JOURNAL OF POWER SOURCES
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2022
·
IF 9.794
Guo Liu,Qi Zeng,Xinyi Sui,Shuhao Tian,Xijuan Li,Qingfeng Wu,Xukun Wang,Kun Tao,Erqing Xie,Zhenxing Zhang
The commercialization of lithium-sulfur battery (LSB) is seriously limited by the shuttling effect and sluggish reaction kinetics. Metal chalcogenides have been widely used as catalysts to enhance electrochemical performance, but the modulation essence of these non-metal anions is unclear. Herein, cubic manganese chalcogenides (MnO, MnS, MnSe) with fixed cation (Mn) and various anions (O, S, Se) are synthesized, and the anion effect on the performance of LSBs is systematically investigated. Based on the complementary experimental characterization and advanced theoretical calculations, it is clear that the interfacial redox reaction dynamics are governed by the catalytic activity of manganese chalcogenides, while the catalytic activity is modulated by the gap between the d-band of cation and p-band of anion (Δd-p). Among these manganese chalcogenides, Se has the largest atom radius and lowest electronegativity , which makes the p-band center of Se move to the Fermi level , thus increasing the electron's energy to react. Consequently, the LSBs based on MnSe catalyst exhibit the best rate (613.5 mAh g −1 at 4C) and cyclic performance (847.5 mAh g −1 after 250 cycles at 0.2C). This comparative study may encourage more effort and provide a new paradigm for developing highly effective catalysts for high-performance LSBs.
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高影响因子
RSC Advances
·
2022
·Vol. 12
·期 19
·11967-11973
·
IF 4.036
Yafeng Zhang,Huizhen Wang,Hu Yu,Xiaoxia Sun
Phenylalanine an essential aromatic amino acid for humans and animals, cannot be synthesized by humans and animals on their own. However, it synthesizes important neurotransmitters and hormones in the body and is involved in gluconeogenesis and lipid metabolism. Moreover, the two opposite configurations of phenylalanine have different activities. For example, L-phenylalanine is a biologically active optical isomer involved in crucial biological processes, the lack of which will lead to intellectual disability, while D-phenylalanine only acts as a chiral intermediate. In this research, an H8-BINOL chiral fluorescent sensor modified with 1,2,3-triazole was synthesized in high yield (95%) by nucleophilic substitution and click reaction. The chiral fluorescent sensor showed high enantioselectivity toward phenylalanine. L-Phenylalanine enhanced the fluorescence response of the probe significantly, while D-phenylalanine had no obvious fluorescence response change. The enantioselective fluorescence enhancement ratio [ef = (IL − I0)/(ID − I0), where I0 is the fluorescence of the sensor without amino acids] for the highest fluorescence intensity at 20.0 equivalents of amino acids was 104.48. In this way, the probe could be used to identify and differentiate different configurations of phenylalanine.
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BIOORGANIC CHEMISTRY
·
2025
·
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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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Zhaoqian Yan,Zhihao Sun,Kaicheng Yue,Anran Li,Lei Qian
Cobalt oxide (CoO) with high theoretical capacity is a potential anode material for lithium ion batteries (LIBs), however its application is limited by high cost and volume expansion. Considering the cheapness of Zn and advantages of bimetallic oxide compounds, CoO/ZnO nanoclusters immobilized on N-doped 3 D reduced graphene oxide (CoO/ZnO-NrGO) were constructed by facile solvothermal and freeze-drying method as the LIBs anode for improving lithium (Li) ions storage. Three-dimensional conductive network structure not only reduced the volume expansion of CoO and ZnO but also accelerated the transfer rate of Li ions. Besides, nitrogen doping provided more active sites for plentiful Li ions storage. Phase composition and microstructure of CoO/ZnO-NrGO were measured by X-ray photoelectron spectroscopy, transmission electron microscopy , Raman spectroscopy , X-ray diffraction and so on. Synchronously, electrochemical property of CoO/ZnO-NrGO was also tested. It was found that the specific capacity of CoO 1.2 /ZnO 0.6 -NrGO 6.78 was 1494 mA h g −1 at 0.1 A g −1 , higher that of other bimetallic oxides such as CoO–MnO, CoO–Co 3 O 4 , CoO–CoFe 2 O 4 and so on. The capacity of CoO 1.2 /ZnO 0.6 -NrGO 6.78 was maintained approximately 600 mA h g −1 at 2.0 A g −1 after 1000 cycles. Taking these advantages into account, composites of bimetallic oxides and carbon material with high specific capacity provide a novel idea for a new generation of LIBs.
