Nature Communications
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2024
·Vol. 15
·期 1
·1-13
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IF 14.7
Xue Dongping,Yuan Yifang,Yu Yue,Xu Siran,Wei Yifan,Zhang Jiaqi,Guo Haizhong,Shao Minhua,Zhang Jia-Nan
Disentangling the limitations of O-O bond activation and OH* site-blocking effects on Pt sites is key to improving the intrinsic activity and stability of low-Pt catalysts for the oxygen reduction reaction (ORR). Herein, we integrate of PtFe alloy nanocrystals on a single-atom Fe-N-C substrate (PtFe@Fe SAs -N-C) and further construct a ferromagnetic platform to investigate the regulation behavior of the spin occupancy state of the Pt d -orbital in the ORR. PtFe@Fe SAs -N-C delivers a mass activity of 0.75 A mg Pt −1 at 0.9 V and a peak power density of 1240 mW cm −2 in the fuel-cell, outperforming the commercial Pt/C catalyst, and a mass activity retention of 97%, with no noticeable current drop at 0.6 V for more than 220 h, is attained. Operando spectroelectrochemistry decodes the orbital interaction mechanism between the active center and reaction intermediates. The Pt dz 2 orbital occupation state is regulated to t 2g 6 e g 3 by spin-charge injection, suppressing the OH* site-blocking effect and effectively inhibiting H 2 O 2 production. This work provides valuable insights into designing high-performance and low-Pt catalysts via spintronics-level engineering.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ting Zhang,Wantong Zhao,Shiyan Li,Wenguang Cui,Baojun Wang,Yuefeng Liu,Riguang Zhang,Zhongkui Zhao
Selective transfer hydrogenation coupling of nitroarenes with benzyl alcohol is one of the most reliable strategies to access functionalized imines, but challenges remain, such as the multiple and complicated operate process, low reactivity, poor selectivity results from deep hydrogenation. Constructing highly efficient catalyst is critical for this organic transformation process. Herein, we propose a unique single-atom Co-N 4 sites on N-doped carbon, with significantly upshifted d -band center, fabricated by a one-pot solid-phase carbonization strategy, which generates an excellent catalyst for one-pot selective transfer hydrogenation coupling of nitroarenes with benzyl alcohol to various functionalized imines. Experimental and theoretical investigations demonstrate the clear linear correlation among the nitrobenzene turnover number ( TON ) and d -band center over the as-prepared Co based samples, indicating the vital effect of electronic structure of Co sites on catalytic performances. Furthermore, owing to the upshifted d -band center of Co-N 4 sites, thedesorption of aniline and N -benzylideneaniline is promoted, which accelerates the spontaneous condensation coupling of aniline with benzaldehyde and inhibits the deep hydrogenation of N -benzylideneaniline. Consequently, an outstanding catalytic performance with high activity and selectivity in transfer hydrogenation coupling for imine synthesis has been realized. This work not only presents a highly efficient non-precious metal catalyst for functionalized imines production, but also illustrates the critical effect of electron structure of metallic active site on catalytic properties and opens a new avenue for fabricating diverse single-atom catalysts for selective hydrogenation reactions.
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Inorganic Chemistry Frontiers
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2025
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IF 6.4
Ruichen Geng,Lin Su,Xiaojun Chu,Zhihan Zhang,Ranran Wei,Yinglong Wang,Shuli Yin
Developing electrocatalysts with high activity and selectivity to promote the oxidation of 5-hydroxymethylfurfural (HMF) holds substantial importance yet presents challenges in the realm of biomass upgrading. Herein, the defect-rich high-entropy alloy AuCuAgRuNi nanofibers (AuCuAgRuNi NFs) were synthesized via a facile one-pot wet chemical synthesis. Remarkably, the AuCuAgRuNi NFs demonstrate exceptional electrocatalytic performance for HMF-to-FDCA conversion under ambient conditions, achieving 97.15% yield and 98.40% selectivity with outstanding stability. Theoretical calculations reveal that defect-induced electronic modulation optimizes reactant adsorption, while d-orbital hybridization among multi-metallic components facilitates electron redistribution, synergistically enhancing catalytic activity. Furthermore, HMF oxidation has been successfully integrated with hydrogen evolution in a flow electrolysis cell, and an energy-efficient coupled system has been established, which holds promise for scalable biomass valorization. This research provides valuable insights into the innovative synthesis and inherent catalytic mechanisms of high-entropy alloy systems.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2025
