Scientific Reports
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2025
·Vol. 15
·期 1
·1-11
·
IF 3.9
Wahid Ehtisham,Ocheja Ohiemi Benjamin,Oguntomi Sunday Olakunle,Pan Run,Grattieri Matteo,Guaragnella Nicoletta,Guaragnella Cataldo,Marsili Enrico
Electrodes functionalised with weak electroactive microorganisms offer a viable alternative to conventional chemical sensors for detecting priority pollutants in bioremediation processes. Biofilm-based biosensors have been proposed for this purpose. However, biofilm formation and maturation require 24–48 h, and the microstructure and coverage of the electrode surface cannot be controlled, leading to poorly reproducible signal and sensitivity. Alternatively, semiconductive biocompatible coatings can be used for viable cell immobilization, achieving reproducible coverage and resulting in a stable biosensor response. In this work, we use a polydopamine (PDA)-based coating to immobilize Saccharomyces cerevisiae yeast viable cells on carbon screen printed electrodes (SPE) for Cu(II) detection, with potassium ferricyanide (K 3 [Fe (CN) 6 ]) as a redox mediator. Under these conditions, the current output correlates with Cu (II) concentration, reaching a limit of detection of 2.2 µM, as calculated from the chronoamperometric response. The bioelectrochemical results are supported by standard viability assays, microscopy, and electrochemical impedance spectroscopy. The PDA coatings can be functionalised with different mutant strains, thus expanding the toolbox for biosensor design in bioremediation.
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ACS Materials Letters
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2024
·
IF 9.6
Cun Chen,Honggang Huang,Yao Chen,Zhe Zhang,Hui Fu,Hanjun Li,Wei-Hsiang Huang,Feili Lai,Nan Zhang,Tianxi Liu
Interface engineering has been widely explored due to its potential for regulating the intermediate adsorption, controlling mass/electron transfer, and preventing severe aggregation of catalysts. Hence, we have synthesized a series of Cu–In metallic aerogels (MAs) with a controlled ratio of Cu/Cu2In interfaces as efficient catalysts for electrochemical carbon dioxide reduction reaction (CO2RR). As a result, Cu–In MAs with the highest Cu/Cu2In interfaces abundance (Cu2In MAs) achieve the high Faradaic efficiency of CO up to 94.5% at −0.6 V vs reversible hydrogen electrode (RHE), outperforming Cu1In MAs, Cu3In MAs, Cu4In MAs, and Cu MAs. Furthermore, Cu2In MAs with the highest Cu/Cu2In interface abundance also exhibit excellent stability after continuous electrolysis for 10 h. Mechanism research indicates that the rich Cu/Cu2In interfaces in Cu2In MAs allow for moderate adsorption of CO2 and accelerate electronic transmission, which greatly reduce the energy barrier of the potential-limiting step, thus improving the CO2RR performance. This study indicates that interface engineering plays an important role in improving the CO2RR performance, providing a new strategy for preparing efficient CO2RR catalysts.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Liang Zhu,Yang Liu,Yanhui Gao,Ningxujin Ding,Danyu Wang,Liuliu Long,Beibei Wang,Junyu Lang,Evgeny I. Vovk,Yong Yang
The hydrogen dissociation and spillover mechanism on oxide-supported Cu catalysts play a pivotal role in the hydrogenation of carbon dioxide to methanol. This study investigates the hydrogen spillover mechanism on Cu/CeO2 catalysts using in situ spectral characterization under high-pressure reaction conditions and density functional theory (DFT) simulations. The research confirms that the Cu sites serve as the initial dissociation points for the hydrogen molecules. The chemically adsorbed hydrogen (H*) then spills over onto the CeO2 support and interacts with the lattice oxygen to form special hydroxyl groups, while simultaneously reducing the surrounding Ce4+ to form Ce3+. Interestingly, the temperature-programmed desorption (TPD) results found that heating the hydroxyl-containing surface mainly reverses H2 dissociation by desorbing H2 instead of forming H2O, while no significant vacancy formation was detected. The DFT calculation identified a subsurface pathway favoring hydrogen migration, which explained the dominating H2 in the TPD products. A chemical loop study after CO2/H2 cofeeding on the catalyst reveals that hydrogen spillover facilitates the highly reduced surface serving as the active centers, enabling a secondary methanol synthesis in a vacuum. This study provides a model of the formation and desorption pathways of hydrogen species on Cu/CeO2 catalysts and illustrates the key role of the hydrogen spillover mechanism in promoting the CO2 hydrogenation to methanol reaction through important experimental analysis.
