Molecular Catalysis
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2024
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IF 3.9
Yun Zhang,Guangfei Qu,Zhishuncheng Li,Junhong Zhou,Rui Xu,Junyan Li
This research has made significant advancements in the field of high-value bio-oil production, specifically focusing on the synthesis of the rare sugar D-Allose. Notably, synthesizing D-Allose through cellulose pyrolysis has long been challenging due to its high synthetic difficulty, which has limited related studies. By employing a one-pot synthesis approach using Al x -Fe y nano-catalysts prepared through a unique cellulose pretreatment method, this experiment successfully achieved efficient generation of D-Allose during rapid pyrolysis. Systematic experimentation demonstrated that at 330 °C with the Al 1 -Fe 5 nano-catalyst, the yield of D-Allose from cellulose pyrolysis reached an impressive 50.69 %, accompanied by a detection of 14.35 % furfural in the bio-oil. This breakthrough not only significantly contributes to the high-value utilization of bio-oil but also provides robust support for further development in this area. Simultaneously, the success of this research extends beyond high-value bio-oil utilization and makes a substantial impact on both the scientific community and industry.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Yanping Liu,Ying Zou,Hong Hu,Hongxia Gao,Yuan Yuan,Mianhong Chen,Ruyi Li,Yaping Dai,Xiaobing Huang,Chenghui Zhang,Jihua Li,Wei Zhou
Natural essential oils, such as d -limonene, are frequently used as flavoring agents and fragrances in the food industry. However, their susceptibility to volatilization and chemical degradation poses challenges for widespread application. In this study, cellulose nanocrystals (CNCs) and cellulose nanofibers (CNFs) were used to stabilize palm oils (POs) with different melting points to prepare Pickering emulsions (PEs) for the encapsulation of d -limonene. The physicochemical properties, environmental stability, 3D printing performance, and retention of d -limonene were explored. It results indicated that CNFs stabilized PO emulsions exhibit a stronger gel network structure, particularly pronounced in high melting point PO. CNF-stabilized emulsions enhanced stability to pH changes, salt ion, and storage conditions, due to a greater gel structure. Notably, it should be noted that CNCs and CNFs slowed down the release of d -limonene in both fresh and heat-treated emulsions. Furthermore, CNCs and CNFs emulsions as 3D printing inks, ensure accurate and stable formation of target shapes. The volatilization of d -limonene during the process was effectively suppressed (<9 %). The lower release of d -limonene in CNF emulsions (<2.8 %) could be linked to the tight distribution of CNF particles between the oil/water interface and the droplets, which makes the emulsion more resistant to extrusion. This study provides valuable insights into the use of PEs for encapsulating flavor components in 3D printing applications.
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Food Bioscience
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2024
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IF 4.8
Han Zhang,Zhen Sun,Xinling Du,Qianqian Cheng,Fuchun Ji,Zishen Nie,Julei Zhan,Zhouping Wang,Aitao Li,Irina Delidovich,Yu Xia
d- Allulose is a rare sugar with multiple physiological functions whose application has been restricted by low conversion rate, weak thermostability of the used enzymes, and complex production. In this study, a simplified multienzyme cascade strategy was designed for biosynthesis of d- allulose from d- glucose, and a detailed investigation of the crucial enzyme allulose 6-phosphate phosphatase was conducted. Under optimized conditions, the yield of d- allulose reached 4.12 ± 0.14 and 80.20 ± 3.20 mmol/L using 10.0 and 200.0 mmol/L d- glucose as substrate, respectively. Furthermore, the influence of various factors on the cooling crystallization of d- allulose was investigated, and the crystallization process was optimized. Consequently, a crystallization recovery rate of 77.43% ± 2.50% and a purity of 98.70% ± 0.05% were achieved. Moreover, the obtained crystals of d -allulose were characterized by XRD, TGA-DSC, and optical microscopy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Shiyong Mou,Siyuan Liu,Weidong Dai,Yanjuan Sun,Fan Dong