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IF 3.8
Wang Sikai,Liu Weiping,Wang Lei,Lv Lin,Liu Xiangqin,Luo Xiaojun,Zhang Guoqi,Zhao Yan
d -Galactose (D-Gal), an essential monosaccharide, plays multiple physiological roles in living organisms. Abnormal fluctuations in its concentration are closely associated with various genetic metabolic disorders, such as galactosemia and galactose deficiency. Therefore, the development of an efficient, sensitive, and accurate method for D-Gal detection is critical for disease diagnosis and treatment. In this study, a ratiometric fluorescence-based sensing platform was constructed for the quantitative detection of D-Gal. Galactose oxidase can catalyze the oxidation of D-Gal, resulting in the generation of hydrogen peroxide (H 2 O 2 ). When combined with WSe 2 nanosheets prepared via liquid-phase exfoliation and functioning as nanozymes, in the presence of H 2 O 2 , the substrate o -phenylenediamine (OPD) undergoes oxidation to generate 2,3-diaminophenazine (DAP), which exhibits a fluorescence peak at 570 nm. Simultaneously, DAP quenches the fluorescence of carbon dots (CDs) at 430 nm via an inner filter effect, thereby enabling ratiometric detection with enhanced accuracy and sensitivity. The method exhibits a Limit of detection of 0.004 mM, Linear ranges spanning from 0.01 to 1 mM and from 1 to 300 mM, with recoveries ranging between 91.0 and 100.4%. Furthermore, the proposed method was effectively utilized for the detection of D-Gal in human serum specimens, demonstrating excellent selectivity and reliability. This research presents a novel method for D-Gal detection based on WSe 2 nanosheets and CDs, offering potential applications in the biomedical and biosensing fields. Graphical abstract
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MICROCHEMICAL JOURNAL
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2025
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IF 5.1
Jing Zhang,Ye Yang,Yi-Ping Liu,Guo-Cong Liu,Xi Zhu,Xin-Yu Jiang,Jin-Gang Yu
Electrochemical sensors have been considered as one of the most important methods to determine amino acid (AA) enantiomers. An interesting and highly-efficient electrochemical sensor, gold nanoparticles/D-sorbitol modified glass carbon electrode (Au NPs/D-sorbitol/GCE), was developed for the chiral recognition of Tyrosine (Tyr) enantiomers. Au NPs/D-sorbitol/GCE sensor exhibited excellent chiral recognition efficiency for Tyr enantiomers (I L /I D = 1.99, ∆Ep = 36 mV) by square wave voltammetry (SWV). The possible recognition mechanism was also proposed by cyclic voltammetry (CV) at different scanning rates, wettability measurements, and density-functional theory (DFT) calculations. The smaller steric hindrance and more suitable molecular distance are beneficial to the selective formation of hydrogen bonds between L-Tyr and the chiral interface of the sensor. The energy difference caused by the formation of hydrogen bonds between the chiral interface and Tyr enantiomers can be expressed as different peak currents to achieve chiral recognition. The redox peak current of Tyr enantiomers at Au NPs/D-sorbitol/GCE showed good linear relationship with their concentration, and the limits of detection (LOD) were calculated to be 4.12 μM and 8.07 μM for L-Tyr and D-Tyr, respectively. Importantly, Au NPs/D-sorbitol/GCE can also predict the mass ratios of L-Tyr in the enantiomeric mixtures. In addition, the sensor has shown good anti-interference ability, high stability, and excellent reproducibility.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Yang Yang,Zhu Xiaojuan,Wang Lili,Lang Junyu,Yao Guohua,Qin Tian,Ren Zhouhong,Chen Liwei,Liu Xi,Li Wei,Wan Ying
Pd catalysts are widely used in alkynol semi-hydrogenation. However, due to the existence of scaling relationships of adsorption energies between the key adsorbed species, the increase in conversion is frequently accompanied by side reactions, thereby reducing the selectivity to alkenols. We report that the simultaneous increase in alkenol selectivity and alkynol conversion is achieved by manipulating interstitial atoms including B, P, C, S and N in Pd catalysts. A negative linear relationship is observed between the activation entropies of 2-methyl-3-butyn-2-ol and 2-methyl-3-buten-2-ol which is highly related to the filling of d -orbital of Pd catalysts by the modification of p -block elements. A catalyst co-modified by B and C atoms has the maximum d charge of Pd that achieves a 17-fold increase in the turn-over frequency values compared to the Lindlar catalysts in the semi-hydrogenation of 2-methyl-3-butyn-2-ol. When the conversion is close to 100%, the selectivity can be as high as 95%.
