JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2025
·
IF 6.2
Shuang Du,Nan Zheng,Zehua Zhang,Chenhao Zhang,Huimin Zhou,Yu Deng,Jian Yin,Yongchao Cai,Xiaole Xia
5-Aminolevulinic acid synthase (ALAS) is the key rate-limiting enzyme in the synthesis of the vital biosynthetic intermediate 5-aminolevulinic acid (ALA). However, its catalytic efficiency is compromised due to its low activity and poor stability. Here, we obtained the mutant I325M/V390Y/H391I (T6), which exhibited a 7.0-fold increase in specific activity (2.53 U/mg) compared to the wild type through the application of isothermal compressibility (βT) perturbation engineering in conjunction with two thermal stability prediction algorithms. Moreover, molecular dynamics simulations indicate that positive changes in intermolecular interactions, the substrate channel, and the binding pocket account for the improved catalytic activity of T6. Furthermore, T6 was immobilized on magnetic chitosan nanoparticles, maintaining 73.5% of its original activity after 10 reaction cycles. Overall, combination approaches were employed to construct a superior ALAS variant, providing a novel concept for the synthesis of ALA and a valuable benchmark for optimizing industrial enzymes in related fields.
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PubMed
高影响因子
JOURNAL OF SEPARATION SCIENCE
·
2019
·Vol. 42
·期 15
·2482-2490
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IF 2.516
Lingping Cheng,Jianfeng Cai,Qing Fu,Yanxiong Ke
6-(4-Aminophenyl)-5-methyl-4,5-dihydro-3(2H)-pyridazinone is a key synthetic intermediate for cardiotonic agent levosimendan. Very few studies address the use of chiral stationary phases in chromatography for the enantioseparation of this intermediate. This study presents two efficient preparative methods for the isolation of ( R )(−)-6-(4-aminophenyl)-5-methyl-4,5-dihydro-3(2H)-pyridazinone in polar organic solvent chromatography and supercritical fluid chromatography using polysaccharide-based chiral stationary phases and volatile organic mobile phases without additives in isocratic mode. Under optimum conditions, Chiralcel OJ column showed the best performance ( α = 1.71, Rs = 5.47) in polar organic solvent chromatography, while Chiralpak AS column exhibited remarkable separations ( α = 1.81 and Rs = 6.51) in supercritical fluid chromatography with an opposite enantiomer elution order. Considering the sample solubility, runtime and solvent cost, the preparations were carried out on Chiralcel OJ column and Chiralpak AS column (250 × 20 mm i.d.; 10 µm) in polar organic mode and supercritical fluid chromatography mode with methanol and CO 2 /methanol as mobile phases, respectively. By utilizing the advantages of chromatographic techniques and polysaccharide-based chiral stationary phases, this work provides two methods for the fast and economic preparation of ( R )(−)-6-(4-aminophenyl)-5-methyl-4,5-dihydro-3(2H)-pyridazinone, which are suitable for the pharmaceutical industry.
