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Chang Peng Yuxue Liu Xiaojia Guo Wujun Liu Qing Li Zongbao K. Zhao 《Tetrahedron letters》2018,59(42):3810-3815
Selective carboxylation of substituted phenols is realized in the presence of bicarbonate under ambient pressure by engineered Escherichia coli whole-cells expressing various hydroxybenzoate decarboxylases, leading to their corresponding ortho-hydroxybenzoates. This process may be further developed as an efficient route to upgrade lignin-derived phenolic compounds as valuable building blocks. 相似文献
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Xiaojia Guo Yuxue Liu Qian Wang Xueying Wang Qing Li Wujun Liu Zongbao K. Zhao 《Angewandte Chemie (International ed. in English)》2020,59(8):3143-3146
A non‐natural cofactor and formate driven system for reductive carboxylation of pyruvate is presented. A formate dehydrogenase (FDH) mutant, FDH*, that favors a non‐natural redox cofactor, nicotinamide cytosine dinucleotide (NCD), for generation of a dedicated reducing equivalent at the expense of formate were acquired. By coupling FDH* and NCD‐dependent malic enzyme (ME*), the successful utilization of formate is demonstrated as both CO2 source and electron donor for reductive carboxylation of pyruvate with a perfect stoichiometry between formate and malate. When 13C‐isotope‐labeled formate was used in in vitro trials, up to 53 % of malate had labeled carbon atom. Upon expression of FDH* and ME* in the model host E. coli, the engineered strain produced more malate in the presence of formate and NCD. This work provides an alternative and atom‐economic strategy for CO2 fixation where formate is used in lieu of CO2 and offers dedicated reducing power. 相似文献
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Ji D Wang L Hou S Liu W Wang J Wang Q Zhao ZK 《Journal of the American Chemical Society》2011,133(51):20857-20862
Many enzymes catalyzing biological redox chemistry depend on the omnipresent cofactor, nicotinamide adenine dinucleotide (NAD). NAD is also involved in various nonredox processes. It remains challenging to disconnect one particular NAD-dependent reaction from all others. Here we present a bioorthogonal system that catalyzes the oxidative decarboxylation of l-malate with a dedicated abiotic cofactor, nicotinamide flucytosine dinucleotide (NFCD). By screening the multisite saturated mutagenesis libraries of the NAD-dependent malic enzyme (ME), we identified the mutant ME-L310R/Q401C, which showed excellent activity with NFCD, yet marginal activity with NAD. We found that another synthetic cofactor, nicotinamide cytosine dinucleotide (NCD), also displayed similar activity with the ME mutants. Inspired by these observations, we mutated d-lactate dehydrogenase (DLDH) and malate dehydrogenase (MDH) to DLDH-V152R and MDH-L6R, respectively, and both mutants showed fully active with NFCD. When coupled with DLDH-V152R, ME-L310R/Q401C required only a catalytic amount of NFCD to convert l-malate. Our results opened the window to engineer bioorthogonal redox systems for a wide variety of applications in systems biology and synthetic biology. 相似文献
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Fu W Kiggans J Overbury SH Schwartz V Liang C 《Chemical communications (Cambridge, England)》2011,47(18):5265-5267
Microwave induced rapid decomposition of nitromethane at low temperature exfoliates the graphene sheets from the FeCl(3) and CH(3)NO(2) co-intercalated graphite compound without creating many defects and functional groups. This approach provides a scalable method for high-quality graphene materials via low-temperature exfoliation of graphite under mild chemical conditions. 相似文献
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We design a two-scale finite element method (FEM) for linear elliptic PDEs in non-divergence form \(A(x) : D^2 u(x) = f(x)\) in a bounded but not necessarily convex domain \(\Omega \) and study it in the max norm. The fine scale is given by the meshsize h, whereas the coarse scale \(\epsilon \) is dictated by an integro-differential approximation of the PDE. We show that the FEM satisfies the discrete maximum principle for any uniformly positive definite matrix A provided that the mesh is face weakly acute. We establish a discrete Alexandroff–Bakelman–Pucci (ABP) estimate which is suitable for finite element analysis. Its proof relies on a discrete Alexandroff estimate which expresses the min of a convex piecewise linear function in terms of the measure of its sub-differential, and thus of jumps of its gradient. The discrete ABP estimate leads, under suitable regularity assumptions on A and u, to pointwise error estimates of the form provided \(\epsilon \approx h^{2/(2+\alpha )}\). Such a convergence rate is at best of order \( h \big | \ln h \big |\), which turns out to be quasi-optimal.
相似文献
$$\begin{aligned} \Vert \,u - u^{\epsilon }_h\,\Vert _{L^{\infty }(\Omega )} \le \, C(A,u) \, h^{2\alpha /(2 + \alpha )} \big | \ln h \big | \qquad 0< \alpha \le 2, \end{aligned}$$
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Gao Q Xu W Xu Y Wu D Sun Y Deng F Shen W 《The journal of physical chemistry. B》2008,112(7):2261-2267
In order to disclose the dominant interfacial interaction between amino acids and ordered mesoporous materials, the adsorption behaviors of five amino acids on four mesoporous materials were investigated in aqueous solutions with adjustable amino acid concentration, ion strength, and pH. The selected amino acids were acidic amino acid glutamic acid (Glu), basic amino acid arginine (Arg), and neutral amino acids phenylalanine (Phe), leucine (Leu), and alanine (Ala), and the selected mesoporous materials were SBA-15, Al-SBA-15, CH3(10%)-SBA-15, and CH3(20%)-SBA-15. The adsorption capacities of Glu and Arg were strongly dependent on pH and surface charge of the mesoporous adsorbent. The adsorption of Phe showed pH insensitivity but depended on the surface organic functionalization of mesoporous adsorbent. On the basis of the theoretical analysis about the interaction between amino acid and adsorbent, such a remarkable difference was attributed to the different nature of the interaction between amino acid and adsorbent. Arg could be readily adsorbed on the surface of SBA-15, especially Al-SBA-15, under appropriate pH in which the electrostatic interaction was predominant. The driving force of Phe adsorption on mesoporous adsorbent mainly came from the hydrophobic interaction. Therefore, the adsorption capability of Arg decreased with increasing ion strength of solution, while the adsorption capability of Phe increased with the increasing degree of CH3 functionalization on SBA-15. For neutral amino acid Phe, Ala, and Leu, the adsorption capability increased with the increase of the length of their side chains, which was another evidence of hydrophobic effect. Thus, all the adsorption of amino acids on mesoporous silica materials can be decided by the combined influence of two fundamental interactions: electrostatic attraction and hydrophobic effect. 相似文献
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一类三阶非线性非自治系统解的有界性 总被引:1,自引:0,他引:1
本文利用一为三阶非线性自治系统的李雅夫函数,给出了一类三阶非线性非自治系统解有界的充分性准则,推广了文「1-2」的结果。 相似文献
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Numerous strategies for linking desired chemical probes with target peptides and proteins have been developed and applied in the field of biological chemistry. Approaches for site-specific modification of native amino acid residues in test tubes and biological contexts represent novel biological tools for understanding the role of peptides and proteins. Selective N-terminal modification strategies have been broadly studied especially in the last 10 years, as N-terminal positions are typically so... 相似文献
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