*Article* **Composite of Layered Double Hydroxide with Casein and Carboxymethylcellulose as a White Pigment for Food Application**

**Estee Ngew, Wut Hmone Phue, Ziruo Liu and Saji George \***

> Department of Food Science and Agricultural Chemistry, McGill University, Sainte-Anne-de-Bellevue, QC H9X 3V9, Canada; estee.ngew@mail.mcgill.ca (E.N.); wut.phue@mail.mcgill.ca (W.H.P.); ziruo.liu@mail.mcgill.ca (Z.L.) **\*** Correspondence: saji.george@mcgill.ca

**Abstract:** Titanium dioxide (TiO2) is commonly used in food, cosmetic, and pharmaceutical industries as a white pigment due to its extraordinary light scattering properties and high refractive index. However, as evidenced from recent reports, there are overriding concerns about the safety of nanoparticles of TiO2. As an alternative to TiO2, Mg-Al layered double hydroxide (LDH) and their composite containing casein and carboxymethyl cellulose (CMC) were synthesized using wet chemistry and compared with currently used materials (food grade TiO2 (E171), rice starch, and silicon dioxide (E551)) for its potential application as a white pigment. These particles were characterized for their size and shape (Transmission Electron Microscopy), crystallographic structure (X-Ray Diffraction), agglomeration behavior and surface charge (Dynamic Light Scattering), surface chemistry (Fourier Transform Infrared Spectroscopy), transmittance (UV–VIS spectroscopy), masking power, and cytotoxicity. Our results showed the formation of typical layered double hydroxide with flower-like morphology which was restructured into pseudo-spheres after casein intercalation. Transmittance measurement showed that LDH composites had better performance than pristine LDH, and the aqueous suspension was heat and pH resistant. While its masking power was not on a par with E171, the composite of LDH was superior to current alternatives such as rice starch and E551. Sustainability score obtained by MATLAB® based comparison for price, safety, and performance showed that LDH composite was better than any of the compared materials, highlighting its potential as a white pigment for applications in food.

**Keywords:** white pigment; E171 alternative; layered double hydroxides; casein; carboxymethyl cellulose; sustainability index