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高影响因子
Catalysis Science & Technology
·
2018
·Vol. 9
·期 3
·659-671
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IF 5.365
Yanliang Zhai,Shaolong Zhang,Yunshan Shang,Yu Song,Wenxuan Wang,Tong Ma,Luoming Zhang,Yanjun Gong,Jun Xu,Feng Deng
Herein, a specific core–shell MFI zeolite was designed for the methanol to propylene (MTP) reaction. The core–shell structure of Al-ZSM-5@B-ZSM-5 and Al-ZSM-5@silicalite-1 were easily obtained via a two-step procedure, in which Al-ZSM-5 aggregate acted as the core and B-ZSM-5 or silicalite-1 as the shell. Their core–shell structures, acidity distribution and pore properties were characterized systemically, and new insights were gained into the synergetic effect of acid property and diffusion on the MTP reaction. The Al-ZSM-5@B-ZSM-5 zeolite exhibited a superior catalytic performance with a lifetime of 350 h (WHSV = 3 h−1), propylene selectivity of 49% and high turnover number of 4.3 × 106, while for the Al-ZSM-5 core, the corresponding values were 210 h, 43% and 5.2 × 105, respectively. Al-ZSM-5@silicalite-1 displayed the second best performance with the values of 250 h, 45% and 2.9 × 106, respectively. Gradient strong acid reduction from the core to the shell via the epitaxial growth of the silicalite-1 or B-ZSM-5 shell combined with an appropriate strong/weak acid ratio plays a vital role in inhibiting the hydrogen transfer reaction and thus gives a low consumption of propylene and low coke deposition. For the hydrogen transfer reaction of alkenes to form alkanes and aromatics, strong acid sites are required. Moreover, the acid sites originally existing on the external surface of the Al-ZSM-5 core were converted into internal acid sites due to the formation of an interface zone in the core–shell zeolite, possessing micropore characteristics, which in turn improve the shape selectivity and suppress coke deposition. Especially, the Al-ZSM-5@B-ZSM-5 zeolite displayed more weak acid sites and few strong acid sites on its shell surface, which are beneficial for the low formation of external coke and also account for the highest utilization of acid sites in the MTP reaction, high propylene selectivity and long lifetime.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Sibo Zhao,Hengbin Mao,Weishan Ma,Mingliang Li,Shao Gang,Bingbing Fan,Hailong Wang,Hongliang Xu,Hongxia Lu
All-inorganic halide perovskite nanocrystals (NCs) have attracted much attention in many fields. However, the poor stability of NCs and the toxicity of Pb have greatly hindered their practical applications. Reducing the proportion of Pb with the concept of high-entropy and coating NCs with an outer layer have been regarded as effective strategies to solve the problems. Herein, We have successfully synthesized the all-inorganic high-entropy dual-phase Cs(Pb 1/5 Mn 1/5 Ni 1/5 Zn 1/5 Cd 1/5 )Br 3 /Cs(Pb 1/5 Mn 1/5 Ni 1/5 Zn 1/5 Cd 1/5 ) 2 Br 5 (Cs‘B’Br 3 /Cs‘B’ 2 Br 5 ) perovskite NCs with good luminescence properties by a high-energy ball milling method; On the basis of which, Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs are coated with SiO 2 and EVA resin. Due to the amorphous SiO 2 protection, the Cs‘B’Br 3 /Cs‘B 2 ’Br 5 @SiO 2 NCs maintained 93% of their emission intensity after 90 days compared to their uncoated counterparts. The PL intensity of Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs /EVA was significantly enhanced by a factor of 4.7 for compared to the uncoated NCs. In addition, the PL emission intensity of the Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs /EVA remained 93.7% after 90 days, and the emission peak intensity remained approximately 63% after 8 h of placement in an enclosed environment at 80% humidity through the dense polymer chains and the hydrophobic nature of the film. Finally, the film could expand its application prospects in the field of flexible device.
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MATERIALWISSENSCHAFT UND WERKSTOFFTECHNIK
·
2020
·Vol. 51
·期 9
·1295-1303
·
IF 0.744
Y. Qian,H. Zhang,L. Li,Y. Duan
In this study, ZSM-5 zeolite with hierarchical porosity structure was synthesized by hydrothermal method using Al(OH) 3 , SiO 2 extracted from coal fly ash as aluminum source and silicon source. The optimal synthesis parameters of ZSM-5 zeolite were determined via an orthogonal analysis table. The optimum synthesis conditions were: SiO 2 /Al 2 O 3 /Na 2 O/hexadecyltrimethylammonium bromide/tetrapropyl ammonium bromide/H 2 O = 1/0.08/0.25/0.05/0.17/50, and the optimum crystallization temperature and crystallization time were 160 °C and 48 h, respectively. Scanning electron microscopy showed that the synthesized ZSM-5 zeolite exhibited a spherical shape. Nitrogen adsorption-desorption and Brunauer-Emmett-Teller measurement analysis displayed that the best sample ZSM-5 molecular sieve showed a typical type IV isotherm, and the micropores and mesopores coexisted in the sample, indicating the successful preparation of ZSM-5 zeolite with hierarchical porosity structure. The crystal growth of ZSM-5 under different hydrothermal conditions follows the “S” adjustment.