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Feng Du,Zhikun Yao,Jikai Xiang,Jingsha Li,Changhong Wang,Chunmei Zhang,Tao Hu,Jinlong Liu,Changming Li,Chunxian Guo
To design high-performance electrocatalysts with desired electronic structures is critical to facilitate the conversion of pollutant nitrate (NO 3 − ) to value-added ammonia (NH 3 ) at ambient condition. Nevertheless, the current electrocatalysts for NO 3 − -to-NH 3 still face low Faradaic efficiency and selectivity. We present here a heteroatoms co-doped strategy using phosphorus (P) and oxygen (O) to tune electronic structure of copper (Cu) nanocrystals to form highly active surface for selective NO 3 − -to-NH 3 . By combing experimental results and theoretical calculation, it is found that the heteroatom P, O-doping can negatively shift the Cu d -band center, which optimizes adsorption energies of intermediates, especially for *NO 3 − and *NH 3 . The P, O-doped Cu nanocrystal exhibits an efficient 8-electron transfer process for NO 3 − -to-NH 3 . It achieves both high NO 3 − conversion rate (91.09 %) and NH 3 Faradaic efficiency (91.72 %) in high concentration NO 3 − electrolyte (1.0 M KOH + 1400 ppm NO 3 − -N), retaining its potential applications in practical NO 3 − -to-NH 3 .
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高影响因子
PeerJ
·
2019
·
IF 2.353
Hongli Yin,Ji Ma,Jichun Han,Maoru Li,Jing Shang
Background Quercetin (Qr), isoquercitrin (IQ), and quercetin-3-O-β-D-glucuronide (QG) are powerful phytochemicals that have been shown to exhibit disease prevention and health promotion properties. However, there may exist transformations between Qr, IQ, and QG in vivo . And the pharmacokinetic profiles of Qr, IQ, and QG have not been systematically compared. The pharmacokinetics study would be helpful to better understand the pharmacological actions of them. Methods Herein, we developed a reliable HPLC-MS method to compare the pharmacokinetics of Qr, IQ, and QG after separate (50 mg/kg) oral administration of them in rats, using puerarin as internal standard. The detection was performed using negative selected ion monitoring. This method was validated in terms of selectivity, linearity, precision, accuracy, extraction recovery, matrix effect, and stability; and shows reliabilities in monitoring the pharmacokinetic behaviors of these three compounds. Results Our results showed that after separate oral administration of Qr, IQ, and QG, all of the compounds could be detected in plasma. In addition, QG could be detected in the Qr group; Qr and QG could be measured in the IQ group; and Qr could be found in rat plasma after 1.5 h of QG administration. Moreover, the AUC 0− t of Qr in the; Qr group (2,590.5 ± 987.9 mg/L*min), IQ group (2,212.7 ± 914.1 mg/L*min), and QG group (3,505.7 ± 1,565.0 mg/L*min) was larger than the AUC 0− t of QG in the; Qr group (1,550.0 ± 454.2 mg/L*min), IQ group (669.3 ± 188.3 mg/L*min), and QG group (962.7 ± 602.3 mg/L*min). The AUC 0− t of IQ was the lowest among all groups. Discussion Quercetin, IQ, and QG can all be absorbed into plasma. A mutual transformation exists between Qr and QG, and IQ can be metabolized into Qr and QG in SD rats. These results would provide a meaningful basis for understanding the pharmacological actions of these three compounds.
