JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2018
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IF 3.412
Cun-Duo Tang,Hong-Ling Shi,Jian-He Xu,Zhu-Jin Jiao,Fei Liu,Peng-Ju Ding,Hong-Fei Shi,Lun-Guang Yao,Yun-Chao Kan
d-Mandelate dehydrogenase (DMDH) has the potential to convert d-mandelic acid to phenylglyoxylic acid (PGA), which is a key building block in the field of chemical synthesis and is widely used to synthesize pharmaceutical intermediates or food additives. A novel NAD+-dependent d-mandelate dehydrogenase was cloned from Lactobacillus harbinensi (LhDMDH) by genome mining and expressed in Escherichia coli BL21. After being purified to homogeneity, the oxidation activity of LhDMDH toward d-mandelic acid was approximately 1200 U·mg–1, which was close to four times the activity of the probe. Meanwhile, the kcat/Km value of LhDMDH was 28.80 S–1·mM–1, which was distinctly higher than the probe. By coculturing two E. coli strains expressing LhDMDH and LcLDH, we developed a system for the efficient synthesis of PGA, achieving a 60% theoretical yield and 99% purity without adding coenzyme or cosubstrate. Our data supports the implementation of a promising strategy for the chiral resolution of racemic mandelic acid and the biosynthesis of PGA.
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TALANTA
·
2024
·
IF 5.6
Xiupei Yang,Xiaoyi Xie,Ling Jiang,Yuxiu Fan,Chenglin Zhang,Ya Wang
Most conventional nanozymes have poor specificity and low activity, and designing high-performance nanozymes remains a challenge. In contrast, single-atom nanozymes have high atom utilization and high reactivity. Here, we prepared Cu single-atom nanozymes (Cu-NC) with excellent peroxidase-like activity by high-temperature pyrolysis using Cu as a transition metal source. The introduction of Cu formed the Cu-N x active site, which accelerated charge transfer between the reactants and the active site and was the key for improving the activity. With Cu-NC as a catalyst, H 2 O 2 rapidly oxidized 3,3′,5,5′-tetramethylbenzidine (TMB) to oxTMB, and the solution turned blue with strong absorption at 652 nm. Because d -penicillamine (D-PA) can reduce oxTMB or react with reactive oxygen species radicals to inhibit the color reaction, we built a colorimetric sensing platform around Cu-NC for the determination of D-PA and successfully used it for the determination of D-PA in urine samples. This work provides new ideas for the design of high-performance nanozymes and the detection of D-PA in real environments.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 45
·31518-31525
·
IF 10.7
Qiyan Sun,Yu Miao,Ruixue Zhang,Guang-Rui Xu,Chuanfang Zhang,Kang Liu,Zexing Wu,Lei Wang
Water electrooxidation in proton exchange membrane (PEM) water electrolyzers has been considered to be a four-electron pathway mechanism, which leads to inherent sluggish kinetics that severely limits the scalable production of high-purity H2. Herein, cobalt phosphide/iron phosphide (Co2P/FeP) nanosheets with electron redistribution through aerogel-assisted and gas-phase phosphorization strategies have been reported. Benefiting from the unique nanosheet structure and electron redistribution induced by p–d hybridization interaction, the as-obtained Co2P/FeP nanosheets display outstanding alkaline oxygen evolution reaction (OER) performance. Co–P and Fe–P charge bridges trigger p–d orbital hybridization between the transition metal and P elements, which downshifts the d-band center of Co2P/FeP nanosheets and accelerates the formation of *OOH with a lower energy barrier that can expedite the water electrooxidation process with an overpotential of 257 mV to reach the 10 mA cm−2 current density and a Tafel slope of 39.6 mV dec−1. This work provides a deep insight into understanding the remarkable OER properties of transition metal phosphates by electron redistribution.
