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: Scalable nanomanufacturing of chalcogenide inks: a case study on thermoelectric V–VI nanoplates
Solution-processed semiconducting main-group chalcogenides (MMCs) have attracted increasing research interest for next-generation device technologies owing to their unique nanostructures and superior properties. To achieve the full potential of MMCs, the development of highly universal, scalable, and sustainable synthesis and processing methods of chalcogenide particles is thus becoming progressively more important. Here we studied scalable factors for the synthesis of two-dimensional (2D) V–VI chalcogenide nanoplates (M 2 Q 3  : M = Sb, Bi; Q = Se, Te) and systematically investigated their colloidal behaviour and chemical stability. Based on a solvent engineering technique, we demonstrated scale-up syntheses of MMCs up to a 900% increase of batch size compared with conventional hydrazine-based gram-level syntheses, and such a scalable approach is highly applicable to various binary and ternary MMCs. Furthermore, we studied the stability of printable chalcogenide nanoparticle inks with several formulation factors including solvents, additives, and pH values, resulting in inks with high chemical stability (>4 months). As a proof of concept, we applied our solution-processed chalcogenide particles to multiple additive manufacturing methods, confirming the high printability and processability of MMC inks. The ability to combine the top-down designing freedom of additive manufacturing with bottom-up scalable synthesis of chalcogenide particles promises great opportunities for large-scale design and manufacturing of chalcogenide-based functional devices for broad application.  more » « less
Award ID(s):
1747685
PAR ID:
10298961
Author(s) / Creator(s):
; ; ; ; ; ; ;
Date Published:
Journal Name:
Journal of Materials Chemistry A
ISSN:
2050-7488
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Chalcogenide perovskites have garnered interest for applications in semiconductor devices due to their excellent predicted optoelectronic properties and stability. However, high synthesis temperatures have historically made these materials incompatible with the creation of photovoltaic devices. Here, we demonstrate the solution processed synthesis of luminescent BaZrS3and BaHfS3chalcogenide perovskite films using single‐phase molecular precursors at sulfurization temperatures of 575 °C and sulfurization times as short as one hour. These molecular precursor inks were synthesized using known carbon disulfide insertion chemistry to create Group 4 metal dithiocarbamates, and this chemistry was extended to create species, such as barium dithiocarboxylates, that have never been reported before. These findings, with added future research, have the potential to yield fully solution processed thin films of chalcogenide perovskites for various optoelectronic applications. 
    more » « less
  2. Abstract Flexible thermoelectric (TE) devices hold great promise for energy harvesting and cooling applications, with increasing significance to serve as perpetual power sources for flexible electronics and wearable devices. Despite unique and superior TE properties widely reported in nanocrystals, transforming these nanocrystals into flexible and functional forms remains a major challenge. Herein, demonstrated is a transformative 3D conformal aerosol jet printing and rapid photonic sintering process to print and sinter solution‐processed Bi2Te2.7Se0.3nanoplate inks onto virtually any flexible substrates. Within seconds of photonic sintering, the electrical conductivity of the printed film is dramatically improved from nonconductive to 2.7 × 104S m−1. The films demonstrate a room temperature power factor of 730 µW m−1K−2, which is among the highest values reported in flexible TE films. Additionally, the film shows negligible performance changes after 500 bending cycles. The highly scalable and low‐cost fabrication process paves the way for large‐scale manufacturing of flexible devices using a variety of high‐performing nanoparticle inks. 
    more » « less
  3. Abstract Printed 2D materials, derived from solution‐processed inks, offer scalable and cost‐effective routes to mechanically flexible optoelectronics. With micrometer‐scale control and broad processing latitude, aerosol‐jet printing (AJP) is of particular interest for all‐printed circuits and systems. Here, AJP is utilized to achieve ultrahigh‐responsivity photodetectors consisting of well‐aligned, percolating networks of semiconducting MoS2nanosheets and graphene electrodes on flexible polyimide substrates. Ultrathin (≈1.2 nm thick) and high‐aspect‐ratio (≈1 μm lateral size) MoS2nanosheets are obtained by electrochemical intercalation followed by megasonic atomization during AJP, which not only aerosolizes the inks but also further exfoliates the nanosheets. The incorporation of the high‐boiling‐point solvent terpineol into the MoS2ink is critical for achieving a highly aligned and flat thin‐film morphology following AJP as confirmed by grazing‐incidence wide‐angle X‐ray scattering and atomic force microscopy. Following AJP, curing is achieved with photonic annealing, which yields quasi‐ohmic contacts and photoactive channels with responsivities exceeding 103 A W−1that outperform previously reported all‐printed visible‐light photodetectors by over three orders of magnitude. Megasonic exfoliation coupled with properly designed AJP ink formulations enables the superlative optoelectronic properties of ultrathin MoS2nanosheets to be preserved and exploited for the scalable additive manufacturing of mechanically flexible optoelectronics. 
    more » « less
  4. Abstract Lightweight energy storage devices are essential for developing compact wearable and distributed electronics, and additive manufacturing offers a scalable, low‐cost approach to fabricating such devices with complex geometries. However, additive manufacturing of high‐performance, on‐demand energy storage devices remains challenging due to the need for stable, multifunctional nanomaterial inks. Herein, the development of 2‐dimensional (2D) titanium carbide (Ti3C2TxMXene) ink that is compatible with aerosol jet printing for energy storage applications is demonstrated. The developed MXene ink demonstrates long‐term chemical and physical stability, ensuring consistent printability and achieving high‐resolution prints (≈45 µm width lines) with minimal overspray. The high‐resolution aerosol‐jet printed MXene supercapacitor achieves an areal capacitance of 122 mF cm−2and a volumetric capacitance of 611 F cm−3, placing them among the highest‐performing printed supercapacitors reported to date. These findings highlight the potential of aerosol jet printing with MXene inks for on‐demand, scalable, and cost‐effective fabrication of printed electronic and electrochemical devices. 
    more » « less
  5. Colloidal nanoparticles have been widely studied and proven to have unique and superior properties compared to their bulk form and are attractive building blocks for diverse technologies, including energy conversion and storage, sensing, electronics, etc. However, transforming colloidal nanoparticles into functional devices while translating their unique properties from the nanoscale to the macroscale remains a major challenge. The development of advanced manufacturing methodologies that can convert functional nanomaterials into high-performance devices in a scalable, controllable and affordable manner presents great research opportunities and challenges for the next several decades. One promising approach to fabricate functional devices from nanoscale building blocks is additive manufacturing, such as 2D and 3D printing, owing to their capability of fast prototyping and versatile fabrication. Here, we review recent progress and methodologies for printing functional devices using colloidal nanoparticle inks with an emphasis on 2D nanomaterial-based inks. This review provides a comprehensive overview on four important and interconnected topics, including nanoparticle synthesis, ink formulation, printing methods, and device applications. New research opportunities as well as future directions are also discussed. 
    more » « less