Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Chen-Xuan Li,Rui Wang,Wen Sun,Kangping Cui,Xian-Zhong Fu,Minshu Cui,Yihan Chen,Zhi Guo,Yingying Liu
Advanced oxidation systems (AOS) hold promise for tackling refractory dyes in wastewater, yet the quest for efficient systems tailored to the degradation of dye remains a formidable hurdle. Here, a novel visible-light-driven AOS, consisting of biomimetic Fe(III) salen complex (FeL, salen= N, N-bis(salicylidene)ethylenediamine) and peroxymonosulfate (PMS), was proposed for highly efficient degradation of Rhodamine B (RhB), a model dye. The proposed AOS was capable of degrading 94.8 % RhB in 40 min, outperforming the typical Fe 3+ -based system, which achieved only 52.6 % pollutant degradation under identical conditions. As indicated by experimental results and theoretical calculations, the unique Fe-N 2 O 2 coordination structure of FeL facilitated the adsorption of terminal O (O3) at PMS site, thereby enhancing the heterolysis of the O-O bond and generating high-valent iron-oxo species (i.e., Fe Ⅴ =O) rather than radicals (SO 4 •− , HO • ). The system demonstrated robust resistance to interference from environmental anions (Cl − , NO 3 − , HCO 3 − , SO 4 2− ), pH variations (initial pH 3.0–11.0) and humic acid . More attractively, it achieved 87.3 % chroma and 37.6 % chemical oxygen demand (COD) removal in real dye wastewater samples. This work may shed light on the understanding and development of biomimetic Fe complexes-based AOS for wastewater treatment .
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2025
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IF 3.1
Xiaolin Wu,Qiao Yu,Yuzhao Hou,Xuemei Zhang,Simon Sani Ocholi,Liming Wang,Ziping Yan,Jie Li,Lifeng Han
Cholestatic liver disease(CLD) is caused by impaired bile flow due to obstruction of the biliary tract, and long-term exposure to bile acids in the liver triggers inflammation, eventually leading to liver toxicity and liver fibrosis. Emodin-8- O-β -D-glucopyranoside(EG) is anthraquinone compound that is widely found in traditional Chinese medicine. It possessed antioxidative and anti-inflammatory activities. However, the effect of EG on cholestatic liver injury(CLI) has not been explored. In this study, Alpha-naphthyl isothiocyanate(ANIT)-induced CLI mice were used to investigate the anti-cholestasis and hepatoprotective effects of EG through serum biochemical index detection, non-targeted metabolomics, lipidomics, and intestinal flora 16S rRNA sequencing. The results suggested that EG restores homeostasis of the gut microbiome while regulating bile acids metabolism and lipid-related metabolic pathways to reduce liver damage in ANIT-induced cholestasis. This study provides a new perspective on the mechanism of EG, and help offer a more natural approach to managing liver damage.
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Advanced Healthcare Materials
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2024
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IF 10
Jianshuai Bao,Zengyin Li,Deliang Wang,Jiefei Wang,Guan Huang,Jianlei Qian,Xiaoyan Yang,Peng-Cheng Duan,Sheng Zhang,Feng Bai,Yong Zhong
Near-infrared second region (NIR-II) fluorescence imaging provides enhanced tissue penetration, achieving efficient NIR-II fluorescence and photoacoustic imaging (PA)-guided photothermal therapy (PTT) all in one material remains a challenging yet promising approach in cancer treatment. Herein, open-shell V═O metalloradical complex (VONc) is self-assembled into VONc nanospheres (VONc NPs). VONc NPs exhibit light absorption from 300 to 1400 nm, fluorescence spectra ranging from 900 to 1400 nm, and a distinct fluorescence signal even at 1550 nm. Moreover, VONc NPs exhibit outstanding photostability and a higher photothermal conversion efficiency of 46.6% than that of closed-shell zinc naphthalocyanine nanorods (ZnNc NRs). V═O centered metalloradical serves as transient electron-withdrawing groups to facilitate charge transfer (CT), introducing additional nonradiative energy dissipation pathways and enhancing efficient heat generation. In vitro experiments of VONc NPs indicate that a highly effective photothermal action causes harm to both mitochondria and lysosomes, resulting in the death of tumor cells, closed-shell ZnNc NPs exhibit almost no cell killing as contrast. In vivo anti-tumor therapy results of VONc NPs demonstrate excellent NIR-II fluorescence imaging-guided PTT against tumors with a favorable biosafety profile. “Centered metalloradical boosting CT” toward open-shell metal complexes provides significant insight for developing single-material integrated nanosystems for diagnostic and therapeutic applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yan Chen,Guojun Lv,Xuyang Zou,Shihao Su,Jiangzhang Wang,Chaoyi Zhou,Jialing Shen,Yangbin Shen,Zhongmin Liu
Dealuminated Beta zeolite has a large amount of silanol defects on its interface, which provides an ideal place for embedding metal species and creating metal active sites in a confined microenvironment. The confined metal sites as well as their surroundings are closely related to the reactant activation and transient state achievement. Hence, unraveling the confined metal sites is of great significance for the catalytic reaction process. Herein, niobium species were incorporated into the silanol defects over dealuminated Beta zeolite with a facile dry impregnation method, co-grinding the niobium precursor with dealuminated Beta zeolite support. The successful incorporation of niobium into the silanol defects for 30Nb-Beta zeolite was verified by DRIFT, 1 H MAS NMR, UV–Vis and UV-Raman characterizations. XAS characterization and DFT calculations further disclosed that the confined Nb species existed as (SiO) 2 Nb(OH)(=O), containing two Si−O−Nb bonds, one Nb=O bond as well as one Nb−OH bond. The synthesized 30Nb-Beta zeolite catalyst displayed a superior cyclohexene conversion of 51.1%, cyclohexene oxide selectivity of 83.1% as well as TOF value of 188.2 h −1 ascribed to the inherent electrophilicity of Nb(V) for confined (SiO) 2 Nb(OH)(=O) species as well as the low oxygen transfer energy barrier for Nb V −OOH species. Furthermore, the prepared 30Nb-Beta zeolite can be effectively employed to other cyclic alkene epoxidation reactions.
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GREEN CHEMISTRY
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2024
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IF 9.3
Jie Li,Pengpeng Shao,Weijie Geng,Peng Lei,Jing Dong,Yingnan Chi,Changwen Hu
The oxidative depolymerization of β-O-4 linkages into value-added aromatic chemicals is of great importance for lignin valorization. However, achieving highly selective and rapid cleavage of β-O-4 linkages under mild conditions remains a challenge. Herein, cobalt–cobalt oxides (Co-CoOx) supported on N-doped carbon (CoMA/C900) combined with a green and recyclable base K7HNb6O19 (KNb6) have shown remarkable activity for the one-step oxidative cleavage of lignin β-O-4 linkages. Under relatively mild conditions (100 °C, 0.2 MPa O2), a lignin β-O-4 alcohol model compound was almost completely converted within 3 h, affording a narrow product distribution of phenol (yield: 99%) and methyl benzoate (yield: 98%). Based on the control experiments, kinetic study, and spectroscopic analysis, a synergistic oxidative cleavage mechanism was proposed: CoMA/C900 activates molecular oxygen to form a superoxide radical, while basic KNb6 promotes deprotonation of secondary alcohol, and they synergistically catalyze the oxidation of β-O-4 alcohol and the rapid cleavage of Cβ–O and Cα–Cβ bonds. During the reaction, the oxidation of β-O-4 alcohol to β-O-4 ketone is the rate-determining step, while the cleavage of PP-one to phenol and methyl benzoate can be completed within 15 min. Moreover, the CoMA/C900–KNb6 catalyst is recyclable at least three times and highly active for the oxidative cleavages of other lignin models and organosolv birch lignin.
