MICROPOROUS AND MESOPOROUS MATERIALS
·
2017
·
IF 3.615
Yong Zhang,Huiping Zhang,Ying Yan
A heterogeneous catalyst (Cu/ZSM-5) was prepared by a metal-organic chemical vapor deposition (MOCVD) method under nitrogen atmosphere using Cu(acac) 2 as the copper precursor, and further characterized by XRD , AAS , SEM, BET, H 2 -TPR and XPS as well as catalytic activity performance for the oxidation of toluene. N 2 adsorption data revealed that the samples (CVD-4) prepared by MOCVD with calcination at 500 °C for 4 h possessed higher surface areas than that (CVD-BC) not calcined. The results of XPS demonstrated that CVD-4 exhibited higher redox property and more surface oxygen species compared with CVD-BC and IM (Cu/ZSM-5 catalyst prepared by impregnation). In particular, the CVD-4 catalysts prepared by MOCVD with calcinations showed the highest catalytic activity for toluene oxidation with 90% conversion of toluene at 293 °C with the feed concentration of 1000 ppm and GHSV of 15,000 h −1 , which was lower than IM (310 °C). The results of a reaction durability test revealed that the Cu/ZSM-5 catalysts prepared by MOCVD possessed excellent durability for toluene oxidation for 63 h, while the conversion of toluene fell down from 90% to 60% after 48 h over IM catalyst.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jicheng Wang,Yanhong Quan,Linjie Li,Shunan Yin,Xinxin Ding,Jun Ren
A series of Cu/SBA-15 catalysts with different Cu loadings are prepared by the ammonia evaporation method for the liquid-phase hydrogenation of furfural (FF) to furfuryl alcohol (FA). The results show that the supported Cu loading influences the structure and catalytic activity during FF hydrogenation. The 20Cu/SBA-15 catalyst shows the optimum performance with 99.3 % FF conversion, 99.0 % selectivity to FA, nearly pure FA product, and a turnover frequency reaching up to 81.7h −1 . The effect of Cu loading can be related to Cu dispersion and the interaction between the metal and support, which further promotes the surface Cu + /Cu 0 ratio. Additionally, the correlation of FF conversion with Cu + /Cu 0 ratio confirms that the excellent performance of 20Cu/SBA-15 is mainly derived from the synergy of Cu + and Cu 0 species, although the range of performance is not large. Finally, the optimal reaction conditions are screened using a reaction temperature of 150 °C, a reaction pressure of 4 MPa, a catalyst dosage of 0.1 g, and a reaction time of 60 min. The present study confirms that the Cu loading has a significant effect on the structure of Cu/SBA-15 and nearly pure objective FF product can be feasibly obtained with an appropriate Cu support in the synthesis of FA from FF hydrogenation.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Zhijian Chen,Zhenghui Ma,Guoli Fan,Feng Li
Presently, realizing high ethanol selectivity in CO2 electroreduction remains challenging due to difficult C–C coupling and fierce product competition. In this work, we report an innovative approach for improving the efficiency of Cu-based electrocatalysts in ethanol generation from electrocatalytic CO2 reduction using a crystal plane modification strategy. These novel Cu-based electrocatalysts were fabricated by electrochemically activating three-dimensional (3D) flower-like CuO micro/nanostructures grown in situ on copper foils and modifying with surfactants. It was demonstrated that the fabricated Cu-based electrocatalyst featured a predominantly exposed Cu(100) surface loaded with high-density Cu nanoparticles (NPs). The optimal Cu-based electrocatalyst displayed considerably improved CO2 electroreduction performance, with a Faraday efficiency of 37.9% for ethanol and a maximum Faraday efficiency of 68.0% for C2+ products at −1.4 V vs RHE in an H-cell, accompanied by a high current density of 69.9 mA·cm–2, much better than the particulate Cu-based electrocatalyst. It was unveiled that the Cu(100)-rich surface of nanoscale petals with abundant under-coordinated copper atoms from CuNPs was conducive to the formation and stabilization of key *CH3CHO and *OC2H5 intermediates, thereby promoting ethanol generation. This study highlighted the critical role of CuNP-loaded Cu(100) surface structures on structured Cu-based electrocatalysts in enhancing ethanol production for the CO2 electroreduction process.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Yahui Jiang,Haichuan He,Dan Xia,Hongwei Zhang,Shirui Tan,Li Luo,Yifan Kong,Liu Deng,You-Nian Liu
Cu-based catalysts are widely employed in the electrocatalytic CO2 reduction reaction (CO2RR) toward multi-carbon (C2+) products due to their unique electronic structures. However, Cu-based catalysts are prone to reconstruction under working conditions. Self-reduction and undesirable reconstruction have limited the activity and selectivity of these catalysts. Understanding their reconstruction behavior is crucial for elucidating reaction mechanisms and rationally designing catalysts. In this study, Br-doped Cu-base catalysts were employed to investigate the influence of dopants on catalyst surface reconstruction during CO2RR. Characterizations confirmed that during CO2RR, partial Br− leached from the precursor, while residual bromide ions in the Cu matrix created a bromine-rich environment on the catalyst surface, stabilizing Cu0/Cu+ active sites. The reconstructed catalyst exhibited superior selectivity for C2+ products and higher current density. In situ characterization and theoretical calculations demonstrated that the interaction between Br and Cu atoms suppressed complete Cu reduction. Furthermore, the asymmetric coupling pathway via *CO and *CHO intermediates dominated C2+ product formation, with significantly reduced Gibbs free energy of key intermediates compared to undoped CuO. Notably, halogen doping was validated as a universal strategy—Cu–Cl and Cu–F catalysts similarly enhanced C2+ production while exhibiting analogous reconstruction behavior. This study provided deep insights into catalyst surface reconstruction and offered effective strategies for designing high-performance catalysts for CO2RR.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Weimeng Cai,Haojie Du,Erju Wang,Yuting Qiang,Kunhong Hu,Jianhua Guo
