Chronic inflammation has been identified as a major driver of joint degradation after injury. MRI is very limited to assess chronic inflammation with high specificity. Here we propose a novel contrast agent that targets the interaction of hyaluronan with RAMM cell receptors that represent an important signaling pathway for chronic inflammation. We validated the contrast agent with optical imaging and showed its value as an MRI contrast agent.
Contrast agents
P15-1 is a 15-mer peptide with homology to HA binding sequences of RHAMM10 that reduces inflammation in IL1β-stimulated chondrocytes. Based on its HA-binding capability and the increased levels of HA and HA-receptors in inflamed joint tissues, we anticipated that P15-1 will bind to the sites of active inflammation. We have developed two versions of the contrast agent. First, we conjugated a Cy5.5 fluorophore to the amino-terminal group of P15-1 for near infrared (NIR) imaging and histology validation. Second, we conjugated P15-1 to a Gd-DOTA chelating complex. In both cases, same spacer was used to increase distance between peptide and conjugation site.
Animal model
We induced OA in mature male Sprague-Dawley rats (14-16 weeks of age)11 by surgical transection of the anterior cruciate ligament (ACLT).12 Eight weeks after surgery, the rats generate moderate PTOA that was confirmed by histology.
Validation studies with optical imaging
Eight weeks after surgery, rats were intraarticularly injected with 10μg/50μl of Cy5.5-P15-1 tracer using an ultrasound guided injection setup (n=4 ACLT, n=4 Sham, n=4 control). To reduce self-fluorescence on the 680 nm band animals were on alfalfa-free diet for two weeks before imaging. Rats were positioned in the IVIS scanner using a custom designed device that holds the knee in flexed with 20 degrees of internal rotation allowing for a frontal view of the tibiofemoral space (Fig.1). NIR imaging was acquired before injection, 5 minutes after injection and 3, 6, 12, 24, 48 and 72 h after injection. Tissue localization of the NIR-tracers in the joint was analyzed by fluorescence microscopy in cryosections using the tape method,13 that preserves fluorophore functionality.
Validation studies with MRI
We used MRI to provide topographical information of the contrast agent distribution. We first calculated the change in relaxation rate of the contrast agent with Gd concentration (0 to 2mM) to determine an optimal dose. Then we injected both limbs of three rats intraarticularly with a combination of DOTA-Gd-P15-1 (1mM, half concentration used in humans) and Cy5.5-P15-1 (0.1mM). MRI protocol included an inversion recovery turbo-spin echo (IR-TSE) sequence (resolution=100×100×750 µm3, TE/TR=12.5/5343 ms, turbo-spin factor=5, echo spacing=6.25 s, inversion times(TI)=0.05,0.1,0.15,0.2,0.3,0.4,0.5,0.75,1,1.5,2,3,4,5 s, 8 slices, acquisition time=35 min/knee). All rats underwent bilateral knee MRI 24 h before injection, and 5, 24 and 48 h after injection on a Bruker 7T magnet using a 4-element receive surface coil. After the last imaging session, rats were sacrificed and limbs underwent fluorescence microscopy. T1 maps were calculated from the IR-TSE images and cartilage was segmented to calculate the average T1 value.
Validation studies with optical imaging
Our data shows that accumulation in ACLT limbs is higher than in control (Fig. 1) probing feasibility of the approach to track low-grade inflammation. ACLT joints showed increased retention of the contrast agent from 12 to 72 h after injection. Fluorescence microscopy showed accumulation on menisci and more predominantly in articular cartilage (Fig. 2). Interestingly, contrast agent accumulated primarily into chondrocytes, specially the ones in the deep cartilage layer. One limitation of NIR imaging is that it provides an overall measurement of contrast agent in the joint, including the fraction that is being eluted from the joint (Fig. 3).
Validation studies with MRI imaging
The relaxation rate (r1) of DOTA-Gd-P15-1 contrast agent was 2.82 mM-1s-1. T1 on an ACLT knee changed over time showing a clear decrease in T1 in the femoral trochlea and the patella (Fig 3). Average T1 values were increased in ACLT compared to control limbs. Over 48 hours T1 dropped in ACLT knee between -10% to -25% (-18% globally, Table 1) while it did not change in control groups (-2.7% globally). Contrast agent also accumulated in menisci and fat pad.