Electrochemical oxidative amidation (EOA) strategies offer a sustainable and potentially promising route for amide synthesis. However, the efficiency and activity of catalysts under oxidative conditions are highly dependent on noble metals. Herein, we present our experimental findings and fundamental understanding that fluorine-doped Nb 2 O 5 nanosheet arrays on carbon paper (F-Nb 2 O 5 /CP) serve as an efficient and robust non-noble catalyst for the electrochemical synthesis of formamide from ammonia and methanol under ambient conditions. In 0.5 M KHCO 3 solution, this catalyst achieved a high Faradaic efficiency of 52.0 %, with an N selectivity of 79.1 % at 1.5 V versus Hg/HgO electrode. The catalyst exhibited remarkable stability, maintaining its performance over 120 h. By integrating in-situ spectroscopy studies with density functional theory calculations, we revealed that fluorine doping induces a shift in the d-band center of the Nb site. This shift alters the adsorption behavior of OH - and *NH 2 intermediate on the F-Nb 2 O 5 (100) surface, thereby effectively lowering the C-N coupling energy barrier, and boosting the production of formamide.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-11
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IF 15.7
Long Haoyu,Zhang Xidong,Zhang Zhenyi,Zhang Jianjun,Yu Jiaguo,Yu Huogen
The H 2 -evolution kinetics play a pivotal role in governing the photocatalytic hydrogen-evolution process. However, achieving precise regulation of the H-adsorption and H-desorption equilibrium (H ads /H des ) still remains a great challenge. Herein, we propose a fine-tuning d - p hybridization strategy to precisely optimize the H ads /H des kinetics in a Ni-B x modified CdS photocatalyst (Ni-B x /CdS). X-ray absorption fine-structure spectroscopy and theoretical calculations reveal that increasing B-atom amount in the Ni-B x cocatalyst gradually strengthens the d - p orbital interaction between Ni 3 d and B 2 p , resulting in a consecutive d -band broadening and controllable d -band center on Ni active sites. The above consecutive d -band optimization allows for precise modulation of the H ads /H des dynamics in the Ni-B x /CdS, ultimately demonstrating a remarkable H 2 -evolution activity of 13.4 mmol g -1 h -1 (AQE = 56.1 %). The femtosecond transient absorption spectroscopy further confirms the rapid electron-transfer dynamics in the Ni-B x /CdS photocatalyst. This work provides insights into the optimal design of prospective H 2 -evolution catalysts.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
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IF 5.7
Lichun Guo,Mengqing Zhang,Ying Fei,Wei Zhao
This study examines the inhibitory effects of a range of sweeteners on α-glucosidase. Our findings revealed that only one natural sweetener, namely, glycyrrhetinic acid 3-O-mono-beta-d-glucuronide (GAMG), derived from licorice, exhibited a mixed-type inhibition against α-glucosidase with a IC50 value of 0.73 ± 0.05 mg/mL. The fluorescence intensity of α-glucosidase was quenched by GAMG in the formation of an α-glucosidase–GAMG complex. GAMG has been shown to induce conformational changes in α-glucosidase, likely through hydrogen bonding, van der Waals force, and alkyl–alkyl interactions with amino acid residues, including Arg 281, Leu 283, Trp 376, Asp 404, Asp 443, Trp 481, Asp 518, Phe 525, Ala 555, and Asp 616. Additional animal validation experiments demonstrated that GAMG slowed starch digestion, thereby attenuating the postprandial glycemic response. Taken together, these findings provide evidence that GAMG is a natural sweetener with potent inhibitory activity that selectively targets α-glucosidase. This study supports the use of GAMG as a natural sweetener, which holds a high biological value and may be beneficial for managing postprandial hyperglycemia.
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Chem
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2024
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IF 19.1
Yang Yang,Guohua Yao,Xiaojuan Zhu,Meiqi Gao,Lili Wang,Shunlin Li,Xuerong Li,Xuezhi Duan,De Chen,Weimin Yang,Ying Wan
Selective hydrogenation of phenol is a sustainable alternative to cyclohexane oxidation for the production of cyclohexanone. However, over-hydrogenation of cyclohexanone to cyclohexanol is thermodynamically favorable, limiting its selectivity. Here, we report an unprecedented cyclohexanone selectivity (>99.9%) in continuous-flow phenol hydrogenation using an electron-deficient Pd catalyst. The Pd atom exists in a unique Pd–N 5 C 4 structure in which it is coordinated with four quasi-planar N atoms and one axial N atom in the first shell and an additional four C atoms in the second shell that lie on the curved surface of a pore in ordered mesoporous carbon. The Pd site has a d charge depletion of 1.18 e that prevents cyclohexanone adsorption, which is therefore exclusively produced. Bonding the Pd atom to a curved plane of carbon atoms is an effective way to control the d charge of Pd and increase its selectivity for the green synthesis of fine chemicals.
