APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Fu Li,Jingnan Yang,Xiaomei Zhou,Fei Han,Qian Huo,Qingxin Guan,Wei Li
Converting CO 2 to ethanol through photothermal catalysis faces significant challenges due to it involves multi-electron reduction and kinetically sluggish C-C coupling process. Here, copper and a minor quantity of palladium are encapsulated within the cage of UiO-66 using a dual-solvent-sonication method to form ultrafine Cu 2 O/Cu-Pd clusters. The Cu-Cu 2 O serves as an electron center to enhance CO 2 uptake and activation, while the incorporation of Pd accelerates H 2 activation. Due to differences in electronegativity , electrons tend to transfer from Cu to Pd, which reduces the electrostatic repulsion between intermediates and facilitates the coupling of *CO and *CHO. The photothermal ethanol yield of Cu 6 Pd@UiO-66 reached 1077.69 μmol·g cat –1 ·mL –1 with a selectivity of 94.62%, representing an 11.64-fold increase over the non-illumination, and a 3.11-fold enhancement compared with Cu 6 @UiO-66. This study offers evidence supporting the promotion of C-C coupling through an asymmetric electron distribution , potentially advancing the conversion of CO 2 to liquid products.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
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IF 11.3
Zhenmin Xu,Ting Zhang,Junyu Lang,Mengli Xu,Ya Xie,Chunyan Wu,Huangrong Wang,Han Yu,Zhenfeng Bian
Carboxylates are commonly formed as intermediates during the oxidation of volatile organic compounds (VOCs) and are often regarded as significant barriers to the complete mineralization of organic pollutants. In this study, we present a novel cobalt-doped copper-based catalyst that employs an in situ benzoic acid-mediated oxygen activation strategy for the photocatalytic degradation of toluene under visible-light irradiation. Unlike traditional systems in which carbonyl intermediates contribute to catalyst deactivation, we demonstrate that benzoic acid, generated during toluene oxidation, acts as a potent ligand to modulate the electronic structure of cobalt sites. This interaction significantly enhances oxygen activation and promotes the generation of reactive oxygen species (ROS), facilitating the complete oxidation of toluene to CO2 with nearly 100% efficiency. In situ characterization and density functional theory (DFT) calculations reveal that the migration of benzoic acid from copper to cobalt sites under visible light is critical for the oxidation process. This migration induces a pronounced electron-donating effect, enabling activation of the Co center, which drives efficient ROS production and autocatalytic mineralization of benzoic acid. The resulting Co-Vo-Cu catalyst demonstrates exceptional catalytic activity and stability, outperforming previous systems in VOCs degradation. This work offers new insights into the role of organic intermediates in oxygen activation and presents a promising strategy for the development of next-generation photocatalysts for VOCs elimination.
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RARE METALS
·
2025
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IF 11
Dong Qi,Li Wen-Bin,Zhang Jian-Hua,Yang Hao-Fei,Wu Yu-Mei,Pei Jing-Jie,Huang Xing,Wang Jing-Jing,Li Xi-Fei
Layered V 2 O 5 ·H 2 O (vanadium pentoxide hydrate) is a highly promising cathode material for aqueous zinc-ion batteries owing to its large interlayer space, variable V valence states, and unique interlayer H 2 O. However, the low electronic conductivity and easily exfoliated lattice layers lead to its poor charge transport kinetics and lattice stability. In this regard, we develop a ternary transition metal ions pre-intercalation strategy, where ternary Ni/Mn/Cu cations are successfully pre-intercalated into V 2 O 5 ·H 2 O by one-step hydrothermal method. It is revealed that Mn cation activates the additional Mn 4+ /Mn 3+ redox reaction, and ternary Ni/Mn/Cu cations cause the strong ion column effect, induce the highest p-band center of O, and improve the electrical conductivity, thus simultaneously enhancing the lattice stability and charge transport kinetics. As a result, the energy density of 391 Wh kg −1 at 0.1 A g −1 and the high-rate capability with a capacity of 240 mAh g −1 at 3 A g −1 after 600 cycles are achieved. Besides, the electrochemical reaction mechanism is revealed to be H + intercalation at high potentials, and followed Zn 2+ intercalation at low potentials, and Zn 2+ intercalation contributes most of the capacity (> 65%) and H + intercalation promotes the optimization of electrochemical performance. Graphical abstract
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DESALINATION
·
2025
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IF 9.8
Xueyang Fan,Yuanyuan Guo,Lieyu Zhang,Qingliang Wang,Chen Zhao,Qi Xin,Zhiwu Lei,Eming Hu,Hongqiang Wang
The removal and recovery of uranium from radioactive wastewater are crucial for environmental protection. A photoelectric cooperative catalysis method using Cu-SA/g-C 3 N 4 electrodes has been proposed for the efficient removal and recovery of uranium. The uranium removal efficiency achieves 98.8 % within just 5 min for a 10 mg/L uranium solution at pH 6. The removal rate under photoelectric cooperative catalysis is 22 times higher than that under photocatalytic alone and 12 times higher than that under electrocatalysis alone. Compared to the Cu-based single-atom catalyst electrode, the electrocatalytic uranium removal process achieves a significant reduction in time, decreasing from 180 min to 5 min, which is considerably higher than that reported in the prior literature. The results of PXRD and Raman analysis indicate that the adsorbed uranyl species are initially reduced to unstable U(V) intermediates, which are subsequently oxidized to form Na 2 O(UO 3 ·H 2 O) x deposits. The synergistic advantages of photocatalysis and metal single-atom catalysts are fully utilized to achieve rapid uranium deposition and removal without occupying the electrode's adsorption sites. The cyclic experiment demonstrates an exceptionally high uranium adsorption capacity of 8954 mg/g, with no signs of saturation. The uranium removal rate by the Cu-SA/g-C 3 N 4 electrode from real wastewater is 100 % within 30 min. In summary, the photoelectric cooperative catalytic system enables highly efficient uranium removal, thereby establishing a robust foundation for the removal and recovery of uranium from wastewater.
