Thermoplastic
blends are applied for three-dimensional (3D) printing
to obtain improved functionality. While thermal, chemical, and mechanical
properties of 3D-printed blends are typically examined, biodegradability
of the 3D-printed plastics has rarely been the focus of research.
In this study, we evaluated the biodegradation behavior of 3D-printed
prototypes fabricated from various plastics and blends, including
biodegradable polylactic acid (PLA), poly(3-hydroxybutyrate) (PHB),
non-biodegradable high-density polyethylene (HDPE), and polypropylene
(PP). Letter-shaped specimens were prototyped using a fused deposition
modeling (FDM) printer with various filaments (PLA, PHB, HDPE, PP,
PLA/HDPE, PLA/PP, PHB/HDPE, PHB/PP, and PLA/PHB), and their printing
performance and optimal printing conditions were evaluated. FDM 3D
printing of HDPE and PP has been problematic due to poor adhesion,
warping deformation, and crystallization-induced volume contraction.
We demonstrate that PLA/HDPE and PLA/PP blends are printable, and
PLA/PHB blends exhibit outstanding printing performance. Biodegradation
tests on 3D-printed prototypes were performed employing a systematically
designed respirometer by simulating (i) controlled composting and
(ii) the aerobic aqueous environment. Neat PHB and PLA/PHB blends
(50:50 wt %) showed significant biodegradation in controlled composting
and an aerobic aqueous test (86.4, 85.0% and 73.3, 32.3%, respectively)
in 50 days, while biodegradable/non-biodegradable blends (PLA/HDPE,
PLA/PP, PHB/HDPE, and PHB/PP) were barely biodegraded. The immiscible
biodegradable/non-biodegradable plastic blends revealed evidence of
partial degradation and even antagonism to biodegradation, most likely
due to phase separation and the barrier effect. Taken together, although
PLA/HDPE and PLA/PP blends exhibited resistance to biodegradation,
the low-cost polyolefins (HDPE and PP) as well as some notable improvements
in mechanical properties render them promising FDM 3D printing resources.
On the other hand, the outstanding printing performance, improved
Young’s modulus, and synergetic biodegradation behavior indicate
that the PLA/PHB blend can be an excellent fit for sustainable FDM
printing resources.