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Catalysis Science & Technology
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2024
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IF 4.4
Qingxiu Wang,Weisong Liu,Lijing Chang,Kuncheng Zhang,Yanbing Shen,Lingling Zhang
L-guluronic acid, a patented drug with immunomodulatory and anti-inflammatory properties, is traditionally sourced from natural seaweed species or synthesized chemically. Both methods suffer from low selectivity and environmental concerns and there is a high demand to develop a green and efficient approach for L-guluronic acid production. Herein, we successfully developed a two-step enzymatic route to synthesize L-guluronic acid from D-glucose by two oxidases, glucose oxidase (GOx) and galactose oxidase (GOase). Due to the sluggish kinetics of GOase in catalyzing the oxidation of D-gluconic acid, rational design was implemented. Through molecular docking and iterative saturation mutagenesis, a variant, GOase T406R/K330R/Y329F, was obtained. The variant exhibited a remarkable 13-fold higher oxidation activity towards D-gluconic acid, reaching 7.8 U mg-1. The substitutions synergistically switch the D-gluconic acid molecule to a favorable conformation and facilitate the specific activation of the primary alcohol group at C6 position. In a cascade reaction, complete conversion of 40 mM D-glucose to L-guluronic acid was achieved in 2 h with 100% selectivity, presenting a promising and green bio-manufacturing strategy for the scalable production of L-guluronic acid.
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Animal Models and Experimental Medicine
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2024
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IF 3.8
Xue Wang,Chunyou Ning,Xingyi Cheng,Zhengzhong Wu,Dongbo Wu,Xuemei Ding,Cunxiang Ju,Zhihang Zhou,Lingfeng Wan,Wei Zhao,Peiliang Shi
Background The emerging incidence of pathogenic liver conditions is turning into a major concern for global health. Induction of pyroptosis in hepatocytes instigates cellular disintegration, which in turn liberates substantial quantities of pro-inflammatory intracellular substances, thereby accelerating the advancement of liver fibrosis. Consequently, directing therapeutic efforts towards inhibiting pyroptosis could potentially serve as an innovative approach in managing inflammation related chronic hepatic disorders. Methods GSDMD-NT ki/wt mice and Alb-cre ki/wt mice were generated using CRISPR/Cas9 technology. After crossing the two strains together, we induced conditional cell death by doxycycline to construct a mouse model of liver fibrosis. We analyzed differentially expressed genes by RNA sequencing and explored their biological functions. The efficacy of obeticholic acid (OCA) in the treatment of liver fibrosis was assessed. Results Doxycycline-treated GSDMD-NT ki/wt × Alb-cre ki/wt mice showed severe liver damage, vacuolation of hepatocytes, increased collagen fibers, and accumulation of lipid droplets. The expression of liver fibrosis related genes was greatly increased in the doxycycline-treated mouse liver compared with untreated mouse liver. RNA-sequencing showed that upregulated differentially expressed genes were involved in inflammatory responses, cell activation, and metabolic processes. Treatment with OCA alleviated the liver fibrosis, with reduced ALT and AST levels seen in the GSDMD-NT ki/wt × Alb-cre ki/wt mice. Conclusions We successfully constructed a novel mouse model for liver fibrosis. This GSDMD-NT-induced fibrosis may be mediated by abnormal lipid metabolism. Our results demonstrated that we successfully constructed a mouse model of liver fibrosis, and GSDMD-NT induced fibrosis by mediating lipid metabolism.
