APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Haitao Yan,Didi Li,Zhaocong Jiang,Haoyuan Gu,Mengyuan Zhu,Yi-Fan Han,Minghui Zhu
Cu-based catalysts have been extensively used in the methanol steam reforming (MSR) reaction owing to low cost and high efficiency. In this work, we investigated the promotional effect of Fe on the Cu/ZnO/Al 2 O 3 catalysts prepared by an incipient-wetness impregnation method using a series of (quasi) in situ characterization techniques. The form of the Fe species was found to strongly depend on the Fe content. Fe species are present as highly dispersed FeO x in small amount of Fe with improved the dispersion of Cu. As Fe content increases, Fe species gradually transition to CuFe alloy and eventually to Fe 3 O 4 particles, leading to a decrease in Cu dispersion. With the gradual increase in Fe content, the apparent activity shows a volcanic trend, with CuAl-0.1Fe showing highest activity, whereas the intrinsic activity gradually decreases. Compared with CuAl- x Fe, adding moderate Fe to Cu/ZnO/Al 2 O 3 promotes the dispersion of Cu and Zn, forming abundant Cu-ZnO x interfacial sites, which improves both apparent and intrinsic activities. The best catalytic performance was obtained with the CuZnAl-0.1Fe catalyst, achieving the highest H 2 production rate of 134.7 mmol g cat −1 h −1 at 200 °C. This study reveals the role of Fe in Cu-based catalysts for MSR and inspires the design of improved Cu-based catalysts.
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Advanced Healthcare Materials
·
2025
·
IF 9.6
Hongyang Zhang,Rui-Hong Gong,Yu−Shan Lin,Tao Wang,Dou Luo,Jiahua Li,Li-Sha Shen,Wai-Yeung Wong,Sibao Chen,Guo-Qing Chen
Supramolecular polymers driven by the metal-ligand coordination possess reversible bonds, making them promising candidates for integrating the therapeutic functions of metal ions and small-molecule drugs, and subsequently releasing these components within cells after endocytosis. In this study, a kind of supramolecular polymer, SHICU, is developed, composed of Shikonin ligand and Cu(II) ion. Upon reduction by intracellular glutathione (GSH), SHICU dissociates to release Shikonin, Cu(II), and SHICU fragments. The released Shikonin and Cu(II) exhibit a synergistic antitumor effect through the reactive oxygen species (ROS)-dependent necrosis. Meanwhile, the released SHICU that remains structural integrity induces a distinct antitumor mechanism by triggering cuproptosis in tumor cells. This dual functionality, combining ROS-dependent necrosis and cuproptosis, highlights the potential of SHICU in advancing antitumor therapies, while the integration of supramolecular polymers with the emerging cell death mechanism of cuproptosis facilitates the development of innovative cancer drugs.
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PubMed
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MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Zhongqiu Zhao,Zixuan Zhou,Lei Wang,Ying Zhang,Yaguang Sun,Mingchang Zhu,Shuangyan Wu
Riboflavin was first isolated from milk and widely used in food, biological and pharmaceutical fields. Accurate detection of riboflavin content is of great significance for the treatment of related diseases and the supervision of food/drug quality. In this paper, a 1D chain copper-based coordination polymer with excellent water stability was synthesized by hydrothermal method using rigid ligand 1,10-phenanthroline and flexible ligand 1,4-phenylenedioxydiacetic acid, named Cu-phen-PEDA. Based on the Förster resonance energy transfer (FRET) and dynamic quenching detection mechanism, the emission spectrum of Cu-phen-PEDA overlaps with the absorption spectrum of riboflavin. As an energy donor in this case, Cu-phen-PEDA significantly increases the fluorescence intensity of riboflavin (energy acceptor), while simultaneously decreasing its own fluorescence intensity, which is an effective proportional-building strategy. In the lower concentration range, riboflavin can be specifically recognized by ratiometric fluorescence with a good linear relationship, and the detection limit is as low as 23 nM. The potential aspects of its specificity, stability, reusability and practical application were explored.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Zhao Xin,Li Changzhi,Wen Jie,Qiang Qian,Shen Zirong,Yu Haipeng,Zhou Xin,Yue Fengxia,Fang Ruiqi,Li Yingwei,Zhang Tao
