ACS Sustainable Chemistry & Engineering
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2018
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IF 6.14
Junhui Liu,Anfeng Zhang,Xiao Jiang,Min Liu,Yanwei Sun,Chunshan Song,Xinwen Guo
Conversion of CO2 to sustainable chemical feedstocks and fuels by reacting with renewable hydrogen is considered to be a promising direction in energy research. The selectivity of desired products, such as C2–C4= and C5+, is low over unpromoted iron-based catalysts for CO2 hydrogenation. Therefore, promoters are often used to tailor and optimize the product distribution. In this work, the effect of doping Cu into Fe-based supported catalysts on the catalytic performance for CO2 hydrogenation to hydrocarbons was studied with a particularly focus on the interaction between Fe and Cu. For this purpose, catalysts with different Fe and Cu distribution were prepared by various impregnation methods. It was found that the selectivity of C2–C4= over Cu-promoted catalysts decreased, but a significant improvement was obtained for C5+. This promoting behavior is different from that of other promoters (e.g., K, Mn, Zn, etc.). The secondary conversion of produced olefins on Cu-promoted catalysts, which results from the improvement of olefins adsorption, on Cu-promoted catalysts leads to the decrease of C2–C4= (hydrogenation) but the increase of C5+ (oligomerization). Characterization results demonstrate that the catalytic performance is evidently associated with the strength of the interaction between Fe and Cu in the supported catalysts.
研究领域:
催化化学
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能源研究
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化学工程
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可持续化学
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2023
·Vol. 107
·期 4
·2593-2608
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IF 3.9
Fei Chen,Binhua Xiang,Mingyong Jia,Yueqi Wu,Zhifeng Huang,Qiang Shen
In the electronic industry, the composite of copper (Cu) and aluminum nitride (AlN) is widely used, but obtaining Cu/AlN/Cu functionally gradient materials (Cu/AlN/Cu FGMs) in a single step using traditional laminated sintering processes has proven challenging due to significant differences in their physical properties. To address this issue, molybdenum (Mo), with a high melting point and low expansion, was involved in creating a continuous gradient structure with AlN and a quasi-continuous interfacial structure with Cu. The continuous interfacial structure of Mo/AlN gradient materials was obtained by hot pressing at 1650°C. Subsequently, the quasi-continuous interfacial structure of Cu/Mo heterogeneous metal joints with high shear strength was achieved by utilizing the diffusion welding method at 700–950°C. The results indicated that the optimum shear strength of Cu/AlN/Cu FGMs is around 90 MPa. However, Cu/AlN/Cu FGMs with different diffusion interlayers failed in different ways when shear occurred, which greatly depends on the phase compositions at the joint. The challenges are overcome by utilizing Mo to construct the continuous and quasi-continuous interfaces, resulting in Cu/AlN/Cu FGMs with improved shear properties.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Meihua Zhao,Zhuo Li,Fangyuan Si,Ruiqi Fang,Yingwei Li
Catalysts with both metal single atoms and nanoclusters have drawn great attention due to their distinctive catalytic activity and selectivity. Herein, Cu single atoms and Cu nanoclusters are homogeneously dispersed on a porous N-doped carbon framework (Cu 1 Cu n @CN) via an encapsulation pyrolysis strategy. In the selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF), around 100% yield of DFF is achieved over the as-synthesized Cu 1 Cu n @CN under air atmosphere and mild reaction conditions. Density function theory studies demonstrate that the strong interaction between the CuN and Cu cluster sites contributes to the up-shift of the d-orbital center of Cu in Cu 1 Cu n @CN and the Cu clusters can induce obvious electron redistribution around the CuN active center, which significantly improves the capability in substrate adsorption and activation. This work might provide new insights into the design and construction of catalysts with both metal single atoms and nanoclusters and investigations on their synergistic interactions for advanced catalysis applications.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Miaomiao Zhao,Zezhou Zhang,Liying Wang,Xuan Xu,You Li,Ao Liu,Degang Ma,Chunfeng Song
