CHEMOSPHERE
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2016
·
IF 3.698
Ying Han,Zhong-lin Chen,Ji-min Shen,Ji-he Wang,Wei-wei Li,Jun Li,Bin-yuan Wang,Li-na Tong
The role of Cu(II) in the reduction of N -nitrosodimethylamine (NDMA) with zero-valent metals was investigated by determining the effects of Cu(II) on the removal, kinetics, products, and mechanism. NDMA removal was enhanced, and all reactions followed a pseudo-first-order kinetic model except for the Fe and Fe/0.1 mM Cu(II) systems. The iron mass-normalized pseudo-first-order rate constants ( k MFe ) increased with the Cu(II) concentration. The zinc mass-normalized pseudo-first-order rate constants ( k MZn ) were identical to those with the Cu(II) concentrations from 0.1 mM to 1.0 mM and were higher with 2.0 mM Cu(II). The types of products detected were unchanged. Some unknown products were also found. NDMA was reduced to 1,1-dimethylhydrazine (unsymmetrical dimethylhydrazine , UDMH). Then, UDMH was reduced into dimethylamine (DMA) by the Fe/Cu(II) and Zn/Cu(II) systems. Catalytic hydrogenation was proposed as the reduction mechanism. Several copper species, such as Cu(OH) 2 in the Fe/Cu(II) system and Cu 2 O and Cu(OH) 2 in the Zn/Cu(II) system enhanced NDMA reduction. Differences between the Fe/Cu(II) and Zn/Cu(II) systems were caused by the reduction potentials and surface conditions of the different metals and the copper species in the various systems.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiangqian Guo,Chenhui Qiu,Zhiqiang Zhang,Jie Zhang,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction plays an important role in solving environmental issues and alleviating the energy crisis. However, it is still challenging to distribute the surface-active site on photocatalysts with efficient separation of carriers in rational. Herein, the Cu species loaded SrTiO 3 nanofiber was constructed through coaxial electrospinning which could realize the dispersion of the Cu site on the one-dimensional (1D) nanofiber structure. The 1D nanofiber with Cu site exhibited superior performance on photocatalytic CO 2 reduction based on the excellent ability of charge separation. The Cu 2 O and CuO were determined to be located on the surface of 1D SrTiO 3 nanofiber by the TEM and XPS. The work functions of SrTiO 3 , Cu 2 O, and CuO were calculated to be 5.26, 5.47, and 5.51 eV, respectively, suggesting that the carriers could transfer from SrTiO 3 nanofiber to the Cu species. The yield of CH 3 OH with the optimized 8%Cu-SrTiO 3 catalyst could reach 8.08 ± 0.03 µmol⋅g −1 ⋅h −1 . This work provided a coaxial electrospinning strategy to load the Cu species active site on the surface of 1D SrTiO 3 nanofiber for enhancing photoreduction CO 2 .