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ACS Catalysis
·
2024
·
IF 11.3
Xiaofeng Liu,Yuanyuan Sun,Hao Ren,Yan Lin,Mingbo Wu,Zhongtao Li
Electrochemically driven carbon–carbon coupling utilizing renewable electricity under ambient conditions has emerged as an innovative approach for synthesizing high-value chemicals, which still faces inherent challenges such as low conversion rates and poor selectivity. While electroreducing furfural to hydrofuroin can produce high-quality biofuel, its efficiency need to be promoted. Herein, Cu–Sn bimetallic catalyst has been developed with a conversion rate of furfural of >97% and hydrofuroin selectivity of >67% through equilibrium of the interfacial intermediate *H and *fur-CHOH, which exhibits the greatest state-of-the-art overall performance. Characterization and theoretical calculation reveal that Cu serves as the active site for generating *fur-CHOH, whose electron density can be decreased by introducing Sn, and results in a higher *fur-CHOH coverage and a lower energy barrier of dimerization. Moreover, adding Sn also enables sluggish *H formation to balance interfacial *fur-CHOH and *H, leading to reduced hydrogenation byproducts. The as-developed approach provides valuable insights for optimizing other C–C electrocoupling reactions for the synthesis of high-value chemicals.
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ENERGY & FUELS
·
2025
·
IF 5.3
Xiaoteng Cui,Mingsheng Luo,Zhi Yang,Roshni Rahman,Ziyuan Li,Wenshuai Yang,Lingman Xia
As a greenhouse gas, carbon dioxide is also a rich carbon resource that can be effectively utilized to tackle the global warming crisis. This paper presents an in-depth investigation of the impact of the Cu content on the structure of Cu–Zn–Al layered double hydroxides (LDHs) from a novel perspective. The CO2 hydrogenation performance of the derived catalyst, the LDO, is also evaluated in the methanol synthesis reaction. All catalysts were evaluated at 3.0 MPa, a carbon dioxide to hydrogen ratio of 3, and a space velocity of 3600 mL·g–1·h–1. The results from this work indicate that the catalyst with a Cu:Zn ratio of 11:4 exhibited the highest methanol selectivity of 63.9% at 230 °C. At 250 °C, the catalysts also yielded the highest methanol selectivity of 50% only, along with a CO2 conversion as high as 17.8%. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) data suggest that the CO2-to-methanol reaction follows the formate (HCOO*) mechanism for this catalyst. Results from this work offer a novel approach to designing Cu-LDH-based catalysts, which offers valuable insights for the efficient chemical utilization of CO2.
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SOLAR ENERGY MATERIALS AND SOLAR CELLS
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2024
·
IF 6.3
Maoqing Tang,Cong Qi,Linfei Yue
As an environmentally friendly seawater desalination method, solar interface evaporation is considered to be a promising solution to ease the freshwater shortage. In this paper, porous Cu-Fe 3 O 4 /sodium alginate/polyacrylamide hydrogel was prepared by double chemical crosslinking method using sodium alginate, polyacrylamide and Cu-Fe 3 O 4 nanoparticles with good SPR effect as raw materials. The effects of Cu-Fe 3 O 4 nanoparticle concentration, light intensity and salt water concentration on the evaporation performance of hydrogel evaporator were studied. It was found that under the light intensity of 1 sun, the evaporation efficiency and thermal efficiency of 3.5 wt% seawater in the hydrogel evaporator containing Cu-Fe 3 O 4 nanoparticles with a concentration of 0.26 % can reach 64.7 % and 95.24 %, respectively. In addition, the Cu-Fe 3 O 4 /sodium alginate/polyacrylamide hydrogel evaporator has good reusability and salt self-cleaning ability. The seawater desalination experiment in real environment shows that the hydrogel evaporator with low cost benefit has broad application prospects in the field of seawater desalination.
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INORGANIC CHEMISTRY COMMUNICATIONS
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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
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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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