Biodegradable polymers, such as polycaprolactone (PCL), are promising materials in the field of tissue engineering and regenerative medicine, which aims at creating viable options to replace permanent orthopedic implants. The material, cells, and growth-stimulating factors are often referred to as the key components of engineered tissues. In this article, we studied the hypothesis of specific surface modification of PCL being capable of inducing mesenchymal stem cell differentiation in bone cells in the absence of cell-differentiating factors. The systematic investigation of the linearly varying surface-roughness gradient showed that an average PCL roughness of 0.93 μm alone can serve as a compelling alternative to soluble osteogenic inducers in orthopedic applications featuring the clinically relevant biodegradable polymer polycaprolactone.
Chain-density gradients of poly(l-lysine)-graft-dextran (PLL-g-dex), a synthetic comblike copolymer with a poly(l-lysine) backbone grafted with dextran side chains, were fabricated on an oxidized silicon substrate. The influence of the changing dextran chain density along the gradient on the local coefficient of friction was investigated via colloidal-probe lateral force microscopy. Both in composition and structure, PLL-g-dex shares many similarities with bottlebrush biomolecules present in natural lubricating systems, while having the advantage of being well-characterized in terms of both architecture and adsorption behavior on negatively charged oxide surfaces. The results indicate that the transition of the dextran chain density from the mushroom into the brush regime coincides with a sharp reduction in friction at low loads. Above a critical load, the friction increases by more than an order of magnitude, likely signaling a pressure-induced change in the brush conformation at the contact area and a corresponding change in the mechanism of sliding. The onset of this higher-friction regime is moved to higher loads as the chain density of the film is increased. While in the low-load (and low-friction) regime, increased chain density leads to lower friction, in the high-load (high-friction) regime, increased chain density was found to lead to higher friction.
The success of synthetic bone implants requires good interface between the material and the host tissue. To study the biological relevance of fibronectin (FN) density on the osteogenic commitment of human bone marrow mesenchymal stem cells (hBM-MSCs), human FN was adsorbed in a linear density gradient on the surface of PCL. The evolution of the osteogenic markers alkaline phosphatase and collagen 1 alpha 1 was monitored by immunohistochemistry, and the cytoskeletal organization and the cell-derived FN were assessed. The functional analysis of the gradient revealed that the lower FN-density elicited stronger osteogenic expression and higher cytoskeleton spreading, hallmarks of the stem cell commitment to the osteoblastic lineage. The identification of the optimal FN density regime for the osteogenic commitment of hBM-MSCs presents a simple and versatile strategy to significantly enhance the surface properties of polycaprolactone as a paradigm for other synthetic polymers intended for bone-related applications.
The impact of brush-like structure and disorder on the lubricating ability of dextran chains at low and high loads has been investigated by means of AFM.
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