Coatings
·
2025
·Vol. 15
·期 7
·825
·
IF 2.8
Jiefeng Wang,Shilin Li,Yifan Guo,Jiaqi Ding,Zhi Lu
A novel catalyst with a metal sulfide/hydroxide heterostructure was prepared by introducing sulfur ions into NiMnFe layered hydroxide by a simple hydrothermal method, using a series of characterization methods and electrochemical tests to explore the optimal sulfur ion doping amount. The XPS results show that the introduction of sulfur ions leads to a change in metal electron delocalization, which is conducive to the OER procedure. The newly formed metal sulfide can not only improve the conductivity of NiMnFe LDH/NF electrode materials but also enhance the intrinsic catalytic activity of the materials. The electrochemical performance indicated that the S2-NiMnFe LDH/NF catalyst required only 205 mV overpotential to provide a current density of 10 mA−2, and the Tafel slope was only 45.79 mV dec−1. In addition, the large turnover frequency value (1.2614 S−1) reflects the excellent intrinsic activity of the novel catalytic material.
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OPTICAL MATERIALS
·
2025
·
IF 4.2
Jingyan Yu,Rajendran Kalimuthu,Xingchen Liu,Wengao Zhang,Yonggen Tan,Kun Yan,Shenglin Ye,Jun Feng
Carbon quantum dots (CQDs) hold great potential as fluorescence probes due to their tunable optical properties, but remain challenges in tailoring surface functionalization for selective metal ion detection, which is essential for environmental monitoring and water quality analysis. This work, synthesized nitrogen and sulfur co-doped carbon quantum dots (N, S-CQDs) were via a one-pot solvothermal method with two different solvents, N, N-dimethylformamide (DMF) and acetone. The influences of solvent selectivity on the surface functionality of CQDs and their fluorescence quenching mechanisms were evaluated in both experimental and computational methods. To represent CQDs surfaces, density functional theory (DFT) calculations of the total density of states (TDOS) and partial density of states (PDOS) were conducted. Our findings revealed that synthesized CQDs in DMF and acetone exhibited fluorescence quenching as static and dynamic. We have achieved the highest quantum yields of 37.85 % and 28.59 %. This shows excellent sensitivities of Fe 3+ at 0.82 μM and 1.19 μM for Co 2+ . Furthermore, the study extended to validated in real water sample analysis. This approach enabled the development of a novel strategy for the selective and sensitive detection of Fe 3+ and Co 2+ ions.
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ACS Nano
·
2025
·
IF 16
Chenzhi Ding,Yao Ding,Kao Wang,Zhaobo Zheng,Fang Liu,Xuyun Guo,Mohsen Tamtaji,Zhengtang Luo
Heterojunction engineering, serving as a key framework for building blocks between diverse functional materials, has emerged as a highly promising strategy to address the demand for efficient catalysts in lithium–sulfur (Li–S) batteries. However, achieving full matrix electronic control in the bulk phase is a bottleneck in regulating the electrochemical catalytic behavior of heterostructure catalysts. Herein, we report a “tube-in-tube” multifunctional catalyst that can strengthen the sulfur redox reaction (SRR) in Li–S batteries. Benefiting from a large-scale and oriented two-dimensional (2D) superlattice interface, the tailored heterostructure catalysts (MoSe2/MoS2@CNTs) show a “1 + 1 > 2” synergistic effect in lithium polysulfide (LiPSs) adsorption and catalytic conversion during SRR. In situ studies and theoretical results reveal that this 2D Moiré superlattice interface not only optimizes the adsorption of polysulfides but also moderates the overall electronic density of catalysts. Consequently, Li–S batteries assembled with MoSe2/MoS2@CNTs-PP as a modified separator deliver an outstanding discharge capacity of 1225 mAh g–1 at 0.2 C with a Ketjenblack/S cathode while maintaining a specific capacity of 870 mAh g–1 even at 5 C. Additionally, due to the inhibited “shuttle effect” by heterostructure catalysts, the modified separators exhibit a less capacity fading of 0.063% per cycle after 1000 cycles (1 C) even with a high sulfur loading (3.8 mg cm–2). This work focuses on designing an adsorption–catalysis synergistic interface within a full matrix of catalysts for Li–S chemistry and providing insights into the design of multifunctional catalysts for energy-storage systems based on the catalytic reaction, e.g., Zn–I2 and metal–air batteries, etc.
