeit with different size distributions: a broad 5.8 ± 1.9 nm distribution for the ns laser and two distinct distributions of 3.5 ± 0.8 and 10.1 ± 1.4 nm for the fs laser. Despite these differences, both Au–GO nanocomposites had the same high catalytic activity towards p -nitrophenol reduction as compared to unsupported 4–5 nm Au nanoparticles. These results point to the key role of GO photoexcitation in catalyzing metal ion reduction and indicate that both ns and fs lasers are suitable for producing functional metal–GO nanocomposites. 
    more » « less
  2. Solution-phase printing of exfoliated graphene flakes is emerging as a low-cost means to create flexible electronics for numerous applications. The electrical conductivity and electrochemical reactivity of printed graphene has been shown to improve with post-print processing methods such as thermal, photonic, and laser annealing. However, to date no reports have shown the manipulation of surface wettability via post-print processing of printed graphene. Herein, we demonstrate how the energy density of a direct-pulsed laser writing (DPLW) technique can be varied to tune the hydrophobicity and electrical conductivity of the inkjet-printed graphene (IPG). Experimental results demonstrate that the DPLW process can convert the IPG surface from one that is initially hydrophilic (contact angle ∼47.7°) and electrically resistive (sheet resistance ∼21 MΩ □ −1 ) to one that is superhydrophobic (CA ∼157.2°) and electrically conductive (sheet resistance ∼1.1 kΩ □ −1 ). Molecular dynamic (MD) simulations reveal that both the nanoscale graphene flake orientation and surface chemistry of the IPG after DPLW processing induce these changes in surface wettability. Moreover, DPLW can be performed with IPG printed on thermally and chemically sensitive substrates such as flexible paper and polymers. Hence, the developed, flexible IPG electrodes treated with DPLW could be useful for a wide range of applications such as self-cleaning, wearable, or washable electronics. 
    more » « less
  3. Abstract Smart materials are versatile material systems which exhibit a measurable response to external stimuli. Recently, smart material systems have been developed which incorporate graphene in order to share on its various advantageous properties, such as mechanical strength, electrical conductivity, and thermal conductivity as well as to achieve unique stimuli‐dependent responses. Here, a graphene fiber‐based smart material that exhibits reversible electrical conductivity switching at a relatively low temperature (60 °C), is reported. Using molecular dynamics (MD) simulation and density functional theory‐based non‐equilibrium Green's function (DFT‐NEGF) approach, it is revealed that this thermo‐response behavior is due to the change in configuration of amphiphilic triblock dispersant molecules occurring in the graphene fiber during heating or cooling. These conformational changes alter the total number of graphene‐graphene contacts within the composite material system, and thus the electrical conductivity as well. Additionally, this graphene fiber fabrication approach uses a scalable, facile, water‐based method, that makes it easy to modify material composition ratios. In all, this work represents an important step forward to enable complete functional tuning of graphene‐based smart materials at the nanoscale while increasing commercialization viability. 
    more » « less
  4. Traditional manufacturing methods restrict the expansion of thermoelectric technology. Here, we demonstrate a new manufacturing approach for thermoelectric materials. Selective laser melting, an additive manufacturing technique, is performed on loose thermoelectric powders for the first time. Layer-by-layer construction is realized with bismuth telluride, Bi 2 Te 3 , and an 88% relative density was achieved. Scanning electron microscopy results suggest good fusion between each layer although multiple pores exist within the melted region. X-ray diffraction results confirm that the Bi 2 Te 3 crystal structure is preserved after laser melting. Temperature-dependent absolute Seebeck coefficient, electrical conductivity, specific heat, thermal diffusivity, thermal conductivity, and dimensionless thermoelectric figure of merit ZT are characterized up to 500 °C, and the bulk thermoelectric material produced by this technique has comparable thermoelectric and electrical properties to those fabricated from traditional methods. The method shown here may be applicable to other thermoelectric materials and offers a novel manufacturing approach for thermoelectric devices. 
    more » « less
  5. This study investigated the influence of diverse laser processing parameters on the thermophysical properties of Ti-6Al-4V and AlSi10Mg alloys manufactured via laser powder bed fusion. During fabrication, the laser power (50 W, 75 W, 100 W) and laser scanning speed (0.2 m/s, 0.4 m/s, 0.6 m/s) were adjusted while keeping other processing parameters constant. Besides laser processing parameters, this study also explored the impact of test temperatures on the thermophysical properties of the alloys. It was found that the thermophysical properties of L-PBF Ti-6Al-4V alloy samples were sensitive to laser processing parameters, while L-PBF AlSi10Mg alloy showed less sensitivity. In general, for the L-PBF Ti-6Al-4V alloy, as the laser power increased and laser scan speed decreased, both thermal diffusivity and conductivity increased. Both L-PBF Ti-6Al-4V and L-PBF AlSi10Mg alloys demonstrated similar dependence on test temperatures, with thermal diffusivity and conductivity increasing as the test temperature rose. The CALPHAD software Thermo-Calc (2023b), applied in Scheil Solidification Mode, was utilized to calculate the quantity of solution atoms, thus enhancing our understanding of observed thermal conductivity variations. A detailed analysis revealed how variations in laser processing parameters and test temperatures significantly influence the alloy’s resulting density, specific heat, thermal diffusivity, and thermal conductivity. This research not only highlights the importance of processing parameters but also enriches comprehension of the mechanisms influencing these effects in the domain of laser powder bed fusion. 
    more » « less