Figure 2. TIR multimerization and phase transition superactivates its intrinsic NAD + glycohydrolase activity.
(A) NADase activity of purified TIR at increasing TIR protein concentrations is shown. Activity was assessed by incubating TIR protein with 1 mM ε-NAD and monitoring the rate at which the fluorescent product ε-ADPR was produced. Curve represents a nonlinear regression fit of the NADase activity data points (n = 2). (B) NADase activity of 2.5 μM TIR incubated in the presence of 25% (w/v) of macro- (PEG 8000, PEG 3350, and dextran) and micro- (sucrose and glycerol) viscogens was assessed as described in A (n = 2). (C) Dose dependency of macroviscogens on the NADase activity of TIR is shown. A total of 2.5 μM TIR protein was incubated with the indicated PEG compounds at concentrations from 0% to 30% (w/v). NADase activity was assessed as described in A (n = 2). (D) Steady-state kinetic analysis of 2.5 µM TIR incubated in 0–30% (w/v) of PEG 3350 with the ε-NAD substrate at concentrations from 0 to 4000 μM was assessed as described in A. (n = 2). From the steady-state kinetic analysis performed in D, Km(E), kcat (F), and kcat/Km (G) were determined at each PEG 3350 concentration. (H) SDS-PAGE analysis of TIR protein fractions incubated with increasing concentrations of PEG 3350 precentrifugation (C) and after centrifugation, the soluble (S) and pellet (P) protein fractions. NADase activity of TIR protein in each fraction and at each concentration of PEG 3350 was assessed, as described in A, and is represented below the gel image (n = 2, representative image shown). (I) Steady-state kinetic analysis of TIR wild-type, oligomerization mutants (TIRG747P and TIRH833A), and catalytic mutants (TIRE788Q and TIRE788A) in 25% PEG 3350 with 0–2000 μM ε-NAD was assessed as described in D. The inset image outlined in red is an enlarged image of the mutant kinetic data. Kinetic parameters (Km, kcat, and kcat/Km) are shown in the table below the graph (n = 3). (J, K) SDS-PAGE analysis of TIR wild-type, oligomerization mutant (TIRG747P) and catalytic mutants (TIRE788Q and TIRE788A) precipitation in the presence of 25% PEG 3350. Gel represents the soluble (S) and pellet (P) protein fractions of wild-type and mutant TIR following incubation with PEG 3350 and centrifugation. TIRG747P and TIRE788Q were assessed with 10 μM protein in J, and TIRE788A was assessed with 3 μM protein in K (a lower concentration was used for TIRE788A assays because the yield of the purified TIRE788A mutant was low). Quantification of replicates represented below gel images (n = 4, representative images shown). *equals p < 0.05 by one-way ANOVA in J and unpaired t-test in K. (L) Effect of 1,6-hexanediol on TIR NADase activity is shown. TIR protein was incubated in the presence or absence of either 25% PEG 3350 or 500 mM citrate and treated with either 0 or 2% 1,6-hexanediol. The NADase activity of TIR for each condition was assessed using the ε-NAD substrate assay (n = 3). *equals p < 0.05 (unpaired t-test). (M) The NADase activity of TIR protein incubated with either 25% PEG 3350 or 500 mM citrate before (precentrifugation, n = 2) and after centrifugation, the supernatant (n = 4) and precipitant (n = 2) fractions. Precipitation fractions were resuspended in buffer alone or buffer containing 25% PEG 3350 or 500 mM citrate, and NADase activity was assessed. (N) Negative stain electron microscopy in either the absence or presence of 500 mM citrate (diameter of particles = 8.9 nm ± 1.2, n = 65). Representative circular particles are labeled with arrowheads. All error bars reflect SEM. See also Figure 2—figure supplements 1 and 2.