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Advanced Science
·
2025
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IF 14.1
Jingting Jin,Wenzhi Li,Liqun Wang,Lulu Zhang,Xia Zhang
Direct and efficient methane oxidation to methanol is an appealing route for upgrading abundant methane resources while acquiring building blocks of clean fuels and chemicals. However, owing to its highly symmetrical nature imparted chemical stability and steric hindrance, the design of multi-ångstrom (<3.0 Å) spaced active species capable of activating its first C−H bond remains a fundamental challenge. Herein, Cu−Ni dual-atom Pair is constructed using defect engineering and a stepwise deposition method over indium oxide to precisely modulate the C−H polarization with the Cu atom showing affinity to H end and Ni anchoring the C side. The optimal CuNi/InNT achieves an oxygenates (CH 3 OH and CH 3 OOH) productivity of 106 mmol g cat h −1 , surpassing reported systems. Theoretical calculations validate the dominating role of interatomic distance for methane activation. Specifically, the dual-atom orbital coupling effect in the minimally spaced Cu−Ni pair up-shifts the overall d-band center, significantly enhancing its hybridization with C/O 2p. Further modification through macroscopic reactor design boosts CH 3 OH yield to 36818.84 µmol g cat h −1 with 79.37% selectivity in a 1000 mL semi-industrial prototype. This work provides a comprehensive explanation of the Cu−Ni synergy, bridging atomic-scale catalysis with reactor design, and establishes a common design principle for binary catalysts at the electron and orbital level.
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CHEMICAL ENGINEERING SCIENCE
·
2025
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IF 4.3
Zhaohua Jiang,Shiyuan Fan,Huiting Xu,Huibin Liu,Sai Dong,Jing Li,Xiaoteng Yan,Zhijie Cui,Wenchao Peng,Wen Liu,Jiapeng Liu
Aqueous copper-selenium (Cu-Se) battery based on conversion mechanism have garnered interest due to their intrinsic safety features and high specific capacity. However, the slow conversion kinetics presents a challenge for its development. Herein, catalytic host material of NbSe 2 @few-layered Nb 2 C (NbSe 2 @f-Nb 2 C) heterostructure with built-in electric field (BIEF) is prepared by in situ selenization strategy for aqueous Cu-Se battery. Benefiting from the high electrical conductivity of f-Nb 2 C MXene, the high electrocatalytic performance of NbSe 2 and the spontaneous BIEF between NbSe 2 and f-Nb 2 C MXene, the Se redox reactions kinetics is enhanced and the reaction barrier is reduced. Consequently, the specific capacity of Se/NbSe 2 @f-Nb 2 C cathode can reach 1128 mAh g −1 at 0.25 A g −1 with stable cycling performance. Additionally, the conversion mechanism is investigated via comprehensive characterizations and density functional theory calculations. This study provides an innovative approach for designing high performance MXene-based catalytic host materials to enhance the conversion kinetics of aqueous Cu-Se batteries.
