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Fig 1.

(A) Alignment of EF-hands of human secretagogin (SC) and the homologues calretinin (CR), reticulo calbin (RT) and calbindin (CB). The six EF-hands are labelled in different colors (red: EF1, dark red: EF2, green: EF3, pale green: EF4, cyan: EF5 and dark blue: EF6. Cysteines are boxed. (B) Crystal structure of secretagogin from Danio rerio (zebra fish), PDB ID: 2BE4. Six EF hands are colored as above. Cysteines are shown in orange, C193 is visible on the front surface, while C253 and C269 are on the back side. RT6: (X)13 = NYGEDLTKNHDEL.

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Fig 1 Expand

Fig 2.

Illustration of pairwise Cys-Cys distance in human secretagogin structure mapped on Dan rerio secretagogin X-ray structure, PDB ID: 2BE4.

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Fig 2 Expand

Fig 3.

SDS-PAGE analysis of secretagogin dimers.

(3A) Non-reducing gel of apo secretagogin. (3B) Non-reducing gel of calcium-loaded secretagogin. Lane 1 has pre stained protein ladder. Lanes 2–12 have 1 mg/mL secretagogin (30 μM) with 20 mM DTT, 10 mM DTT, 7 mM DTT, 5 mM DTT, 4 mM DTT, 3 mM DTT, 2 mM DTT, 1 mM DTT, 0.7 mM DTT (not present in 3B), 0.5 mM DTT and no DTT respectively. M = monomer; D = dimer; T = trimer (3C) Percent of monomer versus concentrations of DTT and dimer versus DTT concentration. Red: apo protein; blue: calcium-loaded protein; filled box: monomer; non-filled box: dimer.

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Fig 3 Expand

Fig 4.

Anti secretagogin Western blot analysis of recombinant secretagogin oligomers.

Non-reducing Western blot of apo secretagogin exposed for 2 min (4A) and 5 min (4B) with Pierce chemiluminescent Western blotting substrate. Lane 1–11 has 2 μg of 1 mg/mL purified secretagogin with 20 mM DTT, 10 mM DTT, 7 mM DTT, 5 mM DTT, 4 mM DTT, 3 mM DTT, 2 mM DTT, 1 mM DTT, 0.7 mM DTT, 0.5 mM DTT and no DTT respectively. M = monomer; D = dimer; T = trimer.

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Fig 4 Expand

Fig 5.

Anti secretagogin Western blot analysis of endogenous secretagogin in BRIN-BD11 insulinoma cell lysates at selected concentrations of DTT.

(5A) Non-reducing Western blot of native secretagogin exposed for 30 s with low sensitivity Pierce chemiluminescent Western blotting substrate (Thermo Scientific, cat. no. 32106). (5B) Non-reducing Western blot of native secretagogin exposed for 5 min with high sensitivity BM chemiluminescent Western blotting substrate (Roche, cat. no. 11500708001). Each lane has 30 μg of total protein with 20 mM DTT, 10 mM DTT, 5 mM DTT, 1 mM DTT, and no DTT respectively. M = monomer; D = dimer.

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Fig 5 Expand

Fig 6.

Lane 1: Apo secretagogin reduced in 20 mM DTT and dialyzed in glutathione redox buffer of -170 mV potential. Lane 2: Apo secretagogin reduced in 20 mM DTT.

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Fig 6 Expand

Fig 7.

Urea induced denaturation of secretagogin studied in non-reducing conditions (10 mM Tris, 0.15 M KCl [A, D] with 1 mM CaCl2 or 0.5 mM EDTA. pH: 7.5) and reducing conditions (10 mM Tris, 0.15 M KCl, 1mM [B, E] or 4 mM DTT [C, F] with 1 mM CaCl2 or 0.5 mM EDTA, pH: 7.5) using (7A) circular dichroism spectroscopy and (7B) fluorescence spectroscopy.