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Xi Quan,Jun Zhang,Linlin Yin,Yu Tian
In this study, the activation of peroxymonosulfate (PMS) and selective degradation of nonsteroidal anti-inflammatory drugs were investigated using hydrophobically modified Fe 3+ @Cu-MOF. The Fe 3+ @Cu-MOF-CTAB/PMS system demonstrated high-efficiency, achieving near-complete degradation of diclofenac within 120 min. The degradation rate constants for diclofenac, ibuprofen, and naproxen were 0.0048, 0.00103, and 0.00046 min −1 , respectively, positively correlated with their hydrophobicity. Longer hydrophobic surfactant chains in Fe 3+ @Cu-MOFs lead to greater initial adsorption of diclofenac, enhancing degradation efficiency upon the introduction of PMS. The Fe 3+ @Cu-MOF-CTAB/PMS system removes over 80 % of diclofenac in various water matrices, showing optimal efficiency in acidic environments but reduced effectiveness with competing anions. Post-degradation changes in the oxidation states of copper and iron in the MOF structure indicated a synergistic redox mechanism essential for PMS activation. The hydroxylation and C-N bond cleavage in diclofenac were key degradation pathways. This study highlights the potential of hydrophobically modified Fe 3+ @Cu-MOFs in water treatment, providing insights into the interplay between material design, hydrophobic interactions, and catalytic performance.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Min Zhang,Jin Wang,Xinyuan Zhan,Wusong Xu,Maolin He,Ding Ma,Zhengbo Yue
Thiocyanate (SCN − ), a non-volatile inorganic pollutant, is commonly found in various types of industrial wastewater, which is resistant to hydrolysis and has the potential to be toxic to organisms. Premagnetized iron-copper-carbon ternary micro-electrolytic filler (pre-Fe/Cu/C) was prepared to degrade SCN − . Pre-Fe/Cu/C exhibited the most significant enhancement effect on SCN − removal when magnetized for 5 min with an intensity of 100 mT, and the SCN − removal rate was the highest at an initial pH of 3.0 and an aeration rate of 1.6 L/min. The electrochemical corrosion and electron transfer in the pre-Fe/Cu/C system were confirmed through SEM, XPS , FTIR , XRD , and electrochemical tests. This resulted in the formation of more corrosion products and multiple cycles of Fe 2+ /Fe 3+ and Cu 0 /Cu + /Cu 2+ . Additionally, density functional theory (DFT) calculations and electron paramagnetic resonance (EPR) were utilized to illustrate the oxygen adsorption properties of the materials and the participation of reactive oxygen species ( 1 O 2 , ·O 2 − , and ·OH) in SCN − removal. The degradation products of SCN − were identified as SO 4 2− , HCO 3 − , NH 4 + , and N 2 . This study introduced the use of permanent magnets for the first time to enhance Fe/Cu/C ternary micro-electrolytic fillers, offering a cost-effective, versatile, and stable approach that effectively effectively enhanced the degradation of SCN − .
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TALANTA
·
2024
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IF 5.6
Xian Yang,Yujie Xiao,Yue Zhao,Hongping Han,Hong Zheng,Xue Zhang
In this study, Cu doped carbon dots (Cu-CDs) of uniform particle size and good water solubility was synthesized using Angelica Sinensis Radix as precursor materials through a one-step hydrothermal. The Lucigenin-(Cu-CDs) chemiluminescence sensor allows the simultaneous determination of o -toluenesulfonamide (TFA) and sulfamethoxazole (STZ) concentrations. Under optimal conditions, the sensor demonstrates the capability to detect TFA and STZ within the ranges of 50 μM–800 μM and 15 μM–120 μM, respectively. The limits of detection (LOD) for TFA and STZ are determined as 0.09 μM and 0.05 μM, respectively. While the limits of quantification (LOQ) are established at 0.3 μM and 0.17 μM, respectively. The feasibility of the method for determining TFA and STZ content in chicken samples was substantiated, demonstrating spiked recovery rates ranging from 97.5% to 102.3 % and 97.5%–99.8 %, respectively. The possible reaction mechanism was clarified based on chemiluminescence, UV–vis measurement and free radical analysis results. The newly established system is characterized by stability, convenience, and robust anti-interference capabilities, thus expanding the application of carbon dots and offering a promising strategy for the detection of TFA and STZ.