Stable, treatment-resistant Cu complexes in practical wastewater are frequently neglected. Positively charged lysozyme amyloid fibrils (AF), however, exhibit unexplored potential for their adsorption. This study engineered an amyloid fibril-chitosan composite (AF-CS) xerogel and evaluated its adsorption performance in three systems: free Cu 2+ , Cu-Citrate binary, and Cu-EDTA binary. The characterization confirmed successful synthesis of AF-CS, revealing a porous and amine-rich structure with a more positive surface charge than that of pure AF xerogel. Systematic evaluation demonstrated adsorption capacities of 65.37 mg/g (free Cu 2+ ), 166.14 mg/g (Cu-Citrate), and 40.31 mg/g (Cu-EDTA). MINTEQ 3.0 speciation analysis identified anionic Cu-ligand complexes as dominant species in binary systems. Further investigation revealed synergistic adsorption mechanisms in the Cu-Citrate system: electrostatic attraction coupled with decomplexation-complexation pathways liberated citrate ligands, enabling electrostatic shielding and adsorption bridging that enhanced Cu coordination. Conversely, the high stability of Cu-EDTA chelates limited adsorption primarily to mechanisms involving electrostatic attraction, resulting in suboptimal performance. These findings advance the theoretical understanding of AF-CS interactions with diverse Cu species, demonstrating AF-CS as a promising material for Cu recovery from complex wastewater and providing guidance for designing novel remediation materials.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Xinyu Ren,Lu Wang,Zhipeng Xie,Congshu Huang,Jingjing Wang,Shihao Zhang,Bin Liu
Modulating the release of Cu(I) ions from copper-based antifoulants is of notable engineering and scientific importance. However, this approach remains challenging because of a lack of valence-stabilizing protection strategies for Cu(I) sites and the poorly characterized releasing behavior of Cu(I) ions. To address these issues, a novel multivalent antifoulant Cu(I, II)-metal–organic framework (Cu(I, II)-BTC; BTC: 1,3,5-benzenetricarboxylate) was synthesized via an in situ reduction of Cu(II)-BTC under mild conditions. The framework structure of Cu(I, II)-BTC was examined in detail using X-ray diffraction, N 2 sorption analysis, and transmission electron microscopy–selected-area electron diffraction. For the first time, the release behavior of Cu(I) from Cu(I, II)-BTC submerged in seawater was characterized by ultraviolet–visible spectrophotometry. The chemical state of the copper sites in the Cu(I, II)-BTC complex was determined before and after submersion in fresh seawater to investigate whether the framework structure facilitated the retention of Cu(I) ions. Further, the bactericidal activity of Cu(I, II)-BTC was evaluated by measuring the intracellular reactive oxygen species levels to reveal the biocidal effect of the released Cu(I) ions. Finally, the antifouling performance of the resulting Cu(I, II)-BTC-based antifouling coating was comprehensively evaluated via laboratory bioassays (using fouling bacteria and barnacle larvae as test organisms) and long-term marine field trials. This study offers viable avenues for designing novel antifoulants and developing an in-depth understanding of the copper-mediated antifouling process.
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ACS Catalysis
·
2024
·
IF 11.3
Mei-Yao Wu,Shan-Qing Li,Wei-Wei Wang,Chun-Jiang Jia
The structures of active components in practical solid catalysts are seldom homogeneous, which makes it challenging to explore the synergistic effect among the complex catalyst components in heterogeneous catalysis. The active structure of Cu-based catalysts, which are widely used in water gas shift reactions and other important industrial reactions, has been debated. This work prepared Cu–MgO catalysts with the copresence of Cu particles and Cu atoms to investigate the synergistic effects of these Cu species. We found that the Cu nanoparticles served to adsorb and activate the reactant molecule of CO, while the atomic Cu species at the surface of the MgO lattice might exist as the Mg2Cu2–Ov site for water dissociation. The presence of surface-substituted Cu atoms modulated the reactivity of adjacent oxygen vacancy in the MgO surface, enhanced the ability of H2O dissociation to form reactive –OH species, and allowed the oxygen vacancies to recycle, contributing to the continuation of the reaction. A volcano-type relation of catalytic performance versus Cu0/Cu2+ ratio has been established, revealing the existence of synergy between Cu particles and Cu atoms. In addition, due to this synergistic effect, the optimized Cu–MgO catalyst shows a very high activity with a CO conversion rate of 1119 μmolCO gCu–1 s–1 at 300 °C. This work revealed the synergistic effect of different Cu species in the Cu–MgO catalysts, which was important for unraveling the contribution of complex components to catalytic performance.