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TALANTA
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2025
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IF 6.1
Qian Wang,Maoyuan Hu,Xiangwei Yuan,Xiaoli Xiong,Zhaoyu Jin
Hydroquinone (HQ), catechol (CC), and resorcinol (RS), as toxic and hardly degradable dihydroxybenzene isomers, pose threats to the environment and human health. In this study, using multi - walled carbon nanotubes (MWCNTs) and ZIF-8 as precursors, a necklace-like N-doped carbon polyhedron/carbon nanotube composite loaded with Cu nanoparticle (Cu NPs/NC@MWCNTs) electrocatalyst was prepared by hydrothermal and high-temperature carbonization processes. Comprehensive characterization data from XRD, SEM, TEM, XPS, BET, and Raman spectroscopy confirmed that the unique necklace-like porous structure and synergistic effect between ZIF-derived N-doped carbon polyhedra and MWCNTs regulate the electronic structure and surface properties of the catalyst, thereby accelerating the electron transfer rate. Under neutral conditions, the Cu NPs/NC@MWCNTs/CP electrode exhibits good electrocatalytic activity for the separate or simultaneous determination of three dihydroxybenzene isomers (HQ, CC, and RS) with low detection limit of 0.16 μM, 0.14 μM and 0.10 μM (S/N = 3), respectively. Density functional theory (DFT) calculations further reveal the differences in selectivity and sensitivity among the three isomers. In addition, this sensor has been successfully applied to the detection of three dihydroxybenzene isomers in actual environmental water samples, achieving satisfactory recovery rates of 97.8–106 %.
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ACS Applied Nano Materials
·
2025
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IF 5.5
Xinran Li,Yuwei Zhong,Habib Ullah,Jian Luo,Lee Li,Ghafar Ali,Alaa G. M. Osman,Xiujian Zhao,Yi Xie
The intrinsic structural lability and limited processability of inorganic halide perovskites heavily hamper their commercial applications. Herein, we develop a facile and scalable room-temperature (RT) water-based procedure for the synthesis of Na–Cu-codoped CsPbIxBr3–x-embedded Pb(OH)I (denoted as the Na–Cu–CsPbIxBr3–x@Pb(OH)I) composite to overcome the above-mentioned bottlenecks. Compared to Na doping, the codoping with Na and Cu leads to a slight shift of the photoluminescence (PL) peak position from ∼612 to 622 nm, increases the PL intensity by 32.5 times, and improves the PL quantum yield from 1% to 5%. Notably, the optimized Na–Cu–CsPbIxBr3–x@Pb(OH)I composite displays outstanding stability under various harsh environments such as soaking in RT water or hot water (up to 90 °C) and annealing at high temperature, which indicates that Pb(OH)I can act as an effective water-blocking and protective encapsulation layer. It is more interesting that the photoluminescence (PL) intensity of Na–Cu–CsPbIxBr3–x@Pb(OH)I can be significantly increased to 2.17 and 1.29 times after soaking the sample in RT water for 35 and 105 days, respectively, and 1.25 times even after immersing in hot water (90 °C) for 6 h, indicating an improved optical property. Meanwhile, the crystal structure and emission wavelength are maintained. The insight of this work is quite beneficial for designing highly stable inorganic perovskite-based nanomaterials for realization in light-emitting devices and other optoelectronic devices.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Mingyu Chang,Jingcheng Lv,Lianhui Sun,Aihong Chen,Fengbo Zhang,Guangjian Fan,Zhanliang Liu,Jun Li,Hongliang Shen,Mingjun Shi,Yinong Niu,Ye Tian,Xijian Liu,Boyu Yang
Benign prostatic hyperplasia (BPH) presents a significant clinical challenge, with conventional therapies carrying substantial risks, including urinary retention, sexual dysfunction, and prolonged recovery. To address the urgent need for safer, ultra-minimally invasive alternatives, we developed a sonosensitizing nanoplatform using copper–manganese-doped mesoporous silica nanoparticles (Cu–Mn@SiO2) for ultrasound-induced sonodynamic therapy (SDT). Here, we demonstrate that this innovative strategy provides highly effective and precisely targeted therapy for BPH. In vitro studies revealed that Cu–Mn@SiO2-mediated SDT significantly amplified intracellular reactive oxygen species (ROS) generation, triggering oxeiptosis characterized by PGAM5 cleavage, mitochondrial membrane depolarization, and mitochondrial damage in both BPH-1 epithelial and WPMY-1 stromal cells. In a testosterone-induced BPH rat model, a Cu–Mn@SiO2-combined, localized SDT treatment resulted in a substantial 60% reduction in prostatic weight and a marked improvement in urinary function. Thermal imaging confirmed prostate-specific hyperthermia without affecting the surrounding tissues. Histopathology revealed reduced collagen deposition and restored glandular morphology with comprehensive biosafety assessments showing no systemic toxicity. By precisely inducing localized oxeiptosis within hyperplastic prostatic tissue via focused ultrasound activation, this Cu–Mn@SiO2-based nanoplatform represents a clinically translatable, ultra-minimally invasive therapeutic strategy offering a superior safety profile for BPH management.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Xiaoqing Li,Min Zuo,Ziwei Lan,Fengling Jiang,Dickon H. L. Ng,Jia Li
