Electron-induced rapid crosslinking in supramolecular metal-peptide assembly and chemically responsive disaggregation for catalytic application

doi:10.1016/S1872-2067(20)63655-5

Abstract

Abstract:

The applications of supramolecular metal-peptide assemblies as catalyst or catalyst precursor have recent attracted increasing attentions. In this work,a fragment of the amyloid β-peptide,NH2-KLVFF-COOH,was assembled into nanofilms with encapsulated Pd,Pt and Au nanoparticles (NPs) via a one-step room temperature electron induction method. The effects of building block,intermolecular interaction,driving force and side-chain on the assembly were investigated. The assembly mechanism was thereby proposed. The crosslinking of peptide monomers results in mainly random and unordered structures. The obtained metal-peptide assemblies are extremely stable in water at neutral pH for long term. However,the metal NPs are able to be responsively released under basic and reductive conditions. The released NPs show a high activity to catalyze the reduction of 4-nitrophenol. The present studies on assembly mechanism and responsive release will be helpful for the design of organic skeletons and also for the future development of peptide stabilized metallic NPs with applications beyond catalysts.

Key words: Metal, Peptide, Assembly, Responsive release, Reduction, Catalyst

Zongyuan Wang, Jiajun Wang, Zeyu Sun, Wenlong Xiang, Chenyang Shen, Ning Rui, Mingzhu Ding, Yingjin Yuan, Honggang Cui, Chang-jun Liu. Electron-induced rapid crosslinking in supramolecular metal-peptide assembly and chemically responsive disaggregation for catalytic application[J]. Chinese Journal of Catalysis, 2021, 42(3): 376-387.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63655-5

https://www.cjcatal.com/EN/Y2021/V42/I3/376

Figures/Tables 8

Fig.1. Schematic synthesis and SEM images of the metal-peptide nanofilms. (a) The digital photos of Pd0.5-P0.5 nanofilm product; (b-d) the SEM images and digital photos (insets of b-d) of Pd0.5-P0.5 (b),Pt0.5-P0.5 (c) and Au0.01-P0.2 (d) nanofilms.

Fig.2. TEM images and metal distributions of metal-peptide nanofilms: Pd0.5-P0.5 (a-c),Pt0.5-P0.5 (d-f) and Au0.01-P0.2 (g-i); the insets in (b,e,h) show the distances of crystal facets; (c),(f) and (i) are the statistical result of particle size.

Fig.3. (a) The XRD patterns of pure KLVFF,Pd0.5-P0.5,Pt0.5-P0.5,Au0.01-P0.2 and Au0.1-P0.5 samples; (b-d) the XPS spectra of Pd 3d,Pt 4f and Au 4f.

Fig.4. The AFM images of Pd0.5-P0.5 nanofilms. AFM height (a,b) and phase (c) scanning images; (d,e) the height of the red-line and blue-line section in a and b,respectively; (f) schematic illustration of peptide nanofilms encapsulating metal NPs; (g) approximate geometric length of KLVFF estimated by Materials Studio.

Fig.5. The FTIR and XPS analysis of the electron‐induced assembly process. The FTIR spectra of KLVFF powders (a) and Pd‐P films (b,c) under different conditions; (b) change the Pd ion concentration from 0 to 0.5 mM; (c) change the reaction time from 0 to 10 min; (d-g) The XPS spectra of KLVFF before and after assembly.

Fig.6. The DFT calculatation of the C-H hydroxylation process and 1H-NMR results of KLVFF peptide before and after the electron-induced assembly. (a) The classify of C-H bonds in KLVFF molecule; Potential energy surface of C-H hydroxylation to C-OH through single OH radical S route (b) and double OH radical D route (c). IC,initial complex; TS1,transition state for H-abstraction; TS2-S,transition state for HOH-rebound in S route; INT,intermediate; INT-D,intermediate in D route; FC-S and FC-D,final complex. (d) The 1H-NMR results of KLVFF peptide and M0-P0.5 nanofilms tested in DMSO-d6 with and without D2O.

Fig.7. Schematic illustration of the electron-induced assembly,long-term storage of metal-peptide nanofilms and their responsive release under NaBH4 and glutathione (GSH) conditions.

Fig.8. Catalytic performance of noble-metal-peptide nanofilms. UV-vis absorption spectra and the plot of C/C0 (a,c,e) and ln(C/C0) (b,d,f) versus reaction time during the catalytic reduction of 4-NP over NaBH4 treated Pd0.5-P0.5 (a,d),Pt0.5-P0.5 (b,e) and Au0.01-P0.2 (c,f) samples. Initial curves at 0 s were obtained by adding NaBH4 into 4-NP solution.

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