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Catalysis Science & Technology
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2025
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IF 4.2
Xijun Li,Runze Xue,Yuan Liu,Cuijuan Zhang
Development of highly active and stable catalysts is critical for the hydrogenation of CO2 to methanol. Herein, a Cu-based catalyst was demonstrated by impregnating 20%ZnO onto the Cu–Al spinel followed by reduction. The catalyst delivers a methanol yield of 0.218 g g−1 h−1 with a CO2 conversion of 9.2% at 220 °C, 3 MPa, 6000 mL g−1 h−1, and is stable over a 300 h test. Various characterization techniques reveal that ZnO inhibits the growth of Cu nanoparticles during exsolution. Furthermore, there is strong electronic interaction between the components, i.e., the electron migrates from ZnO to the Cu–Al spinel, which leads to more oxygen vacancies and an electron-rich support and thus beneficial for CO2 hydrogenation to methanol.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10075
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IF 15.7
Jin Hao,Zhu Xuanqi,Zhang Mengsi,Zheng Hao,Chen Yang,Yao Dong,Liu Shuwei,Zhang Hao
Superoxide dismutase (SOD), featured with unique metal catalytic sites, is the first defense against reactive oxygen species (ROS) damage in vivo and well used in the treatment of oxidative stress-related diseases. However, the catalytic activity of natural SOD is limited by the metal ion coordination with rigid amino-acid residues. Inspired by the Cu 2+ /histidine residue coordination in Cu-Zn-SOD, in this work, the Gibbs free energy change of the break/reform of coordination bonds in the tetracoordinated structure formed by Cu 2+ and different groups in histidine is calculated, which reveals that in comparison to the Cu catalytic site coordinated with four imidazolyls, the coordination with one amino, one carboxyl and two imidazolyls possesses the lowest overall energy as well as the lowest breaking energy of one of the coordination bonds. Thus, catalytic site stability and catalytic reaction activity can be balanced sufficiently. Accordingly, the as-prepared Cu/Zn/histidine (CuZnHis) supramolecular assemblies with optimized Cu catalytic site present a significantly enhanced SOD activity up to 37900 Unit/mg, which is at least 5.4 times higher than that of natural Cu-Zn-SOD. As a proof of concept in treating oxidative stress-related diseases, the CuZnHis assemblies promote macrophage polarization from M1 to M2 phenotype and the expression of anti-inflammatory factors, and inhibit the periodontitis in male animal models.
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FOOD CHEMISTRY
·
2023
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IF 8.8
Ya Zhang,Ying Xu,Ning Li,Xiaofang Liu,Yi Ma,SiyiYang,Huibo Luo,Changjun Hou,Danqun Huo
Here, we constructed a novel ultra-sensitive electrochemical sensor based on ZIF-67@antimonene (AMNFs) nanocomposites which are based on the first-principles density functional theory the adsorption properties of antimonene on heavy metal ions were studied for simultaneous determination of Cu 2+ , Pb 2+ and Hg 2+ . The ZIF-67@AMNFs was prepared by using ZIF-67 MOF surface loaded with a large amount of antimonene sheet. Its morphology and crystal structure were characterized by Transmission electron microscope (TEM), Energy Dispersive Spectroscopy (EDS), X-ray diffractometry (XRD) and X-ray photoelectron spectroscopy (XPS). Functional ZIF-67@AMNFs due to its unique layered structure, large active surface area, strong adsorption capacity and good electrical conductivity. In addition, the adsorption capacity of the sensor electrode for Cu 2+ , Pb 2+ and Hg 2+ was effectively enhanced. The detection limits of Cu 2+ , Pb 2+ and Hg 2+ were 0.01 pM, 0.042 pM and 0.031 pM, respectively. The determination mechanism of Cu 2+ , Pb 2+ and Hg 2+ was further clarified based on the adsorption properties and electrochemical accumulation of antimonene on metal atoms. It has been successfully applied to the simultaneous determination of Cu 2+ , Pb 2+ and Hg 2+ in rice, sorghum, corn, milk, honey and tea samples, and has good practicability.
研究领域:
食品科学
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材料科学
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分析化学
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Journal of Materials Chemistry C
·
2021
·Vol. 9
·期 27
·8537-8544
·
IF 7.393
Zhongyuan Guan,Haihang Ye,Peiwen Lv,Lijin Wang,Jing Zhang,Bin Zou,Aiwei Tang
Multinary Cu-based chalcogenide nanocrystals (NCs) are excellent candidates for optoelectronic applications, but their growth mechanism and its impacts on the NCs’ optical properties remain controversial. Herein, we employed a simple colloidal chemistry method for the growth of multinary Cu-based NCs including ternary Cu–In–S NCs, quaternary Cu–In–Se–S NCs, and five-component Cu–In–Zn–Se–S NCs, to explore their growth mechanism and investigate their optical properties. It is found that the ternary Cu–In–S NCs contain a large number of copper vacancies, which affect the major acceptor level for the exciton recombination. With the high reaction activity of Se, the quaternary Cu–In–Se–S NCs form at low reaction temperature and have a red-shift of the photoluminescence (PL) maximum due to the recombination from the conduction band to the acceptor level. The formation process of five-component Cu–In–Zn–Se–S NCs highly depends on the Zn amount, which shows a competitive relationship between the NCs’ growth and diffusion of Zn, leading to the red- and blue-shift of PL maximum, respectively. Our study provides a clear map for the growth of multinary Cu-based NCs and shows their impacts on optical properties.
