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Nonribosomal peptide synthetases (NRPSs) can incorporate nonproteinogenic amino acids into peptidyl backbones to increase structural diversity. Genome mining of Schlegelella brevitalea led to the identification of a class of linear lipoheptapeptides, glidomides, featuring two unusual residues: threo-β-OH-L-His and threo-β-OH-D-Asp. The β-hydroxylation of Asp and His is catalyzed by the nonheme Fe

Asphalt pavement is inevitably exposed to sunlight and different water environment during the service life, and the environment changes have caused the asphalt to be aged under the more complex env...

The Burkholderia genus possesses ecological and metabolic diversities. A large number of silent biosynthetic gene clusters (BGCs) in the Burkholderia genome remain uncharacterized and represent a promising resource for new natural product discovery. However, exploitation of the metabolomic potential of Burkholderia is limited by the absence of efficient genetic manipulation tools. Here, we screened a bacteriophage recombinase system Redγ-BAS, which was functional for genome modification in the plant pathogen Burkholderia gladioli ATCC 10248. By using this recombineering tool, the constitutive promoters were precisely inserted in the genome, leading to activation of two silent nonribosomal peptide synthetase gene clusters (bgdd and hgdd) and production of corresponding new classes of lipopeptides, burriogladiodins A–H (1–8) and haereogladiodins A–B (9–10). Structure elucidation revealed an unnatural amino acid Z- dehydrobutyrine (Dhb) in 1–8 and an E-Dhb in 9–10. Notably, compounds 2–4 and 9 feature an unusual threonine tag that is longer than the predicted collinearity assembly lines. The structural diversity of burriogladiodins was derived from the relaxed substrate specificity of the fifth adenylation domain as well as chain termination conducted by water or threonine. The recombinase-mediating genome editing system is not only applicable in B. gladioli, but also possesses great potential for mining meaningful silent gene clusters from other Burkholderia species.

Nonribosomal peptide synthetases containing starter condensation domains direct the biosynthesis of nonribosomal lipopeptides, which generally exhibit wide bioactivities. The acyl chain has strong impacts on bioactivity and toxicity, but the lack of an in-depth understanding of starter condensation domain-mediated lipoinitiation limits the bioengineering of NRPSs to obtain novel derivatives with desired acyl chains. Here, we show that the acyl chains of the lipopeptides rhizomide, holrhizin, and glidobactin were modified by engineering the starter condensation domain, suggesting a workable approach to change the acyl chain. Based on the structure of the mutated starter condensation domain of rhizomide biosynthetic enzyme RzmA in complex with octanoyl-CoA and related point mutation experiments, we identify a set of residues responsible for the selectivity of substrate acyl chains and extend the acyl chains from acetyl to palmitoyl. Furthermore, we illustrate three possible conformational states of starter condensation domains during the reaction cycle of the lipoinitiation process. Our studies provide further insights into the mechanism of lipoinitiation and the engineering of nonribosomal peptide synthetases., Nonribosomal lipopeptides contain an acyl chain important for bioactivity, but its incorporation into the peptidyl backbone, mediated by the starter condensation (Cs) domain of nonribosomal peptide synthases, is not fully understood. Here, the authors show that acyl chains of different lengths can be obtained by engineering Cs domains and identify residues that determine the selectivity for acyl chains.

Phosphate type single alkyl oxygen base titanates TM-P was used to modify the surface of phosphorus slag powder in this paper. The surface characteristics and modification mechanism of phosphorus slag particles were characterized by using Scanning Electronic Microscopy (SEM). The effects and mechanism of the surface modified phosphorus slag powder to the asphalt and asphalt mixtures were analyzed by Fourier Transform Infrared Spectroscopy (FTIR), dynamic shear rheological test (DSR), Marshall test, rutting test and freeze-thaw splitting test. The results show that phosphorus slag powder modified by TM-P (10% by weight of the powder) enhance the compatibility with asphalt, resulting in the increase of anti-aging, rutting resistance and water damage resistance of asphalt mixture.

Styrene Butadiene Styrene (SBS) polymer-modified asphalt binders have become widely used in asphalt pavement because of their advantages in high- and low-temperature performance and fatigue resistance. Asphalt pavement is inevitably exposed to sunlight and ultraviolet (UV) radiation during its construction and service life. However, consideration of the aging effect of UV radiation is still limited in current pavement design and evaluation systems. In order to evaluate the impact of UV radiation on the aging properties of SBS-modified asphalt binders, UV aging tests were performed on Rolling Thin Film Oven Test (RTFOT)-aged samples with different UV radiation intensities and aging times. Sixteen different groups of tests were conducted to compare the rheological properties and functional group characteristics of SBS-modified asphalt binders. Dynamic Shear Rheometer (DSR), Bending Beam Rheometer (BBR), FTIR, and SEM tests were conducted to evaluate the aging mechanisms in various UV aging conditions. The results found that UV radiation seriously destroys the network structure formed by the cross-linking effect in SBS-modified asphalt binders, which aggravates the degradation of SBS and results in a great change of rheological properties after UV aging. The nature of SBS-modified asphalt binder aging resulted from the degradation of SBS and the changes of asphalt binder base composition, which lead to the transformation of colloidal structure and the deterioration of asphalt binder performance. The tests also found that continuous UV radiation can increase shrinkage stress in the asphalt binder surface and leads to surface cracking of the asphalt binder.

Bitumen aging can lead to the deterioration of asphalt pavement performance, shortening the service life of road. In order to solve the problem that current studies on the ultraviolet (UV) aging of bitumen either ignore the effects of natural environmental conditions or only consider the effects of water. In this study, different aqueous media and UV coupled simulated aging tests were carried out on virgin bitumen and styrene butadiene styrene (SBS) modified bitumen in a UV environment chamber. The combination of macroscopic performance tests and microstructure tests was used to analyze the physical, rheological, and microstructure changes of virgin bitumen and SBS modified bitumen after The film oven test (TFOT) aging and UV aging in different environments (UV, UV + Water, UV + Acid, UV + Salt). Dynamic shear rheometer (DSR) results indicated that UV aging results in the increase of rutting factor and the improvement of rutting resistance at high temperature. The Fourier transform infrared spectrum (FTIR) results illustrated that the bitumen would be oxidized and SBS would be degraded under ultraviolet radiation. The four-component analysis test results showed that light component migrated to the heavy component during the aging process. Moreover, water will aggravate the UV aging of bitumen, and the presence of acid or salt worsens ultraviolet aging.