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NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Rui Zhang,Shimin Li,Jiale Chen,Jiantao Li,Jian Xiong,Zhihao Yu,Xuebin Lu
A template-assisted approach was employed to synthesize a MOF-on-MOF derived catalyst for the selective oxidation of 5-hydroxymethylfurfural (5-HMF) to produce 2,5-furandicarboxylic acid (FDCA). Characterization revealed that the catalyst forms a cobalt–manganese metal oxide composite phase with a hierarchical porous structure and uniformly distributed Co/Mn active sites. The oxygen vacancies work together with the Lewis acid sites to gradually oxidize the hydroxyl and aldehyde groups in 5-HMF. In the context of reaction conditions that have been identified as optimal (140 °C, 6 h, 50 mg catalyst, 5.88 mol L−1 H2O2), the yield of FDCA was 87.55%, accompanied by 5-HMF conversion rate of 98.66%. The catalyst exhibited exceptional cycling stability, sustaining an FDCA yield exceeding 75% across five cycles. Mechanism studies indicate that the Co–Mn bimetallic synergistic effect optimizes the reaction pathway through electron transfer and oxygen species activation, while the microporous structure prolongs the residence time of intermediates through confinement effect, promoting multi-step oxidation. Compared with the single-metal MOFs derived catalysts, this catalyst has significantly improved adsorption performance and oxidation efficiency, providing an efficient solution for the green synthesis of the bio-based polyester monomer FDCA.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Xingyi Tian,Lan Tang,Hanlin Zeng,Yulu Li,Jingdong Peng,Ming Li,Rongxing He
The electrochemical oxidation of 5-hydroxymethylfurfural (HMFOR) offers a promising route for biomass upgrading. However, its kinetics are severely hindered by the competitive adsorption between key reactive species on catalyst surfaces. Herein, we report a CoO/Ni 3 N-2:3 heterojunction catalyst that enables efficient and selective conversion of HMF to 2,5-furandicarboxylic acid (FDCA). A “bipolar synergistic adsorption effect” is identified at the CoO/Ni 3 N-2:3 interface. This effect is driven by a built-in electric field (BIEF) generated through interface polarization and the work function difference (ΔΦ) between Ni 3 N and CoO. In situ spectroscopic studies and theoretical calculations reveal that the BIEF acts as an electron sorter, directing OH − and HMF to respectively adsorb at oppositely charged regions while strengthening their adsorption. This spatially oriented adsorption effectively lowers the reaction energy barrier and suppresses competitive adsorption of key reactive species, thereby enhancing both activity and selectivity. As a result, the CoO/Ni 3 N-2:3 catalyst initiates HMFOR at a low potential of 1.18 V RHE and achieves complete HMF conversion at 1.408 V RHE with 99.2% FDCA yield and 97.2% Faradaic efficiency. This work provides an innovative strategy for designing high-performance electrocatalysts for biomass valorization.