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Catalysts
·
2024
·Vol. 14
·期 8
·496
·
IF 3.8
Kaige Zhao,Xinhao Xu,Manli Wang,Tao Chen,Qianlin Ju,Lulu Hao,Zelin Chen,Xiaolong Yu,Changjiu Li
The electrocatalytic oxidation of urea combined with wastewater splitting is considered a promising approach for sustainable hydrogen production, characterized by minimal energy consumption. However, its evolution is greatly hindered by the shortage of efficient and easily accessible electrocatalytic materials. Here, a facile electrochemical activation strategy was conceived and proposed to construct a Cu-doped NiOOH nanolayer encapsulated on Cu2O nanodendrites on Cu mesh substrate (Cu-NiOOH/Cu2O/CM) from the electrodeposited Ni/Cu2O/CM heterostructured precatalyst. It was verified that the incorporation of Cu not only facilitates the rapid formation of Ni(III)species but also contributes to the formation of Cu-Ni(III)bifunctional electrocatalytic active sites. Benefiting from the accessible Cu-Ni(III)dual active sites, high active surface area, good hydrophilic and aerophobic surface properties and superior electrical conductivity of the Cu mesh substrate, the as-prepared Cu-NiOOH/Cu2O/CM exhibits enhanced bifunctional electrocatalytic abilities for electrocatalytic urea oxidation reaction (UOR) and hydrogen evolution reaction (HER). Particularly, for the Cu-NiOOH/Cu2O/CM||Cu-NiOOH/Cu2O/CM configuration toward the UOR||HER coupled system, a significantly reduced cell voltage of 1.43 V vs. RHE @ 10 mA·cm−2was obtained. The observed cell voltage for the conventional overall water splitting is approximately 190 mV higher than that observed for overall urea splitting. This study proposes a viable approach to achieve and optimize the bifunctional UOR/HER performance of NiOOH active species, which holds significant importance for efficient and stable hydrogen generation from urea-contaminated substandard water.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Zichen Song,Wenqian Wang,Jiantao Fu,Xiangbo Ma,Xiaolei Wang,Guiling Wang,Zhiyu Ren,Honggang Fu
Ligand-directed inheritance creates asymmetric Cu–N/Cu–O motifs for CO 2 reduction. • Symmetry-breaking preserves highly active Cu δ+ interfaces under dynamic conditions. • Dual-mode *CO adsorption (atop/bridge) effectively bypasses C 2+ scaling laws. • Optimized sites lower C–C coupling barriers while poisoning hydrogen evolution. • Achieved 82.2% C 2+ FE at 0.9 A cm −2 with stable 50 h ampere-scale electrolysis. The electrochemical CO 2 reduction reaction (ECR) to multi-carbon (C 2+ ) chemicals is intrinsically hindered by the rigid scaling relations and geometric homogeneity of pristine copper surfaces, which enforce a singular atop-type *CO intermediate. Herein, we implement a ligand-directed motif inheritance strategy to synthesize nitrogen-doped CuO (N-CuO) nanoparticles, uniquely characterized by asymmetric Cu–N/Cu–O lattice motifs. Under severe cathodic polarization, these robust Cu–N bonds structurally modulate the metallic reconstruction, preserving local non-metal coordination to sustain a highly active, mixed-valence Cu δ+ species. Operando spectroscopic and theoretical analyses reveal that this local structural asymmetry disrupts adsorption homogeneity, explicitly driving the spatial co-adsorption of bridge- and atop-type *CO intermediates. This dual-mode configuration bypasses conventional kinetic bottlenecks to drastically accelerate C–C dimerization. Consequently, the N-CuO catalyst delivers a record-level C 2+ Faradaic efficiency of 82.2% at an industrially relevant current density of 0.9 A cm −2 , exhibiting exceptional structural and catalytic stability over 50 h of continuous flow-cell operation. This work establishes atomic-scale lattice asymmetry as a decisive design principle for stabilizing active Cu δ+ species and steering multi-carbon electrosynthesis at practical reaction rates. Download: Download high-res image (301KB) Download: Download full-size image A ligand-directed motif inheritance strategy is developed to precisely integrate asymmetric Cu–N/Cu–O motifs within the CuO lattice. This local structural asymmetry enforces the *CO atop /*CO bridge dual-mode co-adsorption, bypassing conventional scaling relations to lower the C–C coupling barrier while suppressing HER. The catalyst delivers a state-of-the-art C 2+ Faradaic efficiency of 82.2% at an industrially relevant 0.9 A cm −2 .
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