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ANALYTICAL LETTERS
·
2024
·
IF 1.6
Jin-Wen Liu,Tingting Chen,Meiqun Cai,Yingfeng Qin,Mei Li
Accurate, rapid, and quantitative detection of D-penicillamine (D-PA) in pharmaceutical formulations is imperative for drug quality and clinical medication guidance. Various colorimetric and fluorescent assays have been constructed for D-PA based on nanomaterials. However, the reliable and rapid detection of D-PA in pharmaceutical formulations remains a challenge because these methods suffer from shortcomings such as time-consuming procedures, poor uniformity, and complicated nanomaterial preparation. In this work, an effective and facile homogeneous dual-mode optical sensing strategy was established based on the strong complexation between D-PA and Cu2+ and catalyzed the oxidation of O-phenylenediamine. This platform displayed a sensitive response to D-PA from 5 to 100 µmol/L, with a detection limits of 0.54 µmol/L (fluorescence) and 0.76 µmol/L (colorimetry). As expected, the method was successfully applied to the determination of D-PA in pharmaceutical formulations with satisfactory results. Overall, this developed strategy provides a facile and rapid dual-mode optical platform for D-PA and has great potential in D-PA-related pharmaceutical quality control.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Fang Li,Haili Lin,Huiqin Yu,Xuemei Jia,Shifu Chen,Jing Cao
Replacing the sluggish oxygen evolution reaction with the oxidation of benzyl alcohol to construct the hybrid water electrolysis system has been attractive for its merits of environmentally friendly and economically efficient. However, the activity of the catalyst to oxidize alcohols needs to be further improved. Tailoring the d-band center (E d ) has been proven as an effective method to promote the hydrogen evolution reaction (HER). How feasible is this strategy in the oxidation of benzyl alcohol? Here, using Co 2 C as a research platform, the doping nonmetal heteroatom (P, S, N) engineering is adopted to promote its electrocatalytic BA oxidation and HER performance. The results of electrochemical tests show that the P-doped Co 2 C (P–Co 2 C) only requires a low potential of 1.33 and 1.38 V vs. RHE to achieve current densities of 20 and 100 mA cm −2 for BA oxidation, which is superior to that of S–Co 2 C, N–Co 2 C, and pristine Co 2 C. The conversation and faradaic efficiency for BA is up to 98.1% and 93.8% during ten consecutive cycle tests. The P–Co 2 C also exhibited outstanding activity and stability toward HER. The density functional theory (DFT) calculation revealed that specified P doping could modify the d-band center of Co 2 C approaching the peak of the volcano map (electrochemical overpotentials ∼ E d ). The Gibbs free energy of the BA oxidation was also reduced, thus optimizing the adsorption and desorption process of intermediates. On the other hand, the catalyst surface physical properties of Co 2 C such as hydrophilicity was promoted by the doped heteroatoms which was favorable for the gas-liquid-solid triphase electrocatalytic reaction. This work offers a facial perception of regulating the d-band to design advanced bifunctional electrocatalysts for organic matter oxidation and HER.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2012
·
IF 2.237
Shimin Kang,Xianglan Li,Juan Fan,Jie Chang
Hydrothermal carbonization of cellulose, lignin, d-xylose (substitute for hemicellulose), and wood meal (WM) was experimentally conducted between 225 and 265 °C, and the chemical and structural properties of the hydrochars were investigated. The hydrochar yield is between 45 and 60%, and the yield trend of the feedstock is lignin > WM > cellulose > d-xylose. The hydrochars seem stable below 300 °C, and aromatic structure is formed in all of these hydrochars. The C content, C recovery, energy recovery, ratio of C/O, and ratio of C/H in all of these hydrochars are among 63–75%, 80–87%, 78–89%, 2.3–4.1, and 12–15, respectively. The higher heating value (HHV) of the hydrochars is among 24–30 MJ/kg, with an increase of 45–91% compared with the corresponding feedstock. The carbonization mechanism is proposed, and furfural is found to be an important intermediate product during d-xylose hydrochar production, while lignin hydrothermal carbonization products are made of polyaromatic hydrochar and phenolic hydrochar. The formation of microspheres on the surface of cellulose and WM hydrochars is discussed, and transformation of the hemicellulose should be the reaction for WM microsphere production.
