INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Wenhua Feng,Ze Xiao,Binyi Chen,Yunhong Pi,Changsong Hu,Wenli Zhang,Qingwei Meng,Tiejun Wang
As non-noble metal catalyst, Cu-based catalyst shows promising applying potential in the aqueous-phase reforming of methanol (APRM) due to its high dehydrogenation activity and low CO selectivity, but the poor thermal and hydrothermal stability. Herein, a Cu@S-1 catalyst with ultrasmall-2nm Cu nanoparticles size was synthesized for the first time using one-step in-situ encapsulation strategy. By the confinement effect of the zeolite Silicalite-1 (S-1) micropores, the 1 wt%Cu@S-1 catalyst exhibited absolutely superior thermal stability without using any other promoter, as well as relatively good hydrothermal stability. After 600–700 °C high-temperature treatment, no obvious aggregation of the Cu nanoparticles was found, and superior performance in the steam reforming of methanol (SRM) was maintained after running for 36 h at 300 °C. In the APRM at 210 °C, the 1 wt%Cu@S-1 catalyst showed six-fold higher hydrogen releasing rate (4.26 × 10 5 μ mo l H 2 · g Cu − 1 · h − 1 ) than the impregnated 1 wt%Cu/S-1-im catalyst, meanwhile it exhibited even better performance than the commercial 5%Pd/C catalyst. Compared with the impregnated 1 wt%Cu/S-1-im catalyst, the confinement effect of the internal pores of the S-1 for the Cu nanoparticles in the 1 wt%Cu@S-1 catalyst effectively inhibited aggregation of the Cu particles and Cu leaching in APRM, thus greatly improved the activity and hydrothermal stability.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Jiahui Zhao,Yixuan Zhao,Xuefeng Shao,Ying Sun,Huang Wen,Jian Liu
Developing a synthesis-free, multifunctional, and effective colorimetric assay system based on 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation is attractive yet challenging. Herein, we established a synergetic Cu2+/Cr6+-promoting strategy for TMB-based colorimetric detection of Cr6+. By introducing Cu2+, critical TMB·+···Cu(I/II)···TMB charge transfer complex (TMC) intermediates were in situ formed to reduce the activation energy of TMB oxidation, thereby accelerating Cr6+-mediated TMB oxidation. TMC intermediates also played a pivotal role in H2O2-participated TMB oxidation, clarifying the secondary responsibility of reactive oxygen species frequently caused by Fenton-like reactions. Leveraging the synergetic capacity between Cu2+ and Cr6+ for TMB oxidation, we demonstrated sensitive and specific colorimetric detections for Cr6+ with a limit of detection of 0.006 μM. With its convenient operation and rapid responsiveness, this strategy successfully enabled the practical detection of Cr6+ in real water samples. This work not only enhances the understanding of the internal acceleration mechanism in colorimetric sensing but also provides valuable opportunities to advance synthesis-free detection platforms.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yifan Cui,Dezhi Yang,Qiulan Li,Zhongmei Peng,Zitao Zhong,Yuzhu Song,Qinqin Han,Yaling Yang
Nanozyme-mediated antioxidative therapy is a promising star for treating a myriad of important diseases through eliminating excessive reactive oxygen species (ROS) such as O2·– and H2O2, a critical mechanism for inflammatory bowel disease (IBD). This work provides a high biocompatibility iodine–copper–zinc covalent doped carbon dots (Cu,Zn,I-CDs) with the catalase (CAT)-, superoxide dismutase (SOD)- and glutathione peroxidase (GPx)-like catalytic activities for treating ulcerative colitis (UC) by scavenging overproduced ROS. We found that I dopant aids in counteracting the positive charge at Cu,Zn dopants brought on by low pH, enabling Cu,Zn,I-CDs to process strong triple antioxidant nanozyme activities rather than Cu,Zn-CDs. Vitro experiments displayed that the Cu,Zn,I-CDs could scavenge the excessive ROS to protect cellular against oxidative stress and reduce the expression of proinflammatory cytokines, such as TNF-α, IL-1β, and IL-6. In sodium dextran sulfate (DSS)-induced colitis mice models, Cu,Zn,I-CDs with excellent biocompatibility could effectively relieve the inflammation of the colon, containing the reduction of the colon length, the damaged epithelium, the infiltration of inflammatory cells, and upregulation of antioxidant genes. Therefore, the therapy of Cu,Zn,I-CD antioxidant nanozymes is an effective approach and provides a novel strategy for UC treatment.