C/OVs-Ni-Cu-LDHs@MnO2 tubular micromotors with enzyme-like activity and abundant oxygen vacancies (OVs) were synthesized hydrothermally using kapok as a biotemplate. MnO2 acted as the micromotor’s “driving engine”, catalyzing the generation of H2O2 bubbles to provide driving force for the motor, enabling efficient motion (144.45 ± 3.97 μm/s in 5% H2O2). The micromotors also exhibited enzyme-like activity, oxidizing 3,3′,5,5′-tetramethylbenzidine (TMB) via reactive radicals. A sensor for the colorimetric detection of GLY (lowest detection limit 0.63 μM) was developed by utilizing the enzyme inhibition induced by Cu2+-glyphosate (N-(phosphonomethyl)glycine, GLY) chelation. Meanwhile, the micromotor catalyzes H2O2 and activates peroxymonosulfate (PMS), efficiently generating hydroxyl radicals (•OH), superoxide radicals (O2•–), and single-linear oxygen (1O2). Under the synergistic effect of self-driven propulsion and efficient catalysis, achieving 93.71% GLY degradation in 40 min. This study provides an intelligent strategy for developing dynamic sensors with dual functions of simultaneous detection and degradation of GLY.
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Surfaces and Interfaces
·
2025
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IF 6.3
Hui Wang,Xuefei Wang,Ju Liu,Junru Li,Hongle An,Xiaodong Wang,Bingchun Xue
In this study, two Cu-doped covalent organic frameworks (Cu@COFs, namely Cu@TpBD and Cu@TpMDA) were successfully synthesized via the solvothermal method to address the challenge of bisphenol A (BPA) removal in aqueous systems. The adsorption behaviors of both Cu@COFs conformed to the pseudo-second-order kinetic model and the Langmuir isotherm model, indicating the monolayer chemisorption as the dominant mechanism. Notably, Cu@TpMDA exhibited a higher adsorption rate and a larger adsorption capacity for BPA compared to Cu@TpBD. This superior performance could be ascribed to the formation of Cu-O coordination bonds, which optimized the pore structure and enhanced the flexible features of Cu@TpMDA. The combination of characterization analyses, adsorption experiments, and density functional theory calculations revealed that the adsorption process was governed by a multi-synergistic adsorption mechanism, involving pore filling, hydrogen bond, π-π stacking, and metal coordination interaction. Remarkably, after five consecutive adsorption-desorption cycles, the BPA removal efficiencies remained over 97 % for Cu@TpMDA and 92 % for Cu@TpBD, confirming their excellent stability and reusability. The constructed coordination-driven flexible Cu@COFs system not only elucidates the structure-property-mechanism relationship, but also provides a theoretical framework for the targeted treatment of organic pollutants in complex aquatic environments.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Liang Tang,Shiwan Zhang,Zhenheng Long,Bo Lei,Peng Zhang,Ying Liu,Haoyu Sun,Minghong Wu
Veterinary antibiotics and herbicides could be simultaneously ingested by livestock (especially cattle) due to their co-occurrence in feed, disrupting redox homeostasis. However, limited information is available on the combined molecular-level effects of these agrochemicals on antioxidant enzymes. In this study, sulfadiazine (SD) and metamitron (MET) were respectively selected as the representatives of veterinary antibiotics and herbicides to explore their combined toxic effects on SOD and the underlying molecular mechanisms, using multi-spectroscopic technologies, X-ray photoelectron spectroscopy (XPS), and molecular docking. Binding and conformation characterizations revealed that, at specific compound-to-enzyme ratios, SOD inactivation predominantly originated from direct binding of test chemicals at key sites rather than compound-induced conformational changes. Furthermore, fluorescence quenching analysis demonstrated 1:1 binding stoichiometry, indicating the only one preferential binding site for SD and MET in SOD. An integrated ‘interaction-microenvironment-conformation’ evaluation framework was established to judge the joint toxic effects between SD and MET, suggesting that these chemicals competitively interacted with the same binding site to antagonistically inhibit SOD activity. Considering the proximal amino acid residues (such as glutamate, arginine, and tyrosine residues) confirmed by activity test, synchronous fluorescence, and XPS, a key binding pocket in the SOD inter-subunit cavity was identified as the interaction site for both SD and MET. Computational simulations further validated and visualized the binding characteristics of test chemicals within this key SOD dimer interface. This study elucidates the interaction characteristics between SOD and typical agrochemicals, providing a new insight and methodology for assessing the molecular-level health risks of mixed agrochemicals.
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