INORGANIC CHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.4
Xuyong Tang,Fengxi Li,Sijun Huang,Li Xu,Lei Wang,Yi Guo
Nicotinamide-adenine dinucleotide (NADH) as biomimetic units combined with copper ion to form laccases mimics (Cu-NADH). Cu-NADH has the enhanced activity of copper center to mediate aryl C–H amination using air as green oxidants. It could successfully catalyze oxidative coupling between different aromatic compounds and 4-phenylurazole (yield: 72 ∼ 91 %). Recycling catalytic ability (up to 6 times) showed its excellent stability. The Cu-NADH nanozyme was certificated to catalyze C–H amination effectively, and highlighted that it was a proper way to design catalysts according to enzyme-like catalyzing non-natural reaction.
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NATURE MATERIALS
·
2025
·
IF 38.5
Li Zhe,Wang Yueshuai,Liu Hui,Feng Yi,Du Xiwen,Xie Zhiheng,Zhou Jihan,Liu Yang,Song Yun,Wang Fei,Sui Manling,Lu Yue,Fang Fang,Sun Dalin
Precious metals such as Pt are favoured as catalysts for the hydrogen evolution reaction (HER) due to their excellent catalytic activity. However, the scarcity and high cost of precious metals have prompted researchers to explore cheaper alternatives such as Cu. Nevertheless, Cu shows poor catalytic performance due to weak binding with intermediates. Here the catalytic activity of pure Cu is activated via electroreduction-driven modification of the local structure, achieving a HER catalytic performance superior to commercial Pt/C catalysts for working current densities greater than 100 mA cm −2 in acid electrolyte. Activation involved two steps. First, polycrystalline Cu 2 O nanoparticles were prepared via pulsed laser ablation, resulting in grain boundaries within the Cu 2 O particles as observed using electron microscopy. Next, the Cu 2 O particles were electroreduced to pure Cu, inducing the formation of distorted nanotwins and edge dislocations. These local structures induce high lattice strain and decrease the Cu coordination number, enhancing the interaction between Cu and intermediates—as calculated using density functional theory—leading to the excellent catalytic activity and durability of the catalyst. Our observations show that low-cost pure Cu can be a promising HER catalyst for large-scale industrial applications.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Yaohua Gu,Jiping Han,Ni Zhang,Weisong Yan,Yue Guo,Huiyi Tan,Changyi Yang,Fuke Wang,Huiqin Yao
Nanozyme possess the advantages of high enzyme simulation activity, low cost, and excellent stability. As a substitute for natural enzymes, nanozyme have demonstrated significant potential in various fields. In this study, a bimetallic organometallic framework Cu@Co-MOFs was synthesized via the hydrothermal method using terephthalic acid (H2BDC) as a ligand and characterized. Cu@Co-MOFs exhibits outstanding peroxidase activity (POD) by catalyzing the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) and other color-developing substrates through •OH formation. A simple, rapid, and reliable colorimetric method for quantitatively detecting glutathione (GSH) was developed based on the Pod-like activity of Cu@Co-MOFs. The linear range of this method was 1–1200 μM with a detection limit of 0.72 μM. This work not only proposes a bimetallic organic framework with high POD as a straightforward and practical platform for visually detecting GSH but also provides a strategy to enhance the performance of nanomaterials.