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Catalysts
·
2024
·Vol. 14
·期 12
·929
·
IF 3.8
Jingxin Tan,Mengqi Li,Lingtao Liu,Lijian Wang,Haocun Wang,Junjie Bian,Chunhu Li
Biomass platform compound 5-Hydroxymethylfurfural (HMF), with its low price and abundant source, can be used as a renewable resource to replace traditional petrochemicals. MOF-808(Zr) has tunable active sites and excellent stability under high temperatures and acidic as well as basic environments, and the unsaturated coordination of metal ions within its framework structure can exhibit Lewis acidity, facilitating catalytic transfer hydrogenation from HMF to 2, 5-Furandimethanol (BHMF). The hydrothermal–impregnation–reduction method was used to prepare Cu/MOF-808 catalysts with high catalytic performance. Formic acid was chosen as the hydrogen donor solvent. The selectivity and yield of BHMF were 75.65% and 71%, respectively, at 150 °C for 4 h. A reaction pathway for the catalytic hydrogen transfer of HMF to BHMF was proposed. The high activity and stability of the Cu/MOF-808 catalyst with dual active sites provide a viable method for feasible hydrogenation of HMF to high value-added compounds.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
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IF 8.4
Wenjing Yang,Hexue Jia,Tingting Li,Yuepeng Liu,Yi Li
Superoxide radicals (·O 2 − ) has been regarded as one of the reactive oxygen species (ROS) for the elimination of complex contaminants via electro-Fenton like (EF-like) technology. However, the generation path of ·O 2 − is diverse, and the influence of the physicochemical properties of metals on the mechanism of ·O 2 − conversion is significant in the EF-like treatment of wastewater. Herein, metals (M = Mn, Cu) loaded zeolitic imidazolate frameworks catalytic materials (M–NC) were prepared for sulfamethoxazole (SMX) removal to analyze the effect of metals on the pathways of ·O 2 − generation. The removal kinetic rate of SMX by Cu–NC was 1.32 times higher than that of Mn–NC. Quenching experiments demonstrated that ·O 2 − is the most important oxidizing species to achieve SMX removal. The RRDE measurements and quantitative experiment on the concentration of H 2 O 2 experiments indicated that Mn–NC was more inclined to generate ROS through activation of H 2 O 2 and Cu–NC through other ways. Therefore, the transformation pathways of ·O 2 − in different catalytic systems were thoroughly analyzed. Electron paramagnetic resonance test and reactive oxygen species quenching experiments indicated that the pathway for ·O 2 − production of Mn–NC was O 2 → H 2 O 2 → ·O 2 − , and that of Cu–NC was O 2 → ·O 2 − . The strategy of using Mn and Cu-based catalysts to investigate the mechanism of the ·O 2 − generation pathway provided a way to efficiently utilize the conversion of ·O 2 − .
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TRIBOLOGY INTERNATIONAL
·
2024
·
IF 6.1
Zeyang Wu,Jie Fei,Chang Li,Jifeng Yan,Xinyu Ke,Lehua Qi
As a nanoscale carbon material, carbon spheres (CS) are expected to achieve ideal lubrication performance by reducing direct contact between friction pairs and bearing loads. In this work, 2D Cu-MOFs surface modified (CS@Cu(BDC)) CS was added to the base oil, which exhibited a remarkable reduction in friction coefficient and wear rate (62.2%, 33.9%), the width of the friction pair wear marks was decreased by 30.8% relative to the base oil. The improvement in performance can be attributed to the polishing, repairing, filling and tribo-film forming effects of CS@Cu(BDC). This work provided an effective strategy for diversifying the surface structure of CS and opened new avenues for the development of a new generation of green and efficient lubricant additives .