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Processes
·
2024
·Vol. 12
·期 7
·1384
·
IF 2.8
Wuning Yuan,Xiao Yang,Cheng Liu,Liangyao Xue,Wenzhe Niu,Qisheng Yan,Yajie Zhu,Junchao Han,Wen Guo,Bo Zhang
Sodium borohydride (NaBH4) is a nontoxic and ideal storage material for hydrogen due to its safety and high hydrogen storage capacity. In order to improve the practicality of the sodium borohydride hydrogen production system, we deposited non-precious metal catalytic materials on readily available polymer foams using a simple chemical plating method, developing a suitable 3D catalyst. Its high specific surface area enables it to produce hydrogen at a rate of up to 3.92 L min−1g−1. Its unique structure gives the catalyst excellent durability. In addition, an efficient NaBH4-based H2supply system was developed using this catalyst. Co-Cu-B can facilitate stable hydrogen production from NaBH4, yielding a consistent power output ranging from 0 to 100 W. This work provides a new pathway for developing high-efficiency monolithic self-supported catalysts for industrial applications.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Xinran Wang,Xufeng Zang,Hong Zhou,Na Wang,Yishan Fang,Bo Cui
Trichlorfon (TCF) has the possibility of contaminating agricultural crops and posing some health risks to humans. Herein, an electrochemiluminescence (ECL) sensor based on Fe, Cu dual-atom catalysts (Fe/Cu-N-C DACs) and Au@Luminol was developed for the ultrasensitive detection of TCF. Fe/Cu-N-C with diatomic sites has a very high catalytic activity and can be used as a co-reaction accelerator to activate H 2 O 2 to generate a large number of hydroxyl radicals which triggered a strong cathodic ECL signal of luminol. TCF molecularly imprinted polymer (MIP) was further introduced as a specific recognition element, and the interaction between the template molecule and the functional monomer was verified by molecular docking technique. The developed sensing platform was successfully applied to the ultrasensitive detection of TCF with a linear range from 1.0 pg/mL to 5.0 μg/mL with a low detection limit (0.39 pg/mL). This study broadens the application of DACs in ECL sensing.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Zhe Li,Yunshuo Wu,Haiqiang Wang,Zhongbiao Wu,Xuanhao Wu
Nitrous oxide (N2O) is a potent greenhouse gas with a high global warming potential, emphasizing the critical need to develop efficient elimination methods. Electrocatalytic N2O reduction reaction (N2ORR) stands out as a promising approach, offering room temperature conversion of N2O to N2 without the production of NOx byproducts. In this study, we present the synthesis of a copper-based single-atom catalyst featuring atomic Cu on nitrogen-doped carbon black (Cu1–NCB). Attributed to the highly dispersed single-atom Cu sites and the effective suppression of the hydrogen evolution reaction, Cu1–NCB demonstrated an optimal N2 faradaic efficiency (82.1%) and yield rate (3.53 mmol h–1 mgmetal–1) at −0.2 and −0.5 V vs RHE, respectively, outperforming previously reported N2ORR electrocatalysts. Further, a gas diffusion electrode cell was employed to improve mass transfer and achieved a 28.6% conversion rate of 30% N2O with only a 14 s residence time, demonstrating the potential for practical application. Density functional theory calculations identified Cu–N4 as the crucial active site for N2ORR, highlighting the significance of the unsaturated coordination and metal–support electronic structure. O-terminal adsorption of N2O was favored, and the dissociative adsorption (*ON2 → *O + N2) was the rate-determining step. These findings reveal the broad prospects of N2O decomposition via electrocatalysis.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Pengcheng Xiang,Lili Wang,Qin Geng,Changyan Guo,Hongtao Xie,Yizhao Li,Yangyang Yu,Jide Wang
Structural design of semiconductor photocatalysts plays an important role in promoting light absorption, molecular activation, and charge separation in the CO 2 reduction reaction, which is beneficial for improving photocatalytic activity. In this paper, a simple photodeposition strategy was employed to load Cu onto Bi 2 O 2 SO 4 and form a Cu-Bi alloy. Under simulated sunlight conditions, the optimal catalyst demonstrates impressive photocatalytic activity and selectivity for CO 2 reduction, with a corresponding yield of 18.8 μmol g -1 h -1 , 15 times higher than that of pure Bi 2 O 2 SO 4 , and CO selectivity reaching 97.1%. The results indicate that metal deposition enhances light absorption utilization efficiency and promotes the separation and transfer of photogenerated carriers. Additionally, the combination of in-situ FT-IR spectra and theoretical calculations reveal the molecular mechanisms of photocatalytic CO 2 reduction. This work discusses the synergistic effect of metal deposition and oxygen vacancies on photocatalytic reduction of CO 2 , providing a feasible method for constructing metal deposition structures with defects.