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Journal of Materials Chemistry B
·
2024
·
IF 6.1
Fengyuan Liu,Jiashan Xia,Chun Tao,Changmei Chen,Xiangshu Cheng,Rongchun Yi,Lulu Wang,Yue Wang,Tao Deng
Chirality is a ubiquitous phenomenon in nature. The advent of nanomaterials has led to a gradual evolution of chiral studies from the molecular scale to the nanoscale. The emergence of carbon dots (CDs) has inaugurated a novel domain in the scientific and technological realms of carbon nanomaterials. In recent years, CDs have attracted increasing attention due to their luminescent properties, excellent biocompatibility and remarkable bioactivity. However, little attention has been paid to the chirality of the CDs and, in particular, the differences between CDs synthesized from racemic compounds and other chiral CDs, as well as the differences in the biological effects of chiral CDs, remain to be explored. Here, chiral CDs were synthesized from L-/D-/DL-arginine, and the differences in various aspects of chiral CDs were evaluated. We found that L-CDs without extreme differences in structure had brighter fluorescence and a more significant ability of NO generation and lipid droplet inhibition than the other two chiral CDs. Combined with its better drug loading and release ability, we validated its superior efficacy in tumor treatment. Therefore, this study provides a basis for further research on chiral carbon dots and their differences.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yu Sun,Siyu Zuo,Ziye Li,Ping Li,Jianshe Hu
With mercury pollution causes serious threats to ecosystems and human health because of its extreme toxicity and bioaccumulation, the development of efficient removal technologies has become an urgent environmental priority. This study introduces a novel adsorbent thiazolo[5,4- d ]thiazole conjugated microporous polymer (TzTzCMP) for efficient Hg(II) removal from wastewater. TzTzCMP synthesized via condensation of dithiocarbamate and triformyl-phenol, exhibits a coral-like porous structure with a high specific surface area of 436.86 m 2 /g and sulfur-rich active sites containing 15.15 wt% sulfur, enabling exceptional Hg(II) adsorption. Experiments demonstrated rapid kinetics, reaching equilibrium within 10 min, and a maximum adsorption capacity of 1050 mg/g. The adsorption kinetics and isotherm data for Hg(II) on TzTzCMP are well described by the pseudo-second-order and Langmuir models, respectively, indicating that chemical interactions dominate the adsorption process. The material maintained >95 % efficiency over five regeneration cycles and showed good selectivity under coexisting ion interference, attributed to Hg(II) coordination with N/S atoms in TzTzCMP, as confirmed by X-ray Photoelectron Spectroscopy (XPS) analysis and density functional theory (DFT) calculations. Fixed-bed column tests achieved 99.99 % removal, reducing effluent concentration to 1 μg/L and meeting drinking water standards. Combining high adsorption capacity and removal rate, rapid adsorption efficiency, good stability and reusability, TzTzCMP presents a promising solution for industrial Hg(II)-contaminated wastewater treatment.
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Food Science and Human Wellness
·
2024
·
IF 5.6
Lan Li,Shengye Yang,Xinyu Liang,Yameng Liu,Hualing Xu,Xiaozhen Guo,Cen Xie,Xiaojun Xu
Non-alcoholic fatty liver disease (NAFLD) is the main cause of chronic liver disease worldwide. Bupleurum is widely used in the treatment of non-alcoholic fatty liver, and saikosaponin D (SSD) is one of the main active components of Bupleurum. The purpose of this study was to investigate the efficacy of SSD in the treatment of NAFLD and to explore the mechanism of SSD in the improvement of NAFLD based on “gut-liver axis”. Our results showed that SSD dose-dependently alleviated high fat diet-induced weight gain in mice, improved insulin sensitivity, and also reduced liver lipid accumulation and injury-related biomarkers aspartate aminotransferase (AST) and alanine aminotransferase (ALT). Further exploration found that SSD inhibited the mRNA expression levels of farnesoid X receptor ( Fxr ), small heterodimer partner ( Shp ), recombinant fibroblast growth factor 15 ( Fgf15 ) and apical sodium dependent bile acid transporter ( Asbt ) in the intestine, suggesting that SSD improved liver lipid metabolism by inhibiting intestinal FXR signaling. SSD can significantly reduce the gut microbiota associated with bile salt hydrolase (BSH) expression, such as Clostridium . Decreased BSH expression reduced the ratio of unconjugated to conjugated bile acids, thereby inhibiting the intestinal FXR. These data demonstrated that SSD ameliorated NAFLD potentially through the gut microbiota-bile acid-intestinal FXR pathway and suggested that SSD is a promising therapeutic agent for the treatment of NAFLD.