Lignin refining still suffers from great challenges of selective depolymerization and cleavage of stubborn C‒C linkages. Here, a robust atomically dispersed Cu/Ni-SA@HNC catalyst is fabricated for super-selective hydrogenolysis of lignin and model compounds via an unusual “preferential C α –C β bond cleavage in β-O-4 linkages” pathway, affording toluene in yield up to 75.7% from β-O-4 model compounds, and up to 33.7 ± 1.6 wt% (nine parallel experiments) from poplar lignin. The catalyst exhibits high stability, and the scale-up potential is demonstrated by the high space-time yield of toluene (33.7 g·g cat −1 ·h −1 ) in continuous flow reaction of β-O-4 model compound. The origin of the extraordinary selectivity towards C α –C β bond cleavage rather than C‒O bond cleavage in β-O-4 model compounds is uncovered. This work conquers the major challenges in lignin valorization by using non-noble dual-metal single-atom catalyst, not only showcasing the application perspective of atomically dispersed catalysts in biopolymer refinery, but also providing a cost-efficient, petroleum independent solution to valuable commodity chemicals.
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ACS Nano
·
2024
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IF 15.8
Minglei Lu,Zhuoyu Zheng,Weiwei Lu,Haiping Zhu,Junwei Liao,Yuxin Ge,Xueer Huang,Qian Zhang,Jiajin Li,Yiyuan Zhou,Xiaoping Wu,Baozhu Chen,Chunxiao Yang,Xitang Qian,Minhua Shao,Tiejun Wang
Aqueous-phase reforming of methanol represents a promising avenue for hydrogen (H2) production. However, developing highly efficient and low-cost nonprecious catalysts remains challenging. Here, we report the synthesis of Cu-based catalysts with Cu, Cu2O, and CuN3 nanoparticles anchored on the nitrogen-doped carbon, forming Cu0/Cu+/Cu-N3 active sites. This catalyst achieves a H2 production rate of 140.1 μmol/gcat/s at 210 °C, which is several times to 2 orders of magnitude higher than that of Cu-, Ni-, even Pt-based catalysts, demonstrating excellent long-term stability over 350 h at 210 °C. A mechanism investigation reveals that the Cu-N3 site facilitates water dissociation into *OH and improves *CO and *OH conversion, leading to enhanced CO conversion and H2 production kinetics.
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MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Xiao-Zhen Feng,Kun-Zhi Wang,Ke-Hang Song,Guo-Cheng Han,Bing-Lun Li,Heinz-Bernhard Kraatz
Moxifloxacin (MOX) and gatifloxacin (GAT) are structurally similar and possess close oxidation peak potentials, making it difficult for simultaneous detection by electrochemical methods. To address this, an electrochemical sensor was constructed with reduced graphene oxide (rGO) and copper porphyrin complex (Cu-TCPP), achieving signal amplification and simultaneous detection of MOX and GAT. The linear relation range from 5.00 to 600.00 μmol·L −1 for MOX (LOD is 1.34 μmol·L −1 ) and 10 to 300 μmol·L −1 for GAT (LOD is 0.59 μmol·L −1 ). When applied to water samples, it achieved recoveries of 100.09–112.02 % with a relative standard deviation (RSD) of less than 6 % for MOX, and 97.27–110.72 % with an RSD of less than 4 % for GAT. Further calculations indicated that the electro-oxidation of GAT involved two protons and two electrons.