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CARBON
·
2025
·
IF 11.6
Changsheng Xing,Yunzhong Wu,Tong Zhang,Qingtan Ren,Jiaxu Shuang,Jie Li,Bin Liu,Jie Sheng,Lidong Wang,Weidong Fei
In the realm of advanced materials research, graphene/Cu composites have emerged as promising candidates due to their exceptional properties. This study explores the critical role of carbon source type in optimizing the performance of in-situ graphene/Cu composites. By systematically investigating 18-carbon chain olefins with different end-functional groups in octadecene (ODE), oleic acid (OA) and oleamine (OAM) as carbon sources, we uncover their profound impact on graphene quality, composite grain boundaries, and load transfer efficiency. OA and OAM can enhance carbon retention and promote the formation of Cu 2 O and Cu 3 N nanoparticles, thereby enhancing the binding of graphene/Cu interfaces and improving load transfer. Moreover, the functional groups in the carbon sources play a crucial role in copper grain refinement and strengthening, which enhances the overall mechanical properties. Specially, the composites prepared with OAM demonstrated superior mechanical properties, including the highest yield strength (468 MPa), tensile strength (515 MPa), and fracture elongation (11.9 %), as well as good electrical conductivity (87.8 % IACS) and a low resistance temperature coefficient (3.46 × 10 −3 °C −1 ). This study underscores the importance of carbon source selection in optimizing graphene/Cu composites and provides valuable insights into the intricate relationship between chemistry, microstructure, and material properties, paving the way for the rational design of multifunctional materials.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 20
·8750-8755
·
IF 3.5
Wenbo Zhao,Mengyao Li,Shi Hu
Direct ethanol fuel cells (DEFCs), which have been widely recognized as nontoxic and green energy conversion devices, show attractive application prospects for liquid hydrogen-carriers, due to the higher specific energy and lower toxicity of ethanol. Pt-based catalysts are widely used in DEFCs, while their poor poisoning resistance highlights the importance of composition and structure optimization. Herein, we synthesized a series of reduced graphene oxide supported ternary alloy AuxPt1−xCu3/rGO (x = 0-1) catalysts with excellent ethanol oxidation performance and a composition-dependent volcano plot trend of the ordering degree was observed and rationalized. The highest Pt-normalized mass activity of Au0.8Pt0.2Cu3/rGO is attributed to the optimized CO binding energy according to DFT calculations. This work not only provides an efficient EOR catalyst based on ordered alloys AuxPt1−xCu3 (x = 0-1), but also offers valuable insight into the role of a third metal in tuning the structure and function of alloys.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Rong Liu,Yan Gao
Titanium alloys are widely used in marine environments and medical fields due to their excellent corrosion resistance and high specific strength. However, their good biocompatibility can lead to severe biofouling, thereby limiting their effectiveness. To inhibit biofouling on the surface of titanium alloys, this study proposes an antifouling solution, which involves the in situ preparation of Cu-MOF film on titanium alloys by leveraging the antibacterial properties of Cu ions. Here, the dense and stable TiO2 film on the surface of Ti-6Al-4V titanium alloy was removed by alkali-heat treatment; meanwhile, a porous surface structure was simultaneously obtained where OH– ions were retained. In the subsequent step, the retained OH– ions in the pores attracted Cu2+ ions in solution to form Cu(OH)2 in the pores, providing active sites for the formation of Cu-MOFs. Subsequently, Cu(OH)2 reacted with organic ligand (1,3,5-benzenetricarboxylic acid, BTC) at room temperature to form Cu-MOFs in the pores, which then grew quickly to cover the alkali-heat-treated surface within 1 h. The formation mechanism of Cu-MOF film on Ti-6Al-4V was elucidated, which provides a reference for designing and preparing multifunctional MOF film in situ on titanium alloys. The stability of in situ-grown Cu-MOF samples and their inhibitory effects on bacteria and microalgae have also been verified. The results indicate that although the stability of Cu-MOFs is relatively poor, their bactericidal and algicidal effects are extremely significant, suggesting that this material has significant potential for short-term applications that require high antibacterial performance.
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