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Journal of the American Chemical Society
·
2024
·
IF 14.4
Liu Lin,Yunming Xu,Yiting Han,Ruikun Xu,Tongyue Wang,Zemin Sun,Zhenhua Yan
A deep understanding of the mechanism for the spin-magnetic effect on O–H cleavage is crucial for the development of new catalysts for water oxidation. Herein, we designed and synthesized the crystalline Fe-DABDT and Co-DABDT (DABDT = 2,5-diaminobenzene-1,4-dithiol) and optimized an effective magnetic moment to explore the role of the spin-magnetic effect in the regulation of water oxidation activity. It can be found that the OER activity of the catalyst is positively correlated with its effective magnetic moment. Under the external magnetic field, Fe-DABDT with more spin single electrons has a stronger spin-magnetic response to water oxidation than Fe/Co-DABDT and Co-DABDT. The increase in OER current of Fe-DABDT is nearly 2 times higher than that of Co-DABDT. Experimental and density functional theory studies show that magnetized Fe sites could realize nucleophilic reaction, accelerate the polarization of electron spin states, and promote the polar decomposition of O–H and the formation of the O–O bond. This study provides mechanistic insight into the spin-magnetic effect of oxygen evolution reaction and further understanding of the spin origin of catalytic activity, which is expected to improve the energy efficiency of hydrogen production.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yunheng Wang,Hengle Wang,Tiantian She,Renjie Wang,Zhe Xu,Qiuyi Ji,Shaogui Yang,Limin Zhang,Huan He
Transition metals (TMs) are widely employed to improve poor intrinsic activity of biochar for peroxymonosulfate (PMS) activation towards water purification. However, the mechanistic effects of TMs on carbon substrates requires further understanding. Herein, we constructed TM-modified C-Ni and C-Ni-Co catalysts via simple pyrolysis of rice husk precursor, optimizing carbonaceous morphologic and electronic structures. The Co-Ni-Co (0.013 min −1 ) exhibited over 10 times higher performance than pristine biochar for iohexol (IOH) removal. Systemic spectroscopic and electrochemical measurements indicate that embedded Ni increases graphitization degree facilitating IOH adsorption by π-π conjugated attraction. And, the anchored Co enhances work function promoting electron extraction for selective generation of 1 O 2 . The interfacial d-p orbital hybridization increases the acidic degree on biochar for PMS adsorption, accelerating electron exchange for PMS activation. Our work attempts to study the complex interaction between carbon and metal sites by orbital hybridization to design efficient PMS activators for Fenton-like decontamination.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2024
·
IF 5.7
Wenting Wang,Zi Wang,Zhaojie Meng,Shuang Jiang,Zhi Liu,Hong-yan Zhu,Xin-dian Li,Jing tian Zhang,Wei Li
The current study aimed to assess the effectiveness of pharmacological intervention with Platycodin D (PD), a critically active compound isolated from the roots of Platycodon grandiflorum, in mitigating cardiotoxicity in a murine model of type 2 diabetes-induced cardiac injury and in H9c2 cells in vitro. Following oral administration for 4 weeks, PD (2.5 mg/kg) significantly suppressed the elevation of fasting blood glucose (FBG) levels, improved dyslipidemia, and effectively inhibited the rise of the cardiac injury markers creatine kinase isoenzyme MB (CK-MB) and cardiac troponin T (cTnT). PD treatment could ameliorate energy metabolism disorders induced by impaired glucose uptake by activating AMPK protein expression in the DCM mouse model, thereby promoting the GLUT4 transporter and further activating autophagy-related proteins. Furthermore, in vitro experiments demonstrated that PD exerted a concentration-dependent increase in cell viability while also inhibiting palmitic acid and glucose (HG-PA)-stimulated H9c2 cytotoxicity and activating AMPK protein expression. Notably, the AMPK activator AICAR (1 mM) was observed to upregulate the expression of AMPK in H9c2 cells after high-glucose and -fat exposure. Meanwhile, we used AMPK inhibitor Compound C (20 μM) to investigate the effect of PD activation of AMPK on cells. In addition, the molecular docking approach was employed to dock PD with AMPK, revealing a binding energy of −8.2 kcal/mol and indicating a tight interaction between the components and the target. PD could reduce the expression of autophagy-related protein p62, reduce the accumulation of autophagy products, promote the flow of autophagy, and improve myocardial cell injury. In conclusion, it has been demonstrated that PD effectively inhibits cardiac injury-induced type 2 diabetes in mice and enhances energy metabolism in HG-PA-stimulated H9c2 cells by activating the AMPK signaling pathway. These findings collectively unveil the potential cardioprotective effects of PD via modulation of the AMPK signaling pathway.
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