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ACS Nano
·
2025
·
IF 16
Yuhao Liu,Feng Wu,Zhengqiang Hu,Li Li,Renjie Chen
Lithium–sulfur (Li–S) batteries hold great promise due to their high theoretical energy density yet are plagued by sluggish redox kinetics and the polysulfide shuttle effect. Here, we present a light-activated solid–liquid dual-phase catalytic system that addresses these challenges by integrating soluble cobalt phthalocyanine (CoPc) molecules into the electrolyte and anchoring CoPc/carbon nanotube (CNT) composites onto the cathode. This dual-phase architecture expands the catalytic region from the electrode surface into the bulk electrolyte, establishing a dynamic and spatially extended catalytic microenvironment. Upon light irradiation, photogenerated carriers trigger a cooperative catalytic process, where liquid-phase CoPc selectively adsorbs polysulfides, while solid-phase CoPc/CNT accelerates lithium sulfide (Li2S) nucleation and growth. This synergistic mechanism significantly enhances the electrochemical performance, enabling ultrastable cycling over 2000 cycles at 8C with a capacity decay of only 0.019% per cycle. Furthermore, excellent performance is maintained under practical conditions with high sulfur loading of 10.53 mg cm–2 and low electrolyte/sulfur ratio of 4 μL mg–1. This study demonstrates a scalable strategy for constructing spatiotemporally regulated catalytic domains, providing insights into the design of advanced photoassisted energy storage systems.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Mengyang Cui,Shisheng Yuan,Bo Jin,Qing Jiang
Sodium-sulfur (Na-S) batteries are believed as the hopeful energy storage and conversion techniques owing to the high specific capacity and low cost. Nevertheless, unstable sodium (Na) deposition/stripping of Na metal anode, low intrinsic conductivity of sulfur cathode, and severe shuttling effect of sodium polysulfides (NaPSs) pose significant challenges in the actual reversible capacity and cycle life of Na-S batteries. Herein, a self-supporting electrode made of nitrogen-doped carbon fiber embedded with cobalt nanoparticles (Co/NC-CF) is designed to load sulfur. Meanwhile, gel polymer electrolyte (GPE) with high ion transfer ability is obtained by in-situ polymerization inside the battery. During the polymerization process, an integrated electrode-electrolyte and a continuous ion-electron conduction network in a composite cathode are constructed inside the Na-S battery. It is noteworthy that the designed GPE demonstrates superior ionic conductivity and effective adsorption of NaPSs that can significantly suppress the shuttle effect. Leveraging the synergistic interplay between the designed GPE and self-supporting cathode, the assembled quasi-solid-state (QSS) Na-S battery exhibits great cycling stability. These experimental results are further corroborated by COMSOL Multiphysics simulations and density functional theory (DFT) calculations, which mechanistically validate the enhanced electrochemical performance. The findings of this study offer new and promising perspectives for advancing the development of next-generation solid-state batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Fanshuai Gao,Lijia Liu,Huayu Liu,Yudan Wang,Yawen Liu
In aquatic environments, CH 3 Hg + represents a persistent neurotoxin that proves challenging to eliminate. Despite the extensive efforts made by countries in mercury pollution control, it still poses a significant threat to ecological health in some underdeveloped countries and regions. This study introduces a novel amorphous coordination polymer (BD-ACP-A), synthesized through a coordination reaction involving bis(4-hydroxyphenyl) disulfide, adenine, and Cr(NO 3 ) 3 ·9H 2 O. The resulting material exhibited exceptional adsorption performance for CH 3 Hg + across a wide pH range of 2 to 11. At an initial concentration of 300 ppb, adsorption equilibrium was reached within 30 min, with an adsorption capacity exceeding 1460 μg·g −1 and a removal rate surpassing 98.0 %. BD-ACP-A also demonstrated remarkable anti-interference capabilities, maintaining high adsorption efficiency in the presence of elevated concentrations of humic acid or NaCl, as well as in various real water samples. Furthermore, it exhibited excellent reusability; at an initial concentration of 160 ppb, it retained an adsorption capacity of 718 μg·g −1 and a removal rate exceeding 89.8 % after 10 adsorption-desorption cycles. The adsorption process was well described by the Langmuir isotherm and pseudo-second-order kinetic models, yielding a maximum adsorption capacity of 138 mg·g −1 . Mechanistic investigations utilizing FT-IR, XPS analysis and DFT calculations revealed that the adsorption is primarily driven by the synergistic chelation of sulfur atoms and covalent interactions with nitrogen atoms. This work not only provides a highly efficient adsorbent for CH 3 Hg + pollution control but also presents a novel strategy for designing amorphous polymers with broad pH adaptability and rapid adsorption kinetics.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 13
·期 6
·120398
·
IF 7.2
Rui Li,Yangyang Lei,Meilin Yin,Lipeng Wang,Shaokun Tang
Combining ionic liquids (ILs) with metal–organic frameworks (MOFs) functionalizes the MOF pores and provides numerous active sites including Lewis acidic sites and hydrogen bond donors in the resulting heterogeneous composites, making them promising materials for CO 2 capture and conversion. Despite this potential, the prevalent microporosity in most MOFs severely restricts mass transfer. To address this limitation, it is essential to introduce hierarchical porosity into MOFs since it can enhance CO 2 capture and conversion by facilitating mass transfer and molecular diffusion. In this work, a hierarchical porous gel of UiO-66-NH 2 (denoted as HP-UiO-66-NH 2 ) was prepared through a simple sol-gel process, exhibiting micropores within the particles, mesopores between the particles, as well as multiple catalytic sites. Subsequently, poly(ionic liquid)s (PILs) were introduced into the porous framework to successfully construct PILs-MOFs gel materials (HP-MOF@PILs). A comprehensive evaluation was conducted on the synthesized materials regarding their ability to adsorb CO 2 , their catalytic performance in CO 2 cycloaddition with epichlorohydrin, and their recyclability. Benefiting from the synergistic advantages of its hierarchically porous structure and the strong CO 2 and epoxide activation ability of nucleophilic Br ions in PILs, HP-MOF@PIL-2 demonstrated exceptional catalytic performance and achieved high efficiency for the cycloaddition of CO 2 with epichlorohydrin under mild conditions (80 °C, 0.1 MPa, 24 h) without requiring co-catalysts or solvents, showcasing its role as a potential and eco-friendly catalyst in CO 2 conversion processes.
