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Fig 1.

Expression and purification of fusion Aβ(E3Q-42) protein in E. coli BL21 (DE3) pLysS.

(a) 15% Tris/Glycine-SDS-PAGE analysis of the lysates before IPTG induction (t = 0 h) and after IPTG induction leading to expression of fusion Aβ(E3Q-42) (t = 16 h after induction) at 30°C. (b) Analytical RP-HPLC of IMAC purified fusion Aβ(E3Q-40) (red) and fusion Aβ(E3Q-42) (black) with typical retention times of 5 and 7 min, respectively. (c) 15% Tris/Glycine-SDS-PAGE of IMAC and RP-HPLC purified fusion Aβ(E3Q-42).

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Fig 1 Expand

Table 1.

Yields of intermediates and final purified pEAβ peptides in mg per l culture broth.

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Table 1 Expand

Fig 2.

Analytical RP-HPLC of TEV protease cleavage reaction of Aβ(E3Q-40) (a) and Aβ(E3Q-42) (b).

The peptides were applied on an analytical Zorbax SB-300 C8 column and eluted with 30% ACN and 0.1% TFA at 80°C. Black lines indicate analysis after 0.5 h and red lines after 7 h TEV cleavage reaction at 4°C. Peaks for the fusion proteins decreased while peaks indicating cleaved Aβ(E3Q-40) or Aβ(E3Q-42) were increasing. (c) Semi-preparative RP-HPLC of TEV-cleaved fusion Aβ(E3Q-40) to separate Aβ(E3Q-40) from remaining fusion protein.

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Fig 2 Expand

Fig 3.

Non-enzymatic pyroglutamate (pE) formation by acidic and elevated temperature conditions of Aβ(E3Q-40) (a), Aβ(E3Q-42) (b) and wild type Aβ(3–40) (c).

Peptides were incubated at 45°C in sodium acetate buffer pH 3.5 for 24 h. Conversion was observed by analytical RP-HPLC with an analytical Zorbax SB-300 C8 column in 30% ACN/ 0.1% TFA at 80°C. Peaks for non-modified peptides decreased while peaks for the pEAβ variants appeared at a longer retention time. (d) Reaction scheme of the conversion of N-terminal E3 or N-terminal Q3 to pE. (e) Mass spectrometry of [U-15N]Aβ(E3Q-40) compared to N-terminally modified [U-15N]pEAβ40. Molecular mass of the peptides differs in 18 Da due to the loss of the 15NH3 group.

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Fig 3 Expand

Fig 4.

Analytics of final purified pEAβ.

Analytical RP-HPLC of pEAβ40 (a) and pEAβ42 (b) after final purification and corresponding analysis of the proteins by Tris/Tricine-SDS-PAGE (c). The characteristic RP-HPLC retention times are approximately 9.5 min for pEAβ40 and 15 min for pEAβ42.

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Fig 5.

ThT assay of 10 μM recombinant pEAβ40 and pEAβ42.

Experiments were performed in 10 mM sodium phosphate buffer pH 7.4 at 37°C. Binding of ThT (10 μM final concentration) to Aβ fibrils was determined by fluorescence at an extinction of 440 nm and emission at 492 nm.

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Fig 6.

1H,15N-HSQC spectra of Aβ(E3Q-40) (blue) and pEAβ40 (red) (a) or of pEAβ42 (b).

NMR spectra were recorded from 25 μM protein samples solved in 10 mM sodium phosphate buffer pH 7.4 at 5°C on a 600 MHz Bruker spectrometer. Note that in (a) “blue” signals derived from Aβ(E3Q-40) are overlaid with “red” signals from pEAβ40. Therefore “blue” signals are not visible, if identical in shift and intensity to “red” signals.

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Fig 6 Expand