[Θ]222 nm is the ellipticity at 222 nm; λ is the wavelength; Panel A shows [Θ]222 nm versus λ as measured using CD spectroscopy and panel B shows fluorescence intensity versus λ as measured using fluorescent spectrometer.

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Fig 7 Expand

Fig 8.

Urea induced denaturation of secretagogin in non-reducing conditions (10 mM Tris, 0.15 M KCl [A, D] with 1 mM CaCl2 or 0.5 mM EDTA. pH: 7.5) and reducing conditions (10 mM Tris, 0.15 M KCl, 1mM [B, E] or 4 mM DTT [C, F] with 1 mM CaCl2 or 0.5 mM EDTA, pH: 7.5).

Blue and red curves represent calcium-loaded and apo form of secretagogin, respectively. [Θ]222 nm is the ellipticity at 222 nm; λ max is the wavelength at which the fluorescent intensity is highest; Cm is the urea concentration at the transition midpoint. In panels a-c are shown [Θ]222 nm versus urea concentration and in panels d-f λ max versus urea concentration.

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Fig 9.

Thermal stability of secretagogin as analyzed by circular dichroism spectroscopy when heated from 20 to 95°C in six buffers, A-F (Table 3).

[Θ]222 nm is ellipticity at 222 nm. Blue and pale blue dots represent calcium-loaded secretagogin under heating (20–95°C) and cooling (95–20°C), respectively. Red and pale red dots represent apo secretagogin under heating (20–95°C) and cooling (95–20°C), respectively. A. [Θ]222 nm versus temperature. B. Total absorbance (nm) versus temperature.

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Table 1.

Summary of apparent Tm and the real reversibility temperature range of secretagogin in various conditions studied.

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Table 1 Expand

Fig 10.

The reversibility ranges of secretagogin analyzed by circular dichroism spectroscopy.

Curves here represent temperature denaturation of both apo and calcium-loaded secretagogin during heating from 20–55°C and 20–65°C and from the maximum temperature to 20°C, for apo and calcium-loaded secretagogin at 0, 1 and 4 M urea and 0, 1 and 4 mM DTT. [Θ]222 nm is ellipticity at 222 nm. Blue and pale blue dots represent calcium-loaded secretagogin during heating from 20°C to test temperature and reverse scan to 20°C, respectively. Red and pale red dots represent apo secretagogin during heating from 20°C to test temperature and reverse scan to 20°C, respectively. (A) [Θ]222 nm versus temperature and total absorbance (nm) versus temperature at 20–55°C. (B) [Θ]222 nm versus temperature and total absorbance (nm) versus temperature obtained at 20–65°C.

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Fig 11.

Reversible denaturation curves of secretagogin analyzed by circular dichroism spectroscopy.

Secretagogin is tested for temperature reversible denaturation at different temperatures in six buffers, A-F (Table 3). The protein is heated up to the maximum temperature at each specific condition where it can refold. [Θ]222 nm is ellipticity at 222 nm. Blue and pale blue dots represent calcium-loaded secretagogin heated from 20°C to test temperature and reverse scan to 20°C, respectively. Red and pale red dots represent apo secretagogin heated from 20°C to test temperature and reverse scan to 20°C, respectively. A. [Θ]222 nm versus temperature. B. Total absorbance (nm) curves versus temperature.

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Fig 11 Expand

Fig 12.

Cartoon representing the free energy changes (ΔG) involved in folding and calcium binding of an EF-hand protein.

The total free energy change from its unfolded state to calcium-loaded state includes contributions from both folding and binding. Blue circles represent Ca2+ ions.

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Fig 13.

Comparison of Tm values of apo and calcium-loaded form of secretagogin and other calcium binding proteins.

Apo form of protein shown in red and calcium-loaded form in blue.

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Table 2.

Summary of melting temperatures of secretagogin and other calcium binding proteins.

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Table 2 Expand

Table 3.

Various buffer conditions used to study stability of secretagogin.

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Table 3 Expand