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INORGANIC CHEMISTRY
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2024
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IF 4.3
Tianhao Yu,Peng Gao,Yu Wang,Maidina Muhetaer,Hong Du
In response to the limitations of slow reaction kinetics and elevated overpotentials in the OER, a novel core–shell structured electrocatalyst, termed NiCo–ZIF-67@Fe–Co–Ni-PBA or NiCo–ZIF@PBA, has been developed. This material demonstrates exceptional catalytic performance, exhibiting a minimal overpotential of approximately 188 mV at 10 mA cm–2, alongside a Tafel slope of 109 mV dec–1. Its robust stability in a 1 M KOH solution during the OER operations is noteworthy. Theoretical insights from DFT calculations reveal that a Co–O–Fe bridging configuration within NiCo–ZIF@PBA lowers the energy barrier for the reaction to 1.79 eV, a significant reduction from 2.67 eV observed with NiCo–ZIF-67. The improvement in electrochemical performance is primarily due to the emergence of Co3+ ions, which results from the efficient charge transfer occurring at the interface of the PBA and NiCo–ZIF core–shell structure. These findings suggest a promising strategy for designing advanced core–shell materials for electrocatalytic applications.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jialin Li,Yu Wang,Ye Zhang,Wei Zhao,Wenzhe Bao,Yufeifan Duan,Junwei Yu,Bo Zhu,Kun Qiao
Currently, the hydrogen storage application of carbon-based adsorbent materials is mostly implemented under the pressure conditions of 30–300 bar, while there is few targeted studies conducted on the unsaturated adsorption under ambient pressure conditions. Therefore, based on industrialized Lyocell biopolymer fiber precursors and the enhancement effects of dipole-induced hydrogen bonds (DIHB), this work presents a facile construction strategy for P/O co-doped Lyocell-based porous carbon fiber cloth (Ly-ACF-F40). By the technical route of thermal stabilization---sonication assisted phosphoric acid activation---hydrogen bonds introduced by interfacial fluorination, the constructed Ly-ACF-F40 acquires a high specific surface area (1870 m 2 /g) and total pore volume (1.277 cm 3 /g), and an excellent hydrogen storage capacity of 3.22 wt% under ambient pressure conditions (77 K, 1 bar). The study directly demonstrated in the experiment that dipole induced hydrogen bonding H(I)-H(II)···F can effectively enhance the atmospheric hydrogen storage density on the basis of other eliminating influencing factors of specific surface area. The simple construction strategy of porous carbon-based materials can provide reference for the research of unsaturated adsorption hydrogen storage materials under ambient pressure conditions, also assist in the application and promotion of low-cost solid hydrogen storage materials.
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LANGMUIR
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2024
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IF 3.7
Mian Gong,Yihui Dong,Minghai Zhu,Fengxiang Qin,Tianchi Wang,Faiz Ullah Shah,Rong An
Surface-enhanced Raman scattering (SERS) is a remarkably powerful analytical technique enabling trace-level detection of biological molecules. The interaction of a probe molecule with the SERS substrate shows important distinctions in the SERS spectra, providing inherent fingerprint information on the probe molecule. Herein, nonhalogenated phosphonium-based ionic liquids (ILs) containing cations with varying chain lengths were used as trace additives to amplify the interaction between the cytochrome c (Cyt c) and Zr–Al–Co–O (ZACO) nanotube arrays, strengthening the SERS signals. An increased enhancement factor (EF) by 2.5–41.2 times compared with the system without ILs was achieved. The improvement of the SERS sensitivity with the introduction of these ILs is strongly dependent on the cation chain length, in which the increasing magnitude of EF is more pronounced in the system with a longer alkyl chain length on the cation. Comparing the interaction forces measured by Cyt c-grafted atomic force microscopy (AFM) probes on ZACO substrates with those predicted by the extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) theory, the van der Waals forces became increasingly dominant as the chain length of the cations increased, associated with stronger Cyt c–ZACO XDLVO interaction forces. The major contributing component, van der Waals force, stems from the longer cation chains of the IL, which act as a bridge to connect Cyt c and the ZACO substrate, promoting the anchoring of the Cyt c molecules onto the substrate, thereby benefiting SERS enhancement.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Yue Wang,Yiting He,Xianglin Ren,Xiaohui Guo,Xiaodong Tian,Chunju Xu,Huiyu Chen
Functionalization and pore engineering are two effective approaches to enhance the electrochemical performance via augmenting the surface area utilization of carbon nanofiber (CNF) mats. Compared with heteroatom-doping, designing the suitable porous structure under a mild and controlled thermal process remains a formidable task. In this work, porous N, O-codoped CNF mats were prepared by using coal tar pitch/polyacrylonitrile (CTP/PAN) precursor and KCl salt template. Notably, the KCl can not only serve as porogen, but also act as a heat scavenger during the heat treatment process to avoid local temperature overheating, which is conducive to the uniform dissipation of organic small molecules, leading to improved ion-accessible area. The sample treated with 0.5 g KCl shows high areal capacitance and excellent rate performance in both 6 M KOH and 2 M ZnSO 4 electrolyte. Furthermore, the assembled Zn-ion capacitor exhibits a high energy density of 505.93 μW h m −2 at the power density of 496.28 μW m −2 , and maintained a maximum power density of 45.94 mW m −2 while retaining an energy density of 313.91 μW h m −2 . The present method is efficient, and cost-effective, and can be extented to the preparation of other electrode materials with superior electrochemical performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jiaqi Li,Yuxi Zhang,Hanhao Liang,Jiaming Li,Xiao Yu,Jianglin Wang,Yini Long,Zhanhong Yang
Manganese oxide is a promising cathode material for rechargeable batteries due to its high theoretical specific capacity. However, its practical application is hindered by its poor conductivity and rapid capacity decay caused by Jahn-Teller distortion during charging and discharging. This work introduces Na 2 EDTA during the synthesis of Mn O 2 , and the amino group is introduced by adsorption to deposit to form N-doped Mn O 2 . Alkaline N-doped Mn O 2 battery upshifts the d-band center of Mn, improves the conductivity of Mn O 2 and the formation energy of O vacancies during the charge-discharge process, and suppresses Jahn Teller distortion. As a result, N-doped Mn O 2 achieves a high capacity of up to 197mAh g −1 and excellent capacity retention of 94.2% over 250 cycles with slower voltage decay. This strategy enables the material with high cycling performance for single-electron discharge secondary alkaline manganese batteries.