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DESALINATION
·
2025
·
IF 9.8
Xiaoying Lin,Bingqing Huang,Yifan Liu,Yuancai Lv,Chunxiang Lin,Jianhui Huang,Minghua Liu,Xiaoxia Ye,Jie Chen
The development of adsorbents capable of simultaneously achieving high uranium(VI) adsorption capacity, rapid kinetics, and exceptional selectivity remains a critical challenge for sustainable uranium(VI) extraction from seawater, essential for nuclear energy sustainability. Herein, we report the synthesis of a novel ellagic acid immobilized conjugated micro-mesoporous poly(aniline)s (CMP-E) via a Buchwald-Hartwig coupling strategy incorporating ellagic acid prefunctionalization. This synergistic combination of molecular confinement and pore engineering maximizes the density of accessible adsorption sites, overcoming the long-standing trade-off between adsorption site uniformity and surface coverage in conventional adsorbents. The resulting CMP-E showed exceptional uranium(VI) extraction performance, achieving a record adsorption capacity of 515 ± 14 mg g −1 , and the initial adsorption kinetics ( h ) reached 6.5 ± 0.3 mg g −1 min −1 , both exceeding pristine CMP by over 1.5 times. Notably, CMP-E demonstrated outstanding selectivity for uranium(VI), with a selectivity coefficient over 6.8 for uranium(VI)/other ions in the presence of various co-existing ions. This enhanced performance was attributed to the stable negative surface charge of CMP-E across a wide pH range, which promoted efficient electrostatic enrichment of uranium(VI) species. The subsequent coordination of uranium(VI) with lone pair electrons from nitrogen atoms (-NH- and = N-) in the poly(aniline) skeleton and oxygen atoms (-OH and C O) in the ellagic acid moiety further enhanced the uranium(VI) capture. Dynamic adsorption tests in real seawater demonstrated promising performance, achieving >86.3 ± 0.9 % uranium(VI) recovery with negligible capacity loss. Furthermore, a 7-day marine field test conducted in Pingtan revealed an adsorption capacity of 2.32 ± 0.02 mg g −1 under real marine conditions. These results suggested that CMP-E held significant potential as a material for the efficient extraction and recovery of uranium(VI) from seawater.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Yusong Zhang,Wei Shi,Huanlin Li,Lei Yang,Lei Hou,Cheng Ma
Enantiomers often exhibit significant differences or even diametrically opposed effects in pharmacological activity, toxicological properties, and metabolic behavior. Single-enantiomer drugs frequently demonstrate distinct advantages over the racemate. Therefore, accurately distinguishing between enantiomers and racemate is particularly crucial in the fields of chemistry and biomedicine. Racemates, as mixtures of equal amounts of the enantiomers (levorotating and dextrorotating), exist in two forms: racemic mixtures and racemic compounds. Racemic compounds exhibit differences from their enantiomers in absorption spectra, whereas racemic mixtures do not. This study investigates the absorption spectra of ( S )-(+)-2-phenylpropionic acid, ( R )-(-)-2-phenylpropionic acid, and their racemates using terahertz time-domain spectroscopy technology. Experimental results indicate that the enantiomer exhibits absorption peaks similar to those of the racemic mixture, but with a significant difference in absorption intensity. Further combined with density functional theory (DFT), theoretical spectral calculations were performed on the solid state and solution enantiomers based on single molecule and unit cell models respectively. It was found that the enantiomeric simulation spectra were highly consistent. After the sample transitioned from solid to solution state, changes in hydrogen bonds would change its molecular vibration characteristics and intermolecular interaction patterns.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Yu Wen,Yue Liu,Yanghua Teng,Qiwen Yong,Dongmei Pu,Xiaoqiang Fan,Zhi-Hui Xie
A novel and long-lasting N 3 BD/TiO 2 composite photoanode with stable and superior photoelectrochemical and photoelectrochemical cathodic protection (PECCP) performances was achieved by synthesizing and depositing covalent organic framework (N 3 BD) on titanium oxide (TiO 2 ) nanotube arrays. The composite's increased visible light absorption capability enhanced the galvanic corrosion protection of nickel-phosphorus alloy-coated magnesium alloy (Mg/Ni) through PECCP technology. The open circuit potential (OCP) drops of the Mg/Ni electrode coupling with the N 3 BD/TiO 2 composite were 310 and 630 mV at dark state and under illumination, respectively. They remained relatively stable under intermittent visible light irradiation within 72 h, demonstrating excellent long-term stability. The superior photoelectrochemical and PECCP properties of the N 3 BD/TiO 2 are attributed to forming S-scheme heterojunctions, which effectively promote the separation and transfer of photogenerated electron-hole pairs and retain a strong redox capacity. This finding provides new insight into the design and synthesis of COF-modified photoanode with highly efficient and stable photoelectrochemical and PECCP performances.
