Atomically thin gold embedded in inkjet-printed PVA hydrogels: flexible catalysts for ambient phenol degradation

Inkjet-printed gold nanotape (AuNTp) structures embedded in polyvinyl alcohol (PVA) hydrogels provide a reusable, high-surface-area platform for catalytic degradation of phenol and 4-nitrophenol (4-NP) under ambient conditions. AuNTps, featuring distinct three-dimensional "heads" and atomically thin quasi-one-dimensional "tails", enhanced catalytic activity in both reduction and oxidation reactions. Compared to spherical gold nanoparticles (AuNPs), AuNTps are nearly twice as catalytically efficient for 4-NP reduction on a per-mass basis, reflecting the influence of anisotropic morphology on surface-sensitive electron transfer. In contrast, phenol oxidation shows weaker morphology dependence, likely proceeding through hydroxyl radical-mediated pathways that are less sensitive to catalyst shape or facet structure. To enable rapid substrate diffusion and facilitate reuse, AuNTps were formulated into PVA inks and inkjet-printed into micrometre-thick hydrogel mesh architectures (8 to 15 µm thick). Although printed meshes show reduced activity relative to free AuNTps in solution, they achieve a nearly fourfold increase in mass-normalised rate constants for 4-NP reduction compared to drop-cast gels (0.24 × 10⁴ <i>vs.</i> 0.07 × 10⁴ min^-1 g^-1) and achieve 26% phenol, a common water pollutant, in 4 hours at room temperature, with consistent performance over multiple cycles. These findings demonstrate the potential of inkjet-printed nanozyme hydrogels as scalable, heterogeneous catalysts. Further improvements may be achieved by optimising catalyst-matrix interactions to reduce diffusion and accessibility barriers. This work addresses a significant challenge in nanozyme catalysis: translating high-performance nanomaterials into practical, reusable formats suitable for environmental remediation.