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Journal of the American Chemical Society
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2025
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IF 15.6
Mingyan Chuai,Hao Tong,Zimin Yang,Siting Deng,Mingqiang Wu,Jidan Xing,Guoliang Chai
An electrolytic Zn–MnO2 battery is highly valued due to its cost-effectiveness, environmental friendliness, and abundant resource availability. However, the battery’s performance is hindered by the slow kinetics at the poorly conductive MnO2 cathode and hydrogen evolution at the Zn anode. Here, a strategy of P–O–M (M = Mn, Zn) d-pπ backbonding design is proposed for phosphorus–oxygen electrolyte additives, which can be realized by tuning the atomic dipole moment-corrected Hirshfeld (ADCH) population charge of the P/O atom. The reversibility of d-pπ backbonding not only leads to the fast kinetics of Mn2+/Zn2+ at electrodes during both charge and discharge processes to suppress the competitive hydrogen evolution reaction but also enhances the electronic conductivity at the electrode–electrolyte interfaces to sustain the high areal capacity of batteries. Hydroxymethyl dimethyl phosphite (HPD) with d-pπ backbonding is a preferred additive with a suitable ADCH charge. The assembled electrolytic Zn–MnO2 (HPD) battery exhibits a high discharge capacity of 14.05 mAh cm–2 at an areal capacity of 15 mAh cm–2 and superior cycling stability over 1500 cycles. The Zn–MnO2 (HPD) soft-pack battery exhibits a discharge capacity of over 1.60 Ah at a discharge rate of 0.5 C and maintains a Coulombic efficiency of ∼80% over 100 cycles. Furthermore, the assembled 50 V 40 Ah commercial Zn–MnO2 (HPD) battery can drive an electric vehicle for 10 km. The ADCH charge regulation provides a feasible and effective method for developing high-performance aqueous batteries by achieving d-pπ backbonding.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Xi Chen,Xiaoyan Wang,Ziliang Jia,Chao Yang,Zhihong Liu,Yuexing Wei,Mengxue Wang,Meisheng Liang
K-doped Mn–Ce solid solution catalysts were synthesized using a combination of coprecipitation and hydrothermal methods, demonstrating excellent performance in benzene oxidation. The catalyst K 1 Ce 5 Mn 5 exhibited comparable activity to noble metal catalysts, achieving a 90 % benzene conversion at approximately 194 ℃. Durable tests under dry and moist conditions revealed that the catalyst could maintain its activity for 50 h at 218 ℃ and 236 ℃, respectively. Characterization results indicated that the catalyst’s enhanced activity resulted from the weakened Mn–O bonding caused by the introduction of K + , facilitating the activation of oxygen and its involvement in the reaction. CeO x , the main crystalline phase of Mn–Ce solid solutions, provided abundant oxygen vacancies for capturing and activating oxygen molecules for the weakened Mn–O structures. This conclusion was further supported by partial density of state analysis from density functional theory computations, revealing that the introduction of K + weakened the orbital hybridization of Mn3d and O2p. Finally, in situ diffuse reflectance infrared Fourier-transform spectroscopy ( in situ DRIFTS) studies on Ce 5 Mn 5 and K 1 Ce 5 Mn 5 catalysts suggested that the introduction of K + promoted the conversion of adsorbed benzene. Furthermore, intermediate products were transformed more rapidly for K 1 Ce 5 Mn 5 compared to Ce 5 Mn 5 .
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