The synthesis of value-added chemicals from renewable biomass is becoming increasingly important in the transition to a sustainable and low-carbon energy system. Herein, we demonstrate a solvent-polarity modulation strategy to engineer biomass-derived Cu-MOF using 2,5-furandicarboxylic acid (FDCA) as a renewable ligand, where tailored β/α ratios via Kamlet-Taft parameters balance nucleation-growth kinetics to optimize textural properties. Pyrolyzed Cu-MOF at 500 °C under a nitrogen atmosphere yield the Cu/C catalysts, which were subsequently employed in the selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). Among the various solvents used, the Cu-MOF precursor synthesized in a mixed solvent of methanol and N, N-dimethylformamide (DMF) demonstrated the highest catalytic performance, outperforming those synthesized in other solvents. This highlights the significant impact of solvent selection on the structure of Cu-MOF, which in turn affects their hydrogenation activity. Advanced characterization confirming that the uniform Cu dispersion (confirmed by HRTEM mapping) and Cu⁰/Cu⁺ electronic synergy (via Cu Auger analysis) enhanced hydrogenation performance. Additionally, the biomass-derived catalysts exhibited excellent durability. Overall, this research provides a promising approach to develop highly efficient catalysts using renewable ligands and demonstrates the potential of regulating catalyst properties through the strategic selection of solvents, as informed by Kamlet-Taft parameters.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Lixiong Xu,Shuo Geng
Electrocatalytic glycerol oxidation reaction (GOR) coupled with hydrogen evolution reaction (HER) is an ideal method to achieve efficient hydrogen production. However, realizing the stable degradation of glycerol to formate at high current densities still faces great challenges, mainly stemming from the competition between GOR and oxygen evolution reaction (OER) at high potentials. To address this issue, in this study, S–Cu–Ni/NF catalysts were successfully synthesized using Cu–Ni/NF catalysts as precursors. The introduction of Cu effectively suppressed the OER, enabling the catalysts to achieve more than 75% formate Faraday efficiency over a wide potential range from 1.3 V vs RHE to 1.6 V vs RHE. Meanwhile, S doping significantly enhanced the electron transport ability of GOR, enabling the S–Cu–Ni/NF catalyst to achieve a high current density of 100 mA cm–2 at a low potential of 1.395 V vs RHE. In addition, after 24 h of continuous operation at a high current density of 100 mA cm–2, the catalyst potential increased by only 40 mV, demonstrating excellent stability. Scanning electron microscopy with energy dispersive spectra (SEM-EDS), X-ray photoelectron spectra (XPS) and in situ Raman characterization confirmed that the precipitation of S promoted the formation of the active site NiOOH and its dynamic growth during the GOR process. The present study not only improved the selectivity of formate at high potentials by inhibiting OER but also significantly enhanced the GOR performance, demonstrated the potential of stable degradation of glycerol at high current densities, and provided a feasible strategy for the industrial application of glycerol oxidation coupled with hydrogenolysis.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Chenglong Bao,Fengyu Wu,Fan Wang,Longyu Qiu,Menggang Li,Depeng Zhao,Yongsheng Yu,Weiwei Yang
The development of efficient heterogeneous catalysts for copper-catalyzed azide-alkyne cycloaddition (CuAAC) is crucial for overcoming the limitations of homogeneous systems, such as poor recyclability and catalyst leaching. In this study, we report the synthesis of nanosized hollow Cu(I)/Cu(II)-metal-organic frameworks (Nano-hollow Cu(I)/Cu(II)-MOF). The paddlewheel Cu(II) sites persist as robust structural nodes, while partial reduction engenders catalytically active planar tetranuclear Cu(I) sites strategically embedded within the framework. This unique architecture endowed Nano-hollow Cu(I)/Cu(II)-MOF with remarkable catalytic activity, achieving a turnover frequency (TOF) of 456.9 h −1 over 10 min for the CuAAC reaction between phenylacetylene and benzyl azide with a TOF 1.66-fold higher than the nanosphere control, underscoring the hollow structure's advantages. Moreover, the catalyst also demonstrated exceptional recyclability, maintaining a nearly constant catalytic conversion rate over 6 cycles. Theoretical calculations unveiled a dual‑copper synergistic mechanism, wherein coordinated charge redistribution mediated by both copper sites significantly lowered the activation barrier. The alkyne dehydrogenation is identified as the rate-determining step with a theoretical overpotential of 0.82 eV, which was pivotal for enhancing reaction efficiency. Beyond conventional catalysis, the Nano-hollow Cu(I)/Cu(II)-MOF exhibited versatile applicability, including rapid fluorescent molecule synthesis with a rate constant (k Flu ) of 0.1 min −1 and efficient DNA-templated ligation reactions with an apparent rate constant (k obs ) of 0.21 s −1 .