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PROTEINS-STRUCTURE FUNCTION AND BIOINFORMATICS
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2024
·
IF 3.2
Wenwei Tang,Zuxun Huang,Yunying Liu,Xinping Zeng
The microbial manganese removal process is believed to consist of the catalytic oxidation of Mn(II) by manganese oxidase. In this study, the multicopper oxidase CopA was purified and exhibited high manganese oxidation activity in vitro, and it was found that Cu(II) can significantly enhance its manganese oxidation activity. Gene site-directed mutagenesis was used to mutate four conserved copper binding sites of CopA to obtain four mutant strains. The manganese removal efficiencies of the four strains were determined, and it was found that H120 is the catalytically active site of CopA. The loss of Cu(II) and the mutation of the conserved copper binding site H120 resulted in the loss of ethoxyformyl and quinone modifications, a reduction in the number of modifications, and a change in the position of modifications, eventually causing a decrease in protein activity from 85.87% to 70.1%. These results reveal that Cu(II) and H120 play an indispensable role in manganese oxidation by the multicopper oxidase CopA. X-ray photoelectron spectroscopy (XPS) analysis indicates that biogenic manganese oxides produced by strains and by CopA were both composed of MnO 2 and Mn 3 O 4 and that the average valence of Mn was 3.2.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Xubing Sun,Shiyu Yin,Li Zhao,Wenhua Yang,Yaohui You
In this work, tannic acid was selected as a green cross-linking agent to cross-link carboxymethyl chitosan to prepare a magnetic adsorbent (CC-OTA@Fe 3 O 4 ), which was used to remove methylene blue (MB) and Cu 2+ . CC-OTA@Fe 3 O 4 was characterized by FTIR, 13 C NMR, XRD, VSM, TGA, BET and SEM. The adsorption behavior was studied using various parameters such as pH value, contact time, initial concentration of MB and Cu 2+ , and temperature. The results showed that adsorption of MB and Cu 2+ followed the pseudo-second-order model and the Sips model. The maximum adsorption capacities were determined to be 560.92 and 104.25 mg/g MB and Cu 2+ at 298 K, respectively. Thermodynamic analysis showed that the adsorption is spontaneous and endothermic in nature. According to the results of FTIR and XPS analyses, the electrostatic interaction was accompanied by π–π interaction and hydrogen bonding for MB adsorption, while complexation and electrostatic interaction were the predominant mechanism for Cu 2+ adsorption. Furthermore, CC-OTA@Fe 3 O 4 displayed remarkable stability in 0.1 M HNO 3 , exhibited promising recyclability, and could be easily separated from aqueous solutions in the magnetic field. This study demonstrates the potential of CC-OTA@Fe 3 O 4 as an adsorbent for the removal of cationic dyes and heavy metals from wastewater.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Zhichao Ma,Chenyi Wang,Tianfang Yang,Gangya Wei,Jinrui Huang,Mengran Liu,Kun Zhang,Zunjie Zhang,Yang Liu,Shuyan Gao
Electrocatalytic nitrate (NO3−) reduction to ammonia (NH3) (NRA) is of great significance for solving the problem of urgent NO3− pollution in the environment and opening up a new route to synthesize NH3. However, NRA is limited by its multi-electron/proton transfer process and the NRA process relies heavily on atomic H* produced by H2O splitting, undergirding the necessity for effective NRA catalysts. Herein, three-dimensional (3D) porous phosphorus (P)-doped Cu–Ni alloy materials are constructed through a one-step electrodeposition synthesis. 3D porous materials modulate hydrophilicity and enrich active sites. The Cu d-band center can be tuned through Ni alloying to modify the adsorption energies of intermediates such as *NO3−, *NO2−, and *NH2. The hydrogenation evolution capacity of P promotes the hydrogenation process in the atomic H* path and effectively accelerates the NRA reaction rate. Density functional theory (DFT) calculations demonstrate that the charge transfer between the negatively charged Pδ− and the positively charged Niδ+ and Cuδ+ assists in generating more atomic H* for coupling with reaction intermediates, showing an enhanced catalytic activity at low overpotential. The optimal sample exhibits an exceptional NRA performance with an ammonia yield rate of 848.1 μmol h−1 cm−2 and a faradaic efficiency of 96.1%. This work provides a strategy for creating effective NRA catalysts through enhancing the atomic H* reduction strategy.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2024
·Vol. 22
·期 1
·1-19
·
IF 10.6
Wang Yining,Zhou Qiaomei,Luo Wangping,Yang Xiaoyan,Zhang Jinguo,Lou Yijie,Mao Jin,Chen Jiayi,Wu Fan,Hou Jue,Tang Guping,Bai Hongzhen,Yu Risheng