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
·
2011
·Vol. 49
·期 12
·2588-2593
·
IF 3.894
Jing Ma,Hou Chen,Min Zhang,Lingfang Chen
Single electron transfer-living radical polymerization (SET-LRP) has been used as a new technique for the synthesis of polyacrylonitrile (PAN) catalyzed by Cu(0) powder with carbon tetrachloride (CCl 4 ) as the initiator and hexamethylenetetramine (HMTA) as the ligand in N , N -dimethylformamide (DMF) or mixed solvent. Well-controlled polymerization has been achieved as evidenced by a linear increase of molecular weight with respect to monomer conversion as well as narrow molecular weight distribution. Kinetics data of the polymerizations at both ambient temperature and elevated temperature demonstrate living/controlled feature. An increase in the concentration of ligand yields a higher monomer conversion within the same time frame and almost no polymerization occurs in the absence of ligand due to the poor disproportionation reaction of Cu(I). The reaction rate exhibits an increase with the increase of the amount of catalyst Cu(0)/HMTA. Better control on the molecular weight distribution has been produced with the addition of CuCl 2 . In the presence of more polar solvent water, it is observed that there is a rapid increase in the polymerization rate. The effect of initiator on the polymerization is also preliminarily investigated. © 2011 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2011
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ChemistrySelect
·
2024
·Vol. 9
·期 44
·e202403927
·
IF 1.9
Hui Han,He Cui,Jiabo Wang,Kai Ge,Yongfang Yang
Graphical In this paper, 2D MOF-Co, 2D MOF-Co/Cu, and 2D MOF-Co/Cu/Fe are designed and prepared using 1,4-benzendicarboxylic acid (1,4-BDC) as organic ligands. Their charge transfer, separation efficiency, and effects on photocatalytic CO 2 reduction are studied. The results show that 2D multimetallic MOF-Co/Cu/Fe has better photocatalytic CO 2 reduction activity, so it has higher research value and development prospect in the field of photocatalytic CO 2 reduction. In this study, 2D multimetallic MOFs combined with the advantages of 2D nanosheets, with the synergetic effect of multimetallic nodes, exhibited good photocatalytic activity for reduction of CO 2 . Herein, a 2D MOF-Co/Cu/Fe were successfully prepared via one-pot stirring of the solutions of multimetal salts and organic ligands at room temperature. Introduction of the second and third metal (Cu and Fe) into MOF-Co does not change the 2D morphology of MOFs, although it improved the photocatalytic CO 2 reduction performance by broadening the light absorption range of 2D MOF-Co, accelerating the separation efficiency and transfer rate of photogenerated carriers. Upon irradiation with full-spectrum light, the average CO yield of 2D MOF-Co/Cu/Fe achieved 17.06 µmol·g −1 ·h −1 , being about 1.8 and 1.2 times that of 2D MOF-Co and 2D MOF-Co/Cu. This work provides an insight into 2D multimetallic MOFs-based photocatalysts in catalytic CO 2 reduction.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Minglu Li,Siyu Kuang,Yaxin Jin,Haoyuan Chi,Sheng Zhang,Xinbin Ma
Copper-based catalysts exhibit an excellent ability in producing C 2 chemicals during CO 2 RR. However, the unsustainable Faradic efficiency (FE) resulting from the reconstruction makes keeping catalyst behavior challengeable. In this study, we synthesized CuO nanosheets and incorporated a small amount of nickel on surface to improve the stability of nanosheets. By inhibiting the dissolution of Cu through the incorporation of Ni, our CuO + Ni-surface catalyst could achieve a double increase in stability compared to CuO nanosheets. Using a combination of electrochemistry, density functional theory calculations, in situ UV–vis spectrometer and inductively coupled plasma optical emission spectrometry, we elucidate the mechanisms behind the increased stability. The incorporation of Ni reduces the tendency of Cu oxidation at higher overpotential and strengthens the bonds between surface and subsurface Cu atoms. This work highlights a promising approach to enhance the stability and efficiency of copper-based catalysts in CO 2 RR, proposing the way for more sustainable catalytic processes.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Zihan Lv,Zeng Hong,Da Ke,Chao Qian,Xinzhi Chen,Shaodong Zhou
The selective hydrogenation of nitrile compounds represents a pivotal area of research within both industrial and academic catalysis. In this study, we prepared Ni-Cu bimetallic catalysts through a co-deposition-crystallization sequence, aimed at the efficient production of primary and secondary amines. The enhanced selectivity for primary amines is attributed to the downshift of the d-band center of Ni 0.1 Cu, which weakens the adsorption of key imine intermediates. Consequently, the synthesized Ni-Cu catalysts demonstrated exceptional catalytic performance in the selective hydrogenation of nitrile compounds, including those with reduction-sensitive functional groups such as −Cl and −Br, achieving 100 % conversion efficiency and significant yields ranging from 80 % to 99 %. The reaction conditions were comprehensively optimized, taking into account factors such as temperature, solvent, time, additives, and hydrogen pressure. Furthermore, the catalytic performance of Ni 0.1 Cu and Ni 0.4 Cu in the selective hydrogenation of nitriles was sustained over at least five reaction cycles. Temperature-programmed desorption results elucidated the structure–activity relationship, revealing that a strong interaction site prevails in Ni 0.4 Cu, while a weaker or moderate interaction site in Ni 0.1 Cu is responsible for the formation of primary amines. Theoretical calculations indicate that the reaction proceeds via an imine mechanism, with benzylideneimine serving as a key intermediate. This work may stimulate further research into the development of bimetallic nano-catalysts for selective nitrile hydrogenation in industrial catalytic processes.