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Nanoscale Horizons
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2025
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IF 6.6
Xiao Wan Han,Xu Chen,Tianle Yang,Ying Yi Luo,Rui Xue Liang,San Qi An,Xinli Liu
Cuproptosis has recently received much attention in cancer treatment. However, copper ionophores don’t show the obvious clinical efficacy. Although some Cu-based and copper ionophores-loaded nanomaterials have been applied to induce cuproptosis, it is difficult to achieve the clinical translation limited by the complicated composition, harsh synthesis condition, external stimulus, and potential biotoxicity. Phytic acid, a naturally occurring organic phosphorus carbohydrate, possesses distinct antineoplastic effect on multiply types of cancer and high biocompatibility. Based on metal-phosphonate coordination, a novel Cu-phytic acid nanozyme (denoted as CP) with pH/GSH dual-response was fabricated by a “one-spot” method. CP with three enzyme-mimicking activities enhanced cuproptosis therapy through GSH depletion, reactive oxygen species augment, hypoxia relief and the attenuation of glycolysis. As a proof of concept, Elesclomol (a copper ionophore)-resistant A549 cells were used to investigate CP- induced cuproptosis for inhibition of tumor growth in vitro and in vivo.
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ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Zhenyao Li,Wei Wei,Xuli Hu,Zhen Zhang,Yangshun Hu,Yushan Wu,Yao Wang,Junchen Xu,Mingyue Ding
While engineering lattice strain has been proven effective in enhancing the electrochemical CO 2 reduction performance of a catalyst, the correlation between strain effect and the intrinsic catalytic mechanism has remained elusive. Herein, a photolithography-inspired method is proposed to regulate Cu(111) lattice strain. By irradiating the photosensitive Cu(Acac) sol–gel, Acac chelate bond undergoes π→π * electronic transition, and the ring-closed Cu(Acac) decompose into the stabilized Cu(Acac) mesh which presents as nanospots embedded onto the surface of the Cu cluster. The photoinduced nanospots serve to exert compressive strain to the Cu(111) lattice in which the lattice distance is reduced by 5.7–11.4%. Herein, the catalyst with 11.4% lattice compression exhibits enhanced C 2 H 4 production capabilities, reaching a maximal Faradaic efficiency of 57.00%, and a high partial current density of 456.01 mA cm −2 . Theoretical calculations reveal that the compressed Cu(111) lattice exhibits reduced surface energies, leading to a significant drop in the C─C coupling reaction free energy from 1.16 eV over the pristine lattice, to 0.57 eV over the 10% compressed lattice. Additionally, the 10% compressed lattice facilitates spontaneous *O splitting immediately after OC─CHO coupling which leads to the generation of C 2 H 4 -favoring *CCH intermediate.
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COMPOSITES COMMUNICATIONS
·
2025
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IF 7.7
Ke Zhang,Minghui Ou,Yujie Xiao,Zhiwei Wei,Li Yang,Yi Xie,Changsheng Zhao
Copper-based nanozymes have emerged as promising therapeutic agents for oxidative stress-related diseases due to their enzyme-mimicking properties. However, their development is still limited by poor biocompatibility, insufficient broad-spectrum free radical scavenging ability, and potential toxicity from Cu 2+ leakage. To address these challenges, we developed Cu@EA-BTC, a broad-spectrum antioxidant material, by integrating ellagic acid (EA) into copper-based metal-organic frameworks (Cu@BTC). The Cu@BTC serves as a stable copper source, while the EA endows the Cu@EA-BTC with broad-spectrum ROS scavenging and enhanced catalase (CAT)-like activity via facilitating the reduction of Cu 2+ to Cu + . As a result, the Cu@EA-BTC exhibits superior antioxidant properties and excellent biocompatibility, including both cellular and blood compatibility. Meanwhile, the Cu@EA-BTC effectively protects immune cells from oxidative damage, which indicates its potential for oxidative stress-related therapies. This study provides a promising strategy for developing safe and efficient nanozyme-based antioxidant materials for biomedical applications.