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MOLECULES
·
2025
·Vol. 30
·期 8
·1804
·
IF 4.6
Wentao Xiang,Zhenzhen Yu,Renwu Gao,Zhichao Yi,Kun Gong,Kangqiang Lu,Weiya Huang,Changlin Yu,Zeshu Zhang,Man Zhou,Kai Yang
Rapid charge separation and transfer is the key scientific problem in photocatalysis. The construction of S-scheme heterojunction is one of the effective strategies to promote charge separation and maintain the strong redox properties. Herein, the NiO, K0.2WO3, and NiWO4ternary double S-scheme K0.2WO3/NiO/NiWO4heterojunction (W/NiO) was created by a one-step molten salt method. Ultraviolet-visible (UV-Vis) diffuse reflectance spectra, photoluminescence (PL) spectra, photoelectrochemistry tests, and other analyses revealed that the double S-scheme heterostructure broadened the spectral response range of NiO and promoted its separation of photocarriers. Compared with pristine NiO, the modified double S-scheme heterojunction enhanced the surface adsorption of water molecules and the accumulation of intermediate product of HCOO−, and optimized the CO2reduction system, realizing the improved CO yield of 373 μmol·g−1·h−1in Ru(byp)32+/ethanolamine of CO2reduction system. This study indicates that double S-scheme heterojunction could facilitate efficient photogenerated charge transfer and separation, thereby achieving high activity and selectivity for CO2photoreduction. Our work provides a reference for the one-step construction of double S-scheme heterojunction.
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高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Ya Zeng,Lingfeng Qin,Sijie Tian,Caicheng Long,Taiping Qing,Peng Zhang,Bo Feng
Cobalt-based multiphase catalysts can effectively activate peroxymonosulfate (PMS) and degrade organic pollutants. However, their practical application faces critical challenges, including insufficient exposure of active sites, slow reaction kinetics, and cobalt ion leaching, which collectively reduce catalytic efficiency and sustainability. Although there have been attempts to improve the catalytic efficiency through structural modifications such as core-shell structure or porous design, these strategies are still difficult to optimize the active site exposure and cobalt ion stability simultaneously. To overcome these limitations, here we propose a novel triple-shell yolk@shell architecture (3YS-Co@NC) constructed via a stepwise strategy involving crystal extension growth, selective etching, and calcination. The optimized nanoreactor degraded 100 % of bisphenol S (BPS) within 12 min with a rate constant (0.342 min −1 ) 9.5-, 2.34-, and 1.49-fold higher than solid nanoparticles (Co@NC), single-shell (1YS-Co@NC), and double-shell (2YS-Co@NC) counterparts, respectively. Notably, the TOC removal rate of 3YS-Co@NC reached 71 %, surpassing those of 1YS-Co@NC (53 %), 2YS-Co@NC (65 %), and Co@NC (21 %). The enhanced performance results from (i) the yolk@shell structure providing nanoreaction cavities and abundant active sites, and (ii) the robust Co 0 /Co 2+ /Co 3+ redox cycling. Quenching experiments and EPR analysis revealed that SO 4 •- and •OH dominated PMS activation, while O 2 •- played an auxiliary role. In contrast, 1 O 2 exhibited negligible contribution. LC/MS analysis identified key degradation intermediates, and the ECOSAR model predicted reduced biotoxicity of these products. This study not only promotes the development of advanced oxidation processes, but also provides a new insight into the design of cobalt-based catalysts.
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