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 12
·7521-7530
·
IF 3.945
Qixiao Gai,Shoutian Ren,Xiaochun Zheng,Wenjun Liu,Quanli Dong
Low-cost and high-abundance Cu nanostructures are potential near-infrared (NIR) surface plasmonic resonance (SPR) photosensitizers for carbon nitride (C3N4) photocatalysts, but their low activity and stability need to be improved. In this article, doping S into C3N4 (S-C3N4) creates anchoring sites for photo-deposited Cu nanoparticles (NPs), and the spontaneous construction of S-Cu bonds is realized between S-C3N4 and Cu NPs. The optimal hydrogen evolution rate of 1.64 mmol g−1 h−1 is obtained for S-C3N4–Cu, which is 5.5, 4.6 and 1.7 times that of pure C3N4, S-C3N4 and S-C3N4–Cu, respectively. With further loading of a Pt co-catalyst to confirm the role of Cu NPs and improve the photocatalytic activity of the SCN–Cu, the photocatalytic rate can reach up to 14.34 mmol g−1 h−1. Due to the NIR SPR effect of Cu NPs, the apparent quantum efficiency (AQE) of S-C3N4–Cu at 600 and 765 nm is 2.02% and 0.47%, respectively. The enhanced photocatalytic performance of S-C3N4–Cu compared with C3N4–Cu is mainly due to the introduced S–Cu bonds that improve the injection rate of hot electrons. This solution provides a simple and efficient interface optimization strategy for the construction of efficient NIR-driven photocatalysts.
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JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 9
·3930-3946
·
IF 3.5
Miao Xin,Wang Liying,Shi Yunxin,Chen Guohua,Liu Yunfei,Wu Gaoqi,Cao Zhenzhu,Zhang Yongfeng
Microsphere 3D structure of Cu/Mn 3 O 4 @SC composite was fabricated by pyrolyzing the bimetallic CuMn-MOF, which was composed of Cu 2+ , Mn 2+ and sulfur-containing ligand 2,5-thiophene dicarboxylic acid (H 2 TDC). The composite of Cu/Mn 3 O 4 @SC is used as a high-performance anode material for the lithium-ion batteries cycle exhibiting stable capacities of 715 mAh g −1 after 100 cycles at 200 mA g −1 and outstanding long cycle performance with a reversible capacity of 508 mAh g −1 at 0.5 A g −1 after 500 cycles. The superior performance for the Cu/Mn 3 O 4 @SC anode is mainly attributed to the mutual supporting characteristics of heterojunction synergistic effect, thus avoiding damage in the process of energy storage process. In addition, the kinetic analysis based on CV reveals that the transport kinetics mechanism of the Cu/Mn 3 O 4 @SC is synergistically controlled by the surface capacitive and pseudocapacitive behaviors. The EIS proves that the introduction of Cu enhances the conductivity of the material and the rate of lithium-ion diffusion. Graphical abstract Cu- and S-doped multielement microspheres was fabricated by pyrolyzing CuMn-MOF supported by 2, 5-thiophene dicarboxylic acid.