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Energy & Environmental Science
·
2024
·
IF 32.4
Liqun Wang,Jingting Jin,Wenzhi Li,Cunshuo Li,Leyu Zhu,Zheng Zhou,Lulu Zhang,Xia Zhang,Liang Yuan
Direct conversion of methane into high value-added products is of great practical significance. The synergistic effect in catalysts with dual-active components show potential to increase the methanol yield and selectivity. In this work, Cu–Pd/anatase is in situ generated and exhibits a relatively high methanol yield rate of ∼31 800 μmol gcat−1 h−1 and near-exclusive selectivity of liquid products (methanol). The reaction mechanism behind the heterogeneous catalysis process has been investigated. It is confirmed that copper ions hold the ability to produce hydrogen peroxide which can be further promoted by anatase. Chlorine ions can promote the stable adsorption of CO and the formation of *CH3 intermediates, facilitating high activity and selectivity for methanol production. Pd and Cu cooperatively dissociate methane, which promotes the formation of key configuration metal-CH3. The ˙CH3 intermediate desorption will be facilitated on Cu–Pd/anatase through the manner of electron regulation, which is proved by the combination of density functional theory calculations and in situ infrared spectroscopy. Methanol is formed when a ˙CH3 is desorbed from a copper site and combines with a hydroxyl radical.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Mengyao Shi,Qiang Yin,Da Wang,Chengcheng Tian,Lei Zhou
The widespread presence of Cu(II) in aquatic environment has attracked increasing interests in Cu(II)-mediated advanced oxidation processes (AOPs) as a promising “two-birds-one-stone” strategies for environmental remediation. Organically coordinated Cu(II) systems offer dual benefits on facilitating efficient copper redox cycling and generating reactive species for pollutant degradation. However, the activation efficiency disparities among different peroxides and their underlying mechanisms remain poorly understood. Herein, this study presents a comprehensive comparison of organically-cooridinated Cu(II) activated peroxydisulfate (PDS), peroxymonosulfate (PMS) and hydrogen peroxide (H 2 O 2 ) systems, where ofloxacin (OFX) serving as coordinating ligand and target contaminant. Our results demonstrate enhanced activation for all the three peroxides, leading to significantly improved OFX degradation. High-valent copper species Cu(III) is identified as the primary working intermediate across all systems. The peroxides activation efficiency, OFX decay enhancement, and steady-state Cu(III) concentration consistently followed an order of PDS > H 2 O 2 > PMS. The performance differences among the three systems were governed by the initial contact probability between peroxides and copper center and the subsequent electron transfer efficiency, which is further verified by molecular dynamics (MD) simulations. This work establishes a quantitative framework for predicting peroxides activation properties in Cu(II)-mediated AOPs, offering fundamental insights for designing efficient dual-functional systems that combine heavy metal stabilization with organic pollutant degradation in wastewater treatment.
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ACS Catalysis
·
2025
·
IF 13.1
Guihua Yan,Paulina Pršlja,Gaofeng Chen,Jiahui Kang,Yongde Liu,Miguel A. Caro,Xi Chen,Xianhai Zeng,Bo Peng
Syngas conversion into higher alcohols represents a promising avenue for transforming coal or biomass into liquid fuels. However, the commercialization of this process has been hindered by the high cost, low activity, and inadequate C2+OH selectivity of the catalysts. Herein, we have developed Cu/Co carbon wood catalysts, offering a cost-effective and stable alternative with superior selectivity for catalytic conversion. The formation of Cu/Co nanoparticles was found, influenced by water-1,2-propylene glycol ratios in the solution, resulting in bidisperse nanoparticles. The Cu/Co-CW-W1P1 catalyst (the ratio between water and 1,2-propanediol is 0.5:0.5) exhibited a remarkable CO conversion rate of 74.8% and a selectivity of 58.7% for C2+OH, primarily comprising linear primary alcohols. This catalyst demonstrated enduring stability and selectivity under industrial conditions, maintaining its efficacy for up to 350 h of operation. We also employed density functional theory (DFT) to analyze selectivity, particularly focusing on the binding strength of CO, a crucial intermediate for subsequent reactions leading to the formation of alcohols. DFT identified the pathway of CHx and CO coupling, ultimately yielding C2H5OH. This computational understanding, coupled with the high performance of the Cu/Co-carbon wood catalyst, paves the way to develop catalytically selective materials tailored for higher alcohol production from a nature-based source.
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