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ACS Applied Polymer Materials
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2026
·
IF 5.2
Xue Wang,Li Xu,Ziliang Wang,Yuqi Sun,Baixue Li,Yanan Gu,Yusheng Qin
5-Hydroxymethylfurfural (HMF) is a versatile biomass-derived platform chemical, but the efficient and mild conversion of its derivatives to high-performance polymers remains a challenge. In this work, we introduce HMF derivatives into Kabachnik–Fields three-component polymerization (KF-3CP) without isocyanide components to prepare a biobased polymer with α-aminophosphonate. The KF-3CP protocol has proven generally applicable to diverse diamine and dialdehyde monomers, affording polymers with high molecular weights (Mw up to 27,800 g/mol), excellent yields (up to 98%), and favorable water solubility. Remarkably, the prepared KF-3CP polymers exhibited nontraditional intrinsic fluorescence that was efficiently quenched by Fe3+ ions, combined with low cytotoxicity and outstanding cell imaging capability. Furthermore, it can undergo postpolymerization modification through the Diels–Alder reaction, thereby imparting excellent mechanical properties. These findings establish the KF-3CP products derived from HMF derivatives as highly promising candidates for various applications in the biomedical and materials fields.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Yuang Ma,Yihui Zhang,Huixia Ma,Yaolan Yang,Wenhua Zhou,Wentao Jin,Chao Chen,Jianghao Wang,Bolong Li,Huiping Ji,Feng Zhou,Kai Qiao,Zhenyu Zhang,Haoan Fan,Jie Fu
The high production cost and inherent instability of 5-hydroxymethylfurfural (HMF) present major bottlenecks for the scalable synthesis of 5-methoxymethylfurfural (MMF), a promising biobased fuel additive and platform chemical. To address this, we propose a novel and cost-effective one-pot strategy that incorporates quaternary ammonium salts as stabilizers within a dimethyl carbonate (DMC)−methanol solvent system catalyzed by Amberlyst-15. This approach effectively suppresses the degradation of the HMF intermediate during the tandem conversion of fructose, achieving an MMF yield of 77.2% under the optimized conditions. Mechanistic investigations by Fourier transform infrared and 1H nuclear magnetic resonance spectroscopy confirm that the quaternary ammonium stabilizers coordinate with the hydroxyl and aldehyde groups of HMF through electrostatic interactions, thereby shielding it from hydration and enhancing etherification selectivity. Thus, it achieves the necessary intermediate stabilization without the economic and separation penalties of conventional DMSO or ionic liquid systems, providing a practical foundation for developing an economically viable route to MMF production.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Zhen Feng,Jiayao Qiu,Jiashu Tang,Xiangrui Ren,Chengyan Li,Pengxiang Sun,Cancan Zhou,Yi Guo,Ye Chen,Xupo Liu
Electrocatalytic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) offers a sustainable route to synthesize the value-added platform chemical 2,5-furandicarboxylic acid (FDCA). However, the synergistic mechanism of HMF oxidation involving Ni 3 + OOH and the anionic groups generated by the reconstructed nickel-based catalysts remains unclear. Herein, a self-supporting Ni 3 S 2 catalyst is synthesized via a two-step hydrothermal method for efficient HMF oxidation reaction (HMFOR). The synthesized NF/Ni 3 S 2 achieves the current density of 112.50 mA cm −2 at 1.45 V, with 99.59% HMF conversion and 99.18% FDCA yield. In situ Raman spectroscopy and XPS analysis reveal that partial sulfur-containing species are detached from the lattice during the electrochemical reconstruction from S 2− to SO 4 2− . This process generates abundant sulfur vacancies and exposes more nickel active sites, thereby promoting the formation of Ni 3+ OOH species. DFT calculations demonstrate that SO 4 2− incorporation induces charge redistribution in the NiOOH-SO 4 2− system, enhancing the electrophilicity of Ni 3+ sites and reducing the energy barrier across the HMFOR pathway. This work elucidates the synergistic mechanism of SO 4 2− in promoting NiOOH formation and optimizing reaction energetics, providing critical insights for designing advanced sulfide-based electrocatalysts for biomass valorization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Qian Wang,Rui Li,Siyao Yao,Qingde Chen,Qinghu Tang,Futing Xia,Qiu-E Cao,Wenhao Fang
