DIACETYLENES

Materials for time-temperature and radiation indicators


DIACETYLENES (DA): WHERE REACTIONS OCCUR IN THE SOLID STATE

A SEEING IS BELIEVING SYSTEM

Dr. GORDHAN PATEL IS ONE OF THE FEW PIONEERS

As movements of molecules are required, typically, chemical reactions occur in the gas or liquid states. There are only a small number of chemical reactions occur in the solid state. Diacetylenes are a unique class of solid compounds/monomers. They polymerize in the solid state to form highly colored (blue or red) polymers. A large number of reactions of diacetylenes and polydiacetylenes are associated with color changes and hence it is an ideal system for teaching polymer science (J. Chem. Ed. 60, 181 (1983)). Because of unique structural, electronic and optical properties, a large number of products such as biosensors and chemosensors, radiochromic dosimeters, smart inks, paints, and counterfeiting materials, nanostructures (nanotubes and nanowires), nonlinear optics, photocatalysis and pharmaceutical and organic synthesis are proposed in the literature.

Though the color development of diacetylenes is known since 1910, little attention was paid to them till Professor Gerhard Wagner of Germany showed that it is a topographic polymerization in the solid state. Ray Bachmann in Honeywell, Morris Twon, NJ/USA started exploring applications of diacetylenes in 1971. Dr. Patel Joined Dr. Baughman’s group in 1974 and he has been working on diacetylene since then. Dr. Patel has ~40 patents and ~40 research papers on diacetylenes. He pioneered development of a number of products based on diacetylenes, such as time-temperature indicators, radiation dosimeters, freeze indicators, thaw indicators and toxic chemical detectors. Products like time-temperature indicators and radiation monitoring devices are commercially available and the market has reached in hundreds of millions of dollars per year.

Dr. Patel has been working on diacetylenes since 1974 (50 years).
R-C≡C-C≡C-R
R is a substituent group
Most diacetylenes are solid.

SYNTHESIS & EXAMPLES OF SUBSTITUENT GROUPS OF DIACETYLENES

We have synthesized approximately 200 new DAs.

Updated synthesis scheme and examples of substituent groups of diacetylenes

Where Y is a substituted or unsubstituted aliphatic or aromatic functionality.
Where R is a substituent group.

DIACETYLENES – HISTORICAL

PIONEERS OF DIACETYLENES

Gerhard Wagner
Gerhard Wagner
Ray Baughman
Ray Baughman
Gordhan Patel
Gordhan Patel

POLYMERIZATION OF DIACETYLENES, R-C≡C-C≡C-R

MONOMERS: COLORLESS SOLID
POLYDIACETYLENES: COLORED (BLUE) OR (RED)

Diacetylene molecules are packed like steps of a ladder in their crystals.

Diagram of solid-state polymerization of diacetylenes upon radiation or heat, from white monomer to red or blue polymer
Examples of polydiacetylene crystals: powder and crystals grown from solution, with labels matched to their coloured brackets

LARGE CRYSTALS OF A DIACETYLENE (PTS, R=CH2-OSO2-Ph)

~0.1g to 1g crystals of PTS grown from solution by controlled slow evaporation of solvent

Large crystals of a diacetylene PTS

OPTICAL MICROGRAM OF CRYSTALS OF A DA

~1-micron thick crystals of a DA grown by cooling a from a polymer solution

Optical microgram of approximately one-micron thick diacetylene crystals

SCANNING ELECTRON MICROGRAM OF CRYSTALS OF A DA

Scanning electron microgram of diacetylene crystals

EXTREMITY OF POLYMER SINGAL CRYSTALS

Extremity of polymer single crystals

World’s largest polymer single crystal, ~4 mm dimeter ~10 cm long grown from melt by Zakroski method, polymerized by gamma ray


UNIQUE PROPERTIES OF DIACETYLENES

Seeing is believing: different chemical and physical reactions of diacetylenes
J. Chem. Ed. 60, 181 (1983)
Diagram of chemical and physical reactions of diacetylenes

OVERLAPPING OF THE pi-ORBITALS OF BACKBONES OF POLYDIACETYLENES

Diagram showing overlapping pi-orbitals of polydiacetylene backbones

MOLECULAR MODEL OF POLY4BCMU (R=(CH2)4-O-CO-NH-CH2-CO-O-(CH2)3-CH3)

Molecular model of Poly4BCMU
Schematic structures of polydiacetylene backbones in planar, compressed, stretched and interrupted forms

EFFECTIVE CONJUGATION AND COLOR OF PDA

Diagram relating effective conjugation and blue, red and yellow colour of polydiacetylene

EXTRACTION OF UNREACTED MONOMER & COLOR CHANGE

Diagram of extraction of unreacted monomer and color change

DA APPLICATIONS

Diacetylenes simultaneously respond to more than one parameters. E.g., Time, time-temperature, temperature, UV light, humidity, oxygen…

Diacetylenes don’t selectively respond to any one effect unless the other effects are blocked/minimized which is extremely difficult to do.

Diagram showing diacetylene response to temperature, time, time-temperature, UV or X-ray, environment, chemicals, vapour and pressure

INDICATORS FOR MONITORING SHELF LIFE OF PERISHABLES

United States Patent 3,999,946 for time-temperature history indicators

RADIATION DOSIMETERS

From the progress report of NIH/NCI SBIR phase I (1987/1988). The proposal was submitted in 1986.

Radiation dosimeter film colour scale by dose
Radiation dosimeter film colour scale by dose

200 KeV AND 10 MeV X-RAY IMAGES OF A PHANTOM ON A DIACETYLENE FILM

200 KeV and 10 MeV X-ray images of a phantom on diacetylene film

RADIATION THERAPY FILM

JP Labs pioneered the use of radiochromic film for monitoring radiation therapy (1987 - 1993) with funding from National Cancer Institute (USP #5,420,000). However, we were way ahead of our time and could not find a licensee or raise capital.

Scanned and digitized radiation therapy film

Calculator photographed on a SIRAD film, shown horizontally

AN IDEAL EMERGENCY DOSIMETER

Emergency dosimeter product image
Emergency dosimeter colour reference image

COLOR CHANGING FREEZE INDICATOR

Color changing freeze indicator showing blue before freezing and red after freezing

BLOOD RADIATION INDICATOR (BRI)

Blood radiation indicator label
Blood radiation indicator dose colour scale
Blood radiation indicator reference chart

HIGH DOSE DOSIMETERS

High dose dosimeter colour samples
High dose dosimeter colour samples and dose scale
High dose dosimeter dose colour panels

VVM (Vaccine Vial Monitors)

Vaccine vial monitors showing good and bad indicators