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PubMed
高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 26
·期 2
·979-991
·
IF 9.8
Shipeng Chen,Jinping Wang,Li Feng,Zebin Song,Xiaoji Wang,Yubin Ke,Lin Hua,Yange Fan,Zheng Li,Yimin Hou,Baoyu Xue,Luke Liu
To prevent the entry of toxic sulphur-containing contaminants into the atmosphere, extractive desulphurization of fuels with an ionic liquid (IL) as an extractor is a benign and efficient strategy, as compared with traditional hydrodesulphurization. However, ILs have some drawbacks like toxicity, non-biodegradability, low recyclability, and partial solubility in the fuel (leading to contamination), which limit their practical applications. Supramolecular ionogels, obtained from the gelation of ILs, not only retain the desulphurization function of ILs, but also prevent the leakage and achieve the renewable utilization of ILs. Hence, they are effective in overcoming the abovementioned limitations. Herein, a series of efficient D-gluconic acetal-based gelators (NG6, 12, 18 and NGO18) that can harden four different ILs at low concentrations was developed. They were thermally reversible and stable at room temperature with self-healing properties. The gelation and self-healing mechanisms of these gels were also systematically investigated. Furthermore, their desulphurization capacities in fuel-mimicking solutions of thiophene (T), benzothiophene (BT) and dibenzothiophene (DBT) in hexane were investigated. The effects of the concentration of sulphur compounds, fuel volume and temperature on the efficiency of sulphur removal were studied. Interestingly, the NG18-IL2 ionogel was the best-performing, which showed outstanding mechanical properties and fast and complete self-healing characteristics, along with 40.99, 49.76 and 51.68% removal efficiencies for T, BT and DBT, respectively, and 100% for T, BT and DBT in a multi-stage approach. Additionally, the ionogel could be reused six times and regenerated, all of which make it a low-cost and environment-friendly desulphurization material for practical applications.
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高影响因子
CARBONATES AND EVAPORITES
·
2018
·Vol. 34
·期 3
·1131-1139
·
IF 0.947
Li Zhenxuan,Xiao Jiangtian,Huang Lidong,Xu Defu,Liu Dagang,Sun Xiaowen,Yu Luji,Wu Hongsheng
Succinic acid and l -malic acid are known to affect calcite dissolution/crystallization due to their tendency to adsorb on calcite’s surface. Taking into account the structural similarity among succinic acid, l -malic acid, and d -malic acid, a comparative study of their adsorption behavior on calcite was investigated for clarifying their adsorption mechanism. Kinetic results showed that l -malic acid adsorption reached equilibrium within 12 h, while succinic acid required 48 h. Results from the pH effect study showed that the strength of surface complex of succinic acid on calcite was weaker, even compared to its aqueous complex with Ca 2+ ion. Alternately, l -malic acid exhibited a much stronger surface complex strength, even compared to its aqueous complex with Ca 2+ ion. The adsorption isotherm results indicated that the saturated adsorption amount of l -malic acid was twice that of succinic acid, suggesting the surface complex of succinic acid may occupy a larger space on calcite surface compared to that of l -malic acid. Based on these results and those from previous studies, we proposed that succinic acid adsorption is through its two carboxyl groups binding to two adjacent surface sites (> Ca + ), and not only one. Also, l -malic acid adsorption occurs through one carboxyl group and one hydroxyl, which forms a “claw” on calcite surface. The similar adsorption behavior between l -malic acid and d -malic acid reinforces this proposition for l -malic acid adsorption mechanism. Our study will serve as good reference information to provide better understanding into the adsorption of other carboxylic acids on calcite.
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高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
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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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
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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高影响因子
Inorganic Chemistry Frontiers
·
2025
·
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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产品关联
DOI
高影响因子
Journal of Macromolecular Science Part B-Physics
·
2017
·
IF 0.828
Qiao Zhang,Zhihua Zhou,Cheng Peng,Tianlong Huang,Wenjuan Liu,Qingquan Liu,Hu Zhou,Wei Wang,Hua Yan
Three-dimensional biodegradable porous scaffolds play an important role in tissue engineering. A new polymer based on maleated poly(lactic-co-glycolic acid) (MPLGA) was synthesized using direct melt copolymerization from maleic anhydride (MAH), D, L-lactide, and glycolide monomers. MPLGA porous biodegradable scaffolds were prepared by a solution-casting/salt-leaching method. The effects of content and size of the NaHCO3 porogen on the compressive strength of the MPLGA scaffolds were investigated, and the effect of content of the porogen on the porosity of the MPLGA scaffolds was also studied. The results indicated that MAH was grafted onto PLGA successfully and MPLGA scaffolds with interconnective and open pore structure were obtained. Increasing content of NaHCO3 porogen resulted in an increase of porosity and decrease of the compressive strength of the MPLGA scaffolds with the compressive strength of the scaffolds also decreasing with increasing porogen size.
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高影响因子
危险品化学品经营许可证（带存储）