● Au particles were in situ grown on spinel Co 3 O 4 needle-shaped arrays. ● Au induced Co–O lattice distortion, Co vacancies and Co 3 O 4 low-potential reconstruction. ● Au-driven charge redistribution shifted Co 3 d states toward E f and accelerated charge transfer. ● CoOOH active sites enhanced C O adsorption and facilitated HMFCA-to-FFCA oxidation. ● Au-Co 3 O 4 enabled 99.5% FDCA yield and 99.7% FE and rivalled the top Co-based catalysts. 5-Hydroxymethylfurfural electrooxidation (HMFOR) into 2,5-furandicarboxylic acid (FDCA) is a very promising route for biomass upgrading. Although Co 3 O 4 catalyst is favored due to superior redox ability and high activity, it still suffers from harsh reconstruction of Co–O units and sluggish cascade oxidation of intermediates. Here, low-loading Au was discovered to provoke Co 3 O 4 catalytic properties for efficient HMFOR in the alkaline media. The developed Au-Co 3 O 4 catalyst showed a low onset potential at 1.18 V ( vs. reversible hydrogen electrode, RHE) and delivered a current density of 100 mA cm –2 at only 1.34 V in 1 M KOH, outperforming the top Co-based catalysts reported to date in the literature. Au particles in strong interaction with Co 3 O 4 needle-like arrays induced the lattice expansion and anisotropic distortion of octahedral Co 3+ –O units, cobalt-vacancy defects, and surface electronic redistribution of Co 3 O 4 . As a result, these unique properties of Au-Co 3 O 4 enabled enhanced interfacial charge transfer, stronger adsorption of furanic reactants, and substantially accelerated HMFOR kinetics compared with Co 3 O 4 and Au electrodes. It was disclosed that Au-provoked structural and electronic perturbations of Co–O units allowed low-potential reconstruction to CoOOH active sites and promoted formation of OH-derived oxidizing agents under the mild operating potentials. These coupled effects can account for the improved intermediate selective oxidation into FDCA. 99.5% yield of FDCA with 99.7% Faradaic efficiency at 1.36 V was accordingly achieved. To the best of our knowledge, this work can be the first example of success in Au-regulated Co 3 O 4 electrocatalysis for steering selective oxidation of biomass derivatives. Download: Download high-res image (181KB) Download: Download full-size image
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Journal of Advanced Research
·
2026
·
IF 17.1
Xueting Liu,Chang Yan,Ruiqi Su,Mengwen Shi,Zhi Geng,Ying Chen,Liwen Zhu,Zongjie Dai,Junfeng Hui,Xi Chen,Kai-Zhi Jia
Introduction Pyridoxal-5′-phosphate (PLP), the ubiquitous and ancient cofactor, plays important roles in enzymatic elimination, transamination and other reactions. The catalytic efficiency of PLP-dependent enzymes is significantly higher than that of free PLP. The recruitment of solution PLP by the enzymes, particularly through interactions outside the active-site entrance, is the key step determining the occurrence of PLP-mediated catalysis. However, the precise mechanism by which enzymes recruit solution PLP remains elusive. Objectives This study aims to elucidate the mechanism by which enzymes, specifically methionine γ-lyase (MGL) that suppresses cancer cell proliferation through serum or dietary methionine depletion, recruit solution PLP and to investigate the role of the C-terminal domain in this process. The study also seeks to explore the relationship between PLP recruitment and the efficient L-methionine catabolism in the host organism. Methods We report the crystal structure of yMGL, which belongs to a newly identified subgroup of cystathionine γ-lyases, in complex with L-methionine and PLP. To investigate the functional role of the C-terminal domain in PLP recruitment and enzyme activity, we performed C-terminal domain truncations and mutations and assessed their effects both in vitro and in vivo , analyzing changes in PLP binding affinity and L-methionine catabolism, respectively. Results Through structural, biochemical, bioinformatic and metabolic analyses, we demonstrate that the C-terminal domain of yMGL, outside the canonical PLP-binding domain, is essential for the specific interaction between yMGL and PLP, and L-methionine catabolism. A conserved Ser residue within this domain, located outside of active-site entrance, determines PLP recruitment. Conclusion These findings elucidate a previously uncharacterized mechanism of PLP recruitment by MGLs and enable rational design of MGLs with enhanced PLP binding and catalytic performance.
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