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JOURNAL OF CHROMATOGRAPHY A
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2025
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IF 4
Lei Ding,Chundan Ye,Junchen Zhu,Cuirong Sun
Chiral impurity analysis presents significant challenges due to limitations of detection methods. Levodopa (L-Dopa) is the primary medication for Parkinson's disease treatment for over 50 years. However, the detection of its chiral impurity is difficult due to the similarity of polarity. This study presents a novel analytical method for the quantitative detection of trace amount of D-Dopa, as well as other three impurities. The method demonstrated excellent chromatographic resolution for D-Dopa and L-Dopa (resolution = 4.15) and achieved a derivatization efficiency of 97% using a chlorine-labeled chiral probe (D-BPCl) for chemical derivatization, followed by analysis with liquid chromatography-tandem mass spectrometry (LC-MS/MS) on a conventional C18 column. Meanwhile, D-BPCl showed strong chiral selectivity on D-Dopa, and the ratio of mass spectrometric response for labeled D-Dopa to that of L-enantiomers was 2.78-fold under the same condition. The developed method demonstrates high sensitivity with detection limits of 7.88 μ g L -1 for D-Dopa, and 9.85 μ g L -1 for L-Dopa, with good linearity for every analyte (R 2 > 0.99), recoveries ranging from 94.1% to 106.8%, and high repeatability with relative standard deviation (RSD) values predominantly below 5%. Then the method was applied to analyze fifteen batches of levodopa tablets from five manufacturers. D-Dopa was successfully detected with the corresponding content ranging from 0.15% to 0.44%, which suggests that D-Dopa are more likely generated during the production process. The study underscores the significant safety concerns regarding Dopa-containing medications.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Ze Li,Yidan Fu,Lina Han,Pengfei Zheng,Xiaoyuan Zeng,Peng Dong,Jing Feng,Yingjie Zhang
The insufficient d-electron density in V metal atoms limits O2 dissociation, constraining the kinetics and activity of the oxygen reduction reaction and the oxygen evolution reaction in VN-based catalysts. Herein, Co dopant was employed to modulate the electronic characteristics of the d-orbitals and associated free energy of VN, thereby further enhancing its catalytic activity. XPS and XANES spectra revealed that Co atoms replaced V and strongly bonded with neighboring N atoms, effectively regulating the local electronic structure. DFT analysis show that the Co doping strategy effectively regulates the adsorption/desorption equilibrium of oxygen reduction reaction intermediates through d-electron transfer to V atoms, while significantly lowering the activation energy barrier of the rate-determining step. Electrochemically, V0.95Co0.05N/NC/C achieved a low bifunctional index (ΔE = 0.78 V), with a half-wave potential for the ORR of 0.83 V and an OER overpotential of 380 mV at 10 mA cm–2. In Zn-air batteries, it achieved a high specific capacity (708.98 mAh gZn–1) and retained 88% initial voltage after 280 h cycling, demonstrating robust stability for practical applications. This study presents a doping strategy to modulate d-band centers in transition metal nitrides for energy conversion devices.
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Laser & Photonics Reviews
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2025
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IF 10
Di Liu,Pengwei Duan,Junjie Chen,Ming Mu,Yumei Yang,Fuqiu Ma,Bing Zhao,Wei Song
Understanding atomic orbital-level interactions at material-molecule interfaces is crucial for advancing surface-enhanced Raman spectroscopy (SERS). While conventional mechanisms focus on electromagnetic effects or interfacial charge transfer (CT), the role of orbital hybridization in multimetallic systems remains underexplored. Here, a d-band-mediated CT mechanism is proposed through the engineering high-entropy alloy aerogels (HEAAs). A face-centered cubic AuAgCuMnInBi HEAAs synthesized via one-step coreduction achieves ultrasensitive SERS detection of crystal violet. Density of states analyses reveal that Mn-3d orbitals bridge electron reservoirs (Au/Ag/Cu) and In/Bi-p orbitals, enabling efficient charge delocalization. Voltage-tunable SERS signals in MnInBi subsystems confirm d-band-dependent CT enhancement. Beyond molecular sensing, this mechanism allows direct capture of reactive intermediates (OH·, O 2 · – ) and 5 n M uranium detection, bridging SERS enhancement dynamics with catalytic pathway elucidation. These findings establish d-band engineering as a paradigm for designing multifunctional SERS substrates, bridging atomic-scale electronic interactions with ultrasensitive sensing and catalytic mechanism elucidation.
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