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RARE METALS
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2025
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IF 11
Huang De-Xuan,Zhao Jian-Wei,Hu Xue-Lei,Liu Tong
Transition metal oxides have garnered significant attention as electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER). However, their sluggish reaction kinetics and poor stability hinder commercial applications. Herein, we report the synthesis of a bimetallic cobalt manganese oxide, Co 0.99 Mn 2.01 O 4 (CMO), synthesized via a hydrothermal technique, which serves as a highly efficient bifunctional ORR/OER electrocatalyst owing to its impressive half-wave potential of 0.767 V and low overpotential of 1.677 V at 10 mA cm −2 . Theoretical calculations revealed that the d-band centers of Co 3d and Mn 3d in CMO, located at tetrahedral and octahedral sites, are positioned near the Fermi level, facilitating the adsorption of electrocatalytic intermediates. Furthermore, the distance between the Co 3d and O 2p band centers in CMO is smaller than that in Co 3 O 4 , and the distance between the Mn 3d and O 2p band centers in CMO is shorter than that in Mn 2 O 3 , indicating that the Co–O and Mn–O bonds in CMO exhibit greater covalency, significantly enhancing ORR/OER activity. Notably, CMO serves as an advanced air electrode material for rechargeable zinc-air batteries (ZABs), demonstrating improved charge–discharge performance with a low voltage gap of 0.87 V at 5 mA cm −2 , high peak power density of 124 mW cm −2 , and excellent cycle stability of over 540 h at 5 mA cm −2 . This superior ORR/OER activity, combined with the simple material combination, makes CMO a promising catalyst for rechargeable ZABs. Graphical
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2014
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IF 3.785
Yuanyuan Ding,Jingtian Han,Baocheng Tian,Jian Han,Jing Zhang,Hong Zheng,Yuzhen Han,Meishan Pei
Smart nanoparticles based on the mechanisms of asialoglycoprotein (ASGP)-mediated endocytosis and pH-induced drug release were developed for the efficient treatment of hepatoma using a newly developed copolymer, methoxy-polyethylene glycols (PEG)-b-poly ( d -galactopyranose) (MPEG-b-PMaIPG). The particles exhibited spherical shapes, uniform particle size distribution (100 ± 4.43 nm), negative zeta potential (−32.8 ± 0.23 mV), high drug loading (24.77 ± 2.68%) and encapsulation efficiency (66.12 ± 9.44%). The in vitro drug release was also investigated, resulting that the release of drug from particles depended on different pH value. In vitro cell cytotoxicity and hemolysis assays were conducted to confirm the safety of the MPEG-b-PMaIPG nanoparticles. Anticancer activity showed that DOX-loaded MPEG-b-PMaIPG nanoparticles exhibited a high antitumor activity toward HepG2 cells, which was similar to free DOX, while blank MPEG-b-PMaIPG nanoparticles were non-toxic up to a tested concentration of 1.0 mg/mL. Confocal laser scanning microscopy (CLSM) and flow cytometry (FCM) were used to verify the targeting efficiency of d -galactopyranose-modified nanoparticles. The results clearly demonstrated that d -galactopyranose-modified nanoparticles were taken up quickly by the HepG2 cells, which suggests that MPEG-b-PMaIPG nanoparticles with good biocompatibility and non-toxic for normal cells may be used as an effective cancer-targeting drug delivery system for chemotherapy.
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BIOORGANIC CHEMISTRY
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2025
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IF 4.7
Shuaishuai Cui,Cunxin Guo,Liang Yan,Yujian He,Li Wu
The incorporation of D-amino acids can influence the structure and enzymatic stability of proteins or peptides, especially when they are introduced at enzyme cleavage sites, significantly inhibiting the enzymatic hydrolysis of peptides. The abnormal accumulation of these peptides has been linked to age-related conditions, including cataracts and Alzheimer's disease. N-terminal acetylation, an essential post-translational modification, significantly enhances the physicochemical properties of peptides and plays an essential role in regulating their performance within biological systems. This research examined the impact of N-terminal acetylation on the enzymatic hydrolysis of peptides incorporating D-amino acids. Enzymatic activity assessments showed that N-terminal acetylation greatly promoted the enzymatic breakdown of these peptides by Proteinase K (PROK), with the substrate decay rate constant for the acetylated peptide Ac-6-w increasing by 17.5 times. This enhancement was specific to serine-type proteases, which exhibited a comparable cleavage pattern. Molecular docking further demonstrated that N-terminal acetylation improved interactions within the catalytic triad of serine proteases, leading to faster enzymatic degradation. The results provide novel insights into the impact of N-terminal acetylation on the enzymatic behavior of peptides incorporating D-amino acids, and they propose a potential approach for targeting these peptides to preserve normal physiological functions.