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MOLECULES
·
2024
·Vol. 29
·期 8
·1721
·
IF 4.2
Shoudong Wang,Lei Zhou,Hongyun Qin,Zixu Dong,Haoyuan Li,Bo Liu,Zhilu Wang,Lina Zhang,Qiang Fu,Xia Chen
Hydrofluorocarbons (HFCs) have important applications in different industries; however, they are environmentally unfriendly due to their high global warming potential (GWP). Hence, reclamation of used hydrofluorocarbons via energy-efficient adsorption-based separation will greatly contribute to reducing their impact on the environment. In particular, the separation of azeotropic refrigerants remains challenging, such as typical mixtures of CH2F2(HFC-23) and CHF3(HFC-32), due to a lack of adsorptive mechanisms. Metal–organic frameworks (MOFs) can provide a promising solution for the separation of CHF3–CH2F2mixtures. In this study, the adsorption mechanism of CHF3–CH2F2mixtures in TIFSIX-2-Cu-i was revealed at the microscopic level by combining static pure-component adsorption experiments, molecular simulations, and density-functional theory (DFT) calculations. The adsorption separation selectivity of CH2F2/CHF3in TIFSIX-2-Cu-i is 3.17 at 3 bar under 308 K. The existence of similar TiF62−binding sites for CH2F2or CHF3was revealed in TIFSIX-2-Cu-i. Interactions between the fluorine atom of the framework and the hydrogen atom of the guest molecule were found to be responsible for determining the high adsorption separation selectivity of CH2F2/CHF3. This exploration is important for the design of highly selective adsorbents for the separation of azeotropic refrigerants.
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RARE METALS
·
2025
·
IF 11
Zhang Qi,Zhang Zhiqiang,Zeng Fangyuan,Li Wenjie,Liu Jinhao,Ai Shubo,Zheng Yun,Li Zhe,Shao Huaiyu,Liu Zhi-Quan
Kirkendall voids (KVs) at the Cu/Sn interface are a typical failure in integrated circuits, leading to solder joint cracking and electrical disconnection. Although the formation of KVs has been attributed to the difference in atomic diffusion rates at the Cu/Sn interface, the role of Cu intrinsic "quality" parameters (crystal defects) in this process remains unclear. This work systematically investigated the effects of Cu crystal defects on KVs: Cu substrates with different lattice defects and grain boundaries were prepared using proprietary electrodeposition additives, and the number of defects was quantitatively characterized by micro-strain, geometric dislocation density, and geometric phase analysis. The thermal aging experiments further showed that the formation of intermetallic compounds and KVs was related to crystal defect energy. When the grain boundary energy was higher than the lattice energy, the additional driving force resulted in short-circuit diffusion, causing local Cu depletion and voids. The low-crystal-defect samples maintained the local Cu/Sn interdiffusion equilibrium, resulting in fewer voids after 1000 h. This study emphasizes that regulating the crystal defects can reduce KVs and provides a new insight for improving the integrated solder joint’s reliability.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hanqian Li,Bangzhi Ge,Wenqi Xie,Ruoyan Li,Chao Li,Wanqi Jie,Dongxu Zhang,Yi Qin,Yuan Yu,Chongjian Zhou