Pancreatic ductal adenocarcinoma (PDAC), characterized by a dense extracellular matrix (ECM), presents significant therapeutic challenges due to its poor prognosis and high resistance to chemotherapy. Current chemodrugs and diagnostic agents largely fail to cross the barrier posed by the ECM, which severely limits the PDAC theranostics. This study introduces a novel theranostic strategy using thioether-hybridized hollow mesoporous organosilica nanoparticles (dsMNs) for the co-delivery of copper (Cu) and disulfiram (DSF), aiming to induce cuproptosis in PDAC cells. Our approach leverages the ECM-degrading enzyme collagenase, integrated with dsMNs, to enhance drug penetration by reducing matrix stiffness. Furthermore, the innovative use of a pancreatic cancer cell membrane coating on the nanoparticles enhances tumor targeting and stability (dsMCu-D@M-Co). The multifunctional platform not only facilitates deep drug penetration and triggers cuproptosis effectively but also utilizes the inherent properties of Cu to serve as a T1-weighted magnetic resonance imaging (MRI) contrast agent. In vitro and in vivo assessments demonstrate significant tumor size reduction in PDAC-bearing mice, highlighting the dual functionality of our platform in improving therapeutic efficacy and diagnostic precision. This integrated strategy represents a significant advancement in the management of PDAC, offering a promising new direction for overcoming one of the most lethal cancers.Graphical Abstract
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RARE METALS
·
2024
·Vol. 43
·期 8
·3702-3712
·
IF 9.6
Mu Zi-Jie,Gao Yan-Jun,Dong Wen-Shuai,Li Zong-You,Song Qing-Yi,Huang Han-Jiao,Xing Li-Dong,Zhang Jian-Guo,Wang Wei,Yu Qi-Yao
The highly reversible insertion/extraction of large-radius K + into electrode materials remains a tough goal, especially for conversion-type materials. Herein, we design a current collector-integrated electrode (N–CoSe/CoSe 2 –C@Cu) as an advanced anode for potassium-ion battery (PIBs). The conductive CoSe/CoSe 2 heterojunction with rich Se vacancy defects, conductive sp 2 N-doped carbon layer, and the elastic copper foil matrix can greatly accelerate the electron transfer and enhance the structural stability. Consequently, the well-designed N–CoSe/CoSe 2 –C@Cu current collector-integrated electrode displays enhanced potassium storage performance with regard to a high capacity (325.1 mAh·g −1 at 0.1 A·g −1 after 200 cycles), an exceptional rate capability (223.5 mAh·g −1 at 2000 mA·g −1 ), and an extraordinary long-term cycle stability (a capacity fading of only 0.019% per cycle over 1200 cycles at 2000 mA·g −1 ). Impressively, ex situ scanning electron microscopy (SEM) characterizations prove that the elastic structure of copper foil is merged into the cleverly designed N–CoSe/CoSe 2 –C@Cu heterostructure, which buffers the deformation of structure and volume and greatly promotes the cycle life during the potassium/depotassium process. Graphical abstract
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Small
·
2025
·
IF 12.1
Shaojian Jiang,Yuhang Liu,Ruidong Yang,Lijun Zhang,Wenke Liu,Kai Deng,Hongjie Yu,Hongjing Wang,Liang Wang
Since formaldehyde oxidation reaction (FOR) can release H 2 , it is attractive to construct a bipolar hydrogen production system consisting of FOR and hydrogen evolution reaction (HER). Although copper-based catalysts have attracted much attention due to their low cost and high FOR activity, the performance enhancement mechanism lacks in-depth investigation. Here, an amorphous-crystalline catalyst of amorphous nickel hydroxide-coated copper dendrites on copper foam (Cu@Ni(OH) 2 /CF) is prepared. The modification of Ni(OH) 2 resulted in hydrophilic and aerophobic states on the Cu@Ni(OH) 2 /CF surface, facilitating the transport of liquid-phase species on the electrode surface and accelerating the release of H 2 . The Open circuit potential (OCP) and density functional theory (DFT) calculations indicate that this core–shell structure facilitates the adsorption of HCHO and OH − . In addition, the catalytic mechanism and reaction pathway of FOR are investigated through in situ FTIR and DFT calculations, and the results showed that the modification of Ni(OH) 2 lowered the energy barrier for C─H bond breaking and H─H bond formation. In the HER//FOR system, Pt/C//Cu@Ni(OH) 2 /CF can provide a current density of 0.5 A cm −2 at 0.36 V and achieve efficient and stable H 2 production. This work offers new ideas for designing electrocatalysts for bipolar hydrogen production system assisted with formaldehyde oxidation.
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