Three-Dimensional Chiral Supramolecular Microenvironment Strategy for Enhanced Biocatalysis

Abstract

How the three-dimensional (3D) chiral environment affects the biocatalysis remains an important issue, thereby inspiring the development of a microenvironment that highly mimics the natural features of enzyme to guarantee enhanced biocatalysis. In this study, two gelators bearing d/l-phenylalanine as chiral centers are designed to construct the 3D chiral catalytic microenvironment for enhancing the biocatalysis of lipase. Such a microenvironment is programmed through chiral transmission of chirality from molecular chirality to achiral polymers. It shows that the chirality of the microenvironment evidently influences the catalytic efficiency of immobilized lipase inside the system, and the 3D microenvironment constructed by right-handed helical nanostructures can enhance the catalytic activity of lipase inside as high as 10-fold for catalyzing 4-nitrophenyl palmitate (NPP) to 4-nitrophenol (NP) and 1.4-fold for catalyzing lipids to triglycerides (TGs) in 3T3-L1 cells than that of the achiral microenvironment. Moreover, the 3D chiral microenvironment has the merits of good catalytic efficiency, high storage stability, and efficient recyclability. This strategy of designing a 3D chiral microenvironment suitable for biocatalysis will overcome the present limitations of enzymatic immobilization in traditional materials and enhance the understanding of biocatalysis.

Naturally flavonoid-derived PVA nanofibers for antioxidation

“…During the freezing of PVA–SA solution, ice formed in the amorphous region induced the growth of PVA polymer crystallites, which act as nodule points of the network and promote the formation of hydrophobic fibers. 33 The produced PVA–SA fibers were uniform without any beads but showed minor defects (Fig. 1A).…”

3D Chiral Self‐Assembling Matrixes for Regulating Polarization of Macrophages and Enhance Repair of Myocardial Infarction

“…These high‐aspect‐ratio nanofibers template through hydrogen bonding along the long axis of nanofibers and further physically entangle to self‐supportive 3D hydrogels networks by a supramolecular gelation process (Scheme 1A). [ 18 ] The critical gel concentration (CGC) for L ‐BA, D ‐BA, and R ‐BA is 1.0 wt.%, and hydrogel formation was judged by the conventional tube inversion method (Figure S7 and Table S1, Supporting Information). The water content of these three hydrogels was measured by the method of drying and weighing was almost above 98% (Figure S8A, Supporting Information).…”

“…The M ‐type and P ‐type hydrogels showed the absorptive dissymmetry factor g abs , which is defined by the ratio of CD intensity to the corresponding absorption (shown in Supporting Information), were approximately equal in intensity and handedness opposite in chirality (Figure 1F), which indicated that the molecular chirality of the gelators is well transferred to the supramolecular chirality. [ 14,18 ] With the increasing testing temperature, the intensity of the CD signals for both M ‐type and P ‐type self‐assembling hydrogels gradually decreased due to disassembly by heating. At ≈95 °C, the CD signals at 230 and 306 nm both almost disappeared suggesting the disintegration of M ‐type and P ‐type self‐assembled nanofibers, respectively.…”

Herb‐Functionalized Chronic Wound Dressings for Enhancing Biological Functions: Multiple Flavonoids Coordination Driven Strategy

“…During freezing of the solution, the ice created in the amorphous region induced the growth of polymer crystallites, acting as junction knots of the network and enhancing mechanical strength of hydrogel. [ 39 ] CD spectra were measured and compared to investigate the interactions of the hydrogels (Figure 1i). CFPL hydrogel (CS + PVA + LBF) showed negative peaks at ≈227 and 256 nm and positive CD absorptions at ≈206 and 288 nm, while the mirror‐imaged CD spectrum of CFPD hydrogel (CS + PVA + DBF) exhibited three positive bands (204, 226, and 260 nm) and two negative bands (≈208 and 288 nm).…”