Liquid-like thermoelectric materials continuously draw significant attention because of their extraordinary performance. However, liquid-like Cu atoms usually aggregate into clusters, resulting in charge carrier concentration far above the optimized value. Herein, we demonstrate that the dynamic Cu atoms can be homogenized throughout the matrix by a phase-dependent diffusion process. We directly visulized that the typical equilibrium process periodically aggregates Cu atoms into clusters along the grain boundaries, leaving abundant vacancies within the dynamic cation sublattice and thereby causing carrier concentrations that are much higher than the optimal value. We developed a solid-state non-equilibrium quenching process to freeze the homogeneous Cu sublattice in the symmetry cubic phase to ambient environment and removed the unfavorable Cu segregation. This substantially decreases the hole concentration from 1.2 × 1022 cm−3 for the equilibrium sample to 0.8 × 1022 cm-3 for the quenched sample, approaching the calculated optimal value. Notably, the highly uniform Cu sublattice reduces the lattice thermal conductivity to predicted minima of 0.3 W·m−1·K−1 from 300 to 1000 K. The reduced hole concentration and lattice thermal conductivity collectively give rise to a high ZT value of 1.5 at 1000 K, lying in the ballpark of all previously reported stoichiometric copper chalcogenides.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Guangming Wang,Junnan Chen,Ye Qu,Yingjun Dong,Keting Wang,Lihua Qian,Rong Fu,Ying Zhang,Hui-Ming Cheng,Xiaolong Zhang
Electrochemical CO 2 reduction (ECR) to produce chemicals and fuel is a promising technique to build a net-zero carbon circular economy. The performance of ECR has largely advanced in the past decade along with the application of gas diffusion electrodes (GDEs). However, the gas-liquid balance in GDEs is highly fragile due to inefficient CO 2 mass transfer in catalyst layers, which is prone to cause the decay of catalytic performance. In this study, integrated Cu electrodes with controllable mesopores are designed and prepared by copolymer mediated electroless deposition. The optimized Cu electrode shows a selectivity of 81 % (including 65 % for C 2 H 4 ) towards C 2+ products, with a maximum C 2+ partial current density of 232 mA∙cm −2 . Further characterization and simulations reveal that the interconnected mesoporous channels stacked by in-situ reduced Cu nanoparticles leads to an improved CO 2 supply near catalytic sites. In addition, a micro-environment boosting the retention, protonation of *CO intermediates and a unique *CO-CHO coupling step is formed. Our findings provide valuable guidance for enhancing mass transfer and C-C coupling in ECR by creating and controlling intrinsic mesoporous structures in catalyst layers.
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LANGMUIR
·
2025
·
IF 3.9
Jie Chen,Chenyi Zheng,Qiang Wang,Zhipeng Xu,Kui Meng
Many innovations have been made in the morphology and preparation methods of copper–silver core–shell nanomaterials (Cu@AgNMs). The most commonly used method for preparing Cu@AgNMs is to perform a replacement reaction by adding a complexing agent, but there is no universally accepted method to select a complexing agent. This study found that the best complexing agent for preparing Cu@AgNMs is a short-chain complexing agent containing hydrophilic groups through the role of different complexing agents in the synthesis of the material, and the higher the stability of the short-chain hydrophilic complexing agent, the better the integrity of the resulting silver layer. This study clarifies the mechanism of different complexing agents in the synthesis of Cu@AgNSs, provides a reliable reference for the convenient preparation of Cu@AgNMs, and helps us to understand the influence of complexing agents on the silvering effect of the replacement process, thereby promoting the widespread application of a complex-replacement technology.
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