1. M.B. Agustin 1*, B. Ahmmad 2*, E.R. P. De Leon 1, J.L. Buenaobra 1, J.R. Salazar 1, and F. Hirose 2 1 Dept. of Chemistry, CAS, Central Luzon State University, Nueva Ecija, Philippines 2 Graduate School of Science and Engineering, Yamagata University, Yonezawa, Yamagata 992-8510, Japan

2.  Extreme versatility  Lighter weight  Resistance to chemicals, water and impact.  Better safety and hygiene properties for food packaging.  Excellent thermal and electrical insulation properties.  Relatively inexpensive to produce  Extreme durability

5.  Form of plastic derived from renewable biomass Polysaccharides Starch Cellulose Chitin Proteins Collagen/gelatin Silks, fibroin Casein, albumin Polyesters Polyhydroxyalkanoates Others Lignin Natural rubber Lipids Synthetic John and Thomas, 2008

6.  Starch is plasticized by thermomechanical treatment in the presence of water and a plasticizer like glycerol to produce thermoplastic starch (TPS). Starch offers the advantages of being cheap and naturally abundant. However, it suffers from having poor mechanical properties and being strongly hydrophilic.

7.  Common reinforcing fillers are clay, talc, silica, glass fiber, carbon black, natural fibers and cellulose micro/nanofibrils Natural fibers and cellulose nanofibrils inherent renewability, less abrasive character, biocompatibility, and low energy consumption for production

8.  a renewable, biodegradable and the most abundant organic biopolymer on the Earth  the primary structural component of the cell wall of higher plants and it can be obtained from various sources like wood, some bacteria, fungi and some algae.  cellulose content in different plants and trees varies significantly.  Cotton (90-99%)  Wood (40-50%)  Jute (60-70%)

10.  Crystalline cellulose  stronger and stiffer than amorphous cellulose and the native cellulose itself (Lin et al, 2008) Gray, D.G., 2011

11.  Coconut husk (Rosa et al., 2011)  Banana plant wastes (Ellanthikal, S. 2010)  Mulberry barks (Li, R. et al., 2009)  Palm pressed fiber (Wittaya, T, 2009)  Orange mesocarp (Ejikeme, P. 2008)  Baggase (Bhattacharya et al., 2008)  Wheat and cereal straws (Alemdar, A. and Sain, M. 2008)  Flax fibers and straw (Bochek, A.M. et al., 2003)  Soy bean husk (Nelson, Y. U. 2000),  Ground nut shell and rice husks (Okhamafe, A.O. et al., 1991)

13.  To isolate and characterize CNCs from garlic stalks  To prepare bioplastic films with varying amount of the isolated CNCs as reinforcing filler and starch as the biopolymer matrix  To evaluate the effect of CNCs in the morphological structure, mechanical properties, thermal stability and water resistance of the bioplastic films.

15. Sample collection and preparation Bleaching Cellulose fibers Delignification

16. Acid hydrolysisDialysis Characterization FTIR XRD SEM/TEM Sonication CNC suspension

17.  Solution casting method  Glycerol as plasticizer, water as solvent  Treatments: Starch: CNC ratio  T0 – 100:0  T1 – 100: 2.5  T2 – 100:5  T3 – 100: 10  T4 – 100: 15

18.  Tests done:  SEM  Mechanical properties  Thermogravimetric analysis  Moisture uptake

21. Peak Occurrence (cm -1 )Peak AssignmentReference 3442–OH stretching 2922–CH stretching 2364CO 2 Sherman Hsu, 1997 1639Adsorbed waterRosa et al., 2010 1426–CH deformationJonoobi et al., 2010 1377–CH asymmetric deformationJonoobi et al., 2010 1331–OH in plane deformationRosa et al., 2010 1227SulfatesMandal and Chakrabarty, 2011 1062 –COC pyranose ring skeletal vibration Chang et al., 2010 895Glucose ring stretchingJonoobi et al., 2010 830Half-ester sulfate groupChen, 2011 669–CH deformationRosa et al., 2010

22. SampleCI (%) Raw garlic stalks 35.6% Delignified garlic stalks53.1% CNC61.1%

23.  Approximate particle diameter using Semafore : 32 nm Cellulose nanocrystals Raw garlic stalks Cellulose fibers

25. T0: 100:0 T1: 100:2.5 T2: 100:5 T3: 100:10 T4: 100:15

27. TreatmentTensile Strength (MPa)Modulus (MPa) T0 (100:0) 10.0327.3 T1 (100:2.5)14.3416.2 T2 (100:5) 15.6439.6 T3 (100:10) 10.5392.5 T4 (100:15) 9.58349.98

29. Treatment% Moisture uptake T0 (100:0)17.0 T1 (100:2.5) 11.1 T2 (100:5)10.7 T3 (100:10)15.7 T4 (100:15)16.3

31.  Spherical cellulose nanocrystals with an average diameter of 35 nm and crystallinity of 62% can be isolated from garlic stalks through delignification and acid hydrolysis.  The starch to CNC ratio of 100:5 can be considered the optimum in this study. Improvement in tensile strength, modulus and moisture resistance of the film was the highest at this ratio.  Higher CNC load offset the reinforcing effect of CNC attributed to possible agglomeration of CNCs in the starch matrix.

32.  The authors gratefully acknowledge the financial support from the International Foundation for Science thru the research grant of M.B.Agustin.