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ACTA PHYSICO-CHIMICA SINICA
·
2017
·Vol. 33
·期 8
·1672-1680
·
IF 0.767
LIAO Pei-Yi,ZHANG Chen,ZHANG Li-Jun,YANG Yan-Zhang,ZHONG Liang-Shu,GUO Xiao-Ya,WANG Hui,SUN Yu-Han
A series of Cu/Co/Mn/Al catalysts derived from hydrotalcite precursors with different Cu/Co molar ratios (0, 0.1, 0.5, 1.0, and 2.0) were prepared and used for the synthesis of higher alcohols from syngas. N2 physical adsorption desorption, inductively coupled plasma atomic
emission spectrometry (ICP-AES), X-ray diffraction (XRD), scanning electron microscopy (SEM), hydrogen temperature-programmed reduction (H2-TPR), thermogravimetry (TG), and high-resolution transmission electron microscopy (HRTEM) techniques were employed to investigate the physical
and chemical properties of the Cu/Co/Mn/Al catalysts. The results show that the optimum Cu content can increase specific surface area, improve reducibility, and form regular layered structure to provide more uniform distribution of active sites, thereby enhancing catalytic activity and alcohol
selectivity. When the Cu/Co molar ratio was 0.5, the yield of alcohol and the alcohol selectivity reached the maximum values of 0.071 g·g-1·h-1 and 35.9%, respectively.
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International Journal of Minerals Metallurgy and Materials
·
2025
·Vol. 32
·期 12
·3072-3085
·
IF 7.2
Zhang Qian,Liu Bo,An Changcong,Li Qiong,Liu Jiling,Wei Siyu,Fan Jiaxing,Sun Zhe,Zhang Dichuan,Pulatov Bakhtiyor
The effect of heavy metals on the properties and hydration of blast furnace slag–cement composites (BFS-CC) remain unclear. In this study, two BFS-CC (denoted as DBFS-CC and WBFS-CC) were prepared by dry and wet grinding of BFS, respectively. The effect of Cu(II) on BFS-CC’s properties and hydration was investigated by adding representative copper contaminants (CuO, CuCl 2 , and CuS) to the composites. Adding 1.0wt% CuO and 0.5wt% CuS increased the 3-d compressive strength of DBFS-CC by 14.9% and 5.7%, respectively, but suppressed the 3-d strength of WBFS-CC. This trend reversed at 28-d curing, where adding 1.5wt% CuO, 2.0wt% CuCl 2 , and 1.5wt% CuS enhanced the compressive strength of WBFS-CC by 23.4%, 6.2%, and 13.6%, respectively, but adversely affected the strength of DBFS-CC. For 28-d hydration, adding CuCl 2 decreased the hydration degree of DBFS-CC but enhanced that of WBFS-CC. Adding CuO promoted the hydration degree of both composites, while adding CuS exhibited inhibitory effects. DBFS-CC immobilized CuCl 2 better due to a higher hydration degree, while WBFS-CC immobilized CuO and CuS better due to having finer unhydrated BFS particles and a denser matrix. This study not only focuses on the Cu(II) immobilization effect but also reveals the differential effects of Cu(II) species on the hydration process, providing novel insights into heavy metal interactions in BFS-CC systems and their safe disposal.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xiaosen Li,Chun Li,Yifan Fang,Xin Liang,Zhou Fang
Chemical agents present significant threat to international peace, security, and human health due to their potential toxicity. Therefore, developing a sensitive, rapid, and on-site detection method is of great importance. Herein, we developed a highly sensitive and selective glove-based electrochemical sensor based on a metal–organic-framework-modified screen printed electrode (SPE) for chemical agent marker detection. Layered copper benzene-1,3,5-tricarboxylate (Cu-BTC) was successfully constructed to modify screen-printed electrodes (SPE) for detecting electrically inactive ethyl methyl phosphonate (EMPA) and isopropyl methyl phosphonate (IMPA). Additionally, gold nanoparticles (AuNPs) reduced by plasma technology have been applied to create gold nanoparticle-encapsulated copper benzene-1,3,5-tricarboxylate-modified screen-printed electrode (Au@Cu-BTC/SPE) composites for detecting thiodiglycol (TDG). The large surface area and porous structure of Cu-BTC and Au@Cu-BTC enhance the target adsorption and ion diffusion and the efficient use of catalytic materials for rapid electron transfer and zero-distance catalysis. The limit of detection (LOD) was determined to be 4.13 × 10–16 M for EMPA, 7.46 × 10–12 M for IMPA, and 4.05 × 10–12 M for TDG. Following multiple cycles and extended exposure, the sensor demonstrated exceptional repeatability and stability. The response current of Cu-BTC to EMPA and IMPA decreased by 6.75% and 4.86%, and the peak value of Au@Cu-BTC to TDG decreased by 3.3% after 4 weeks, respectively. The peak current showed a good linear relationship with the concentrations of the three target substances, with R2 values all greater than 0.99. The interaction mechanism between the modified electrode and the targets was investigated by density functional theory (DFT) with the generalized gradient approximation of the PBE functional. The results showed that compared with other metal ions, Cu2+ could coordinate tighter with organophosphates. The established MOF-modified SPE integrated with a protective glove sensor was applied for the detection of real-world samples and demonstrated a broad spectrum of practical applications.
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