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TOXICOLOGY
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2019
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IF 3.547
Yuan Liao,Yuhao Luo,Nanjisha Ding,Juanmei Gao,Xingbao Wang,Wanhua Shen
Xylene and its derivatives are known to be neurotoxic to the central nervous system of animals. Our previous work has shown that para-xylene (PX) can cause an increase in apoptotic cells and abnormal avoidance behavior in Xenopus laevis . However, the mechanism underlying the impact of PX on neuronal structural and functional plasticity is less clear. Here, we examined the effects of PX on neuronal development and plasticity in the developing optic tectum. We found that HuC/D-positive neurons were more vulnerable than SOX2-positive progenitor cells or BLBP-positive radial glial cells after exposure to PX at 1 mM for 48 h. The further measurement of postsynaptic receptors and synaptic vesicle proteins showed that the expression levels of GluA1 and GluA2, but not Rab3a and SNAP25, were significantly decreased in the tectal brain. In vivo time-lapse images and electrophysiological recordings showed that PX exposure resulted in significant deficits in neuronal structure, particularly in the total dendritic branch length (TDBL), and visual stimulation-induced excitatory compound synaptic currents (eCSCs) without altering neurotransmitter release probability. Strikingly, coexposure to d -glucuronolactone (GA) and PX rescued the structural and functional deficits caused by PX exposure alone. Furthermore, we found that visual experience-induced structural, functional and behavioral plasticity was blocked by PX exposure, which was also rescued by the simultaneous administration of GA and PX . Thus, our findings indicate that PX is neurotoxic to brain development and plasticity and that GA may be considered a promising candidate to treat PX-induced defects in neural circuits.
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POSTHARVEST BIOLOGY AND TECHNOLOGY
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2025
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IF 6.8
Lijun Ling,Wenyue Zhang,Rui Yue,Yijuan Jiang,Fanjin Kong,Rongxiu Mo,Lijun Feng,Yongpeng Zhou
Grapes are susceptible to fungal infections before, during transport, or after harvest, causing significant economic losses. Traditional methods have high equipment costs and are prone to the development of drug resistance. The antifungal potential of volatile organic compounds (VOCs) produced by endophytic bacteria is beginning to be understood. VOCs are ideal for post-harvest disease control in fruits and vegetables, as they can work without direct contact with the fruit. In this study, we isolated pathogenic fungi ( Penicillium crustosum G-4, Alternaria alternata G-5, Arthrinium phaeospermum G-8) from post-harvest rotting green grape and used G-8 as a test organism, screened the endophytic bacterium Bacillus toyonensis D-6 from Typhonium giganteum Engl. that could produce strong antagonistic active VOCs, analyzed the components of its VOCs and screened for the highly effective inhibitory compound 3-methylvaleric acid (3-MA). The inhibitory activities and mechanisms of action of the VOCs and antifungal compounds were investigated. The results showed that the VOCs and 3-MA produced by D-6 inhibited the growth and reproduction of the pathogenic fungi, which mainly exerted antagonistic effects by destroying the normal morphological structure of mycelium and spores and damaging the integrity of cell membranes. In addition, appropriate concentrations of VOCs and 3-MA inhibited the spread of pathogenic fungi on green grapes and effectively delayed the decline in fruit quality. This opens up new possibilities for post-harvest preservation of green grapes and provides a theoretical basis for related applications.
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JOURNAL OF BIOMATERIALS APPLICATIONS
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2023
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IF 2.9
Tian Yi Wu,Wen Jie Cao,Zi Ling Li,Yan Chun Gong,Xiang Yuan Xiong
Drugs with different solubility can be selectively embedded into polymersomes with the hydrophilic core and hydrophobic bilayer. Novel folate-targeted Pluronic/poly (D,L-lactide-b-glycolide) polymersomes were constructed and used for the co-delivery of paclitaxel (PTX) and doxorubicin (DOX) to improve their inhibitory effect over cancer cells. The particle size of blank polymersomes was mainly distributed below 125 nm. The release of PTX and DOX from polymersomes showed an initial burst release followed by a sustained and slow release. The in vitro cytotoxicity data showed that the targeted co-loaded polymersomes (PTX&DOX FA-Ps) exhibited better inhibitory effect than single-loaded polymersomes and free drugs did. Furthermore, PTX&DOX FA-Ps showed the synergistic therapeutic effect over OVCAR-3 cancer cells. The cellular uptake results also showed that folate modified polymersomes had excellent targeting performance. Therefore, the folate-targeted Pluronic/poly (D,L-lactide-b-glycolide) polymersomes have potential application value as novel drug carriers to co-deliver PTX and DOX.
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