RSC Advances
·
2020
·Vol. 10
·期 35
·20504-20514
·
IF 3.119
Jianwen Wei,Siqi Chen,Yu Li,Zeyu He,Linlin Geng,Lei Liao
To find an alternative adsorbent with high adsorption performance, KIT-6 was prepared by hydrothermal crystallization synthesis using tetraethyl orthosilicate as a silicon source and triblock copolymer P123 as a template. Then the silane coupling agent (3-chloropropyl)trimethoxysilane was first grafted onto KIT-6 mesoporous material and then the polyethyleneimine (PEI) was further grafted through the substitution reaction between amino groups and chlorine atoms. The functionalized KIT-6 was denoted as PEI/KIT-6. The samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), N2 adsorption–desorption, elemental analysis (EA), Fourier transform infrared spectroscopy (FT-IR) and thermal gravimetric analysis (TGA). The Cu2+ adsorption performance was determined by inductively coupled plasma (ICP). The results showed that the average loading of the amino groups was 3.74 mmol g−1, and the modified KIT-6 still has a stable mesoporous structure without pore blockage. With the dosage of 1 g L−1 PEI/KIT-6 and at room temperature, the optimum pH value for adsorption of 100 mg L−1 Cu2+ was 6.0. The adsorption capacity of PEI/KIT-6 for Cu2+ increased with the increase of reaction temperature, and the maximum adsorption capacity of Cu2+ was 36.43 mg g−1. The adsorption capacity tends to reach equilibrium after 120 min, and the optimum adsorption temperature was 35 °C. The pseudo-second-order kinetic model was found to be well suited for the adsorption process of Cu2+. Adsorption equilibrium data could also be described well by the classical Langmuir and Freundlich isotherm models. The adsorption tends to be the chemisorption of a monolayer.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·23817-23827
·
IF 12.732
Manman Feng,Xuemei Wu,Huiyuan Cheng,Zihao Fan,Xiangcun Li,Fujun Cui,Shuai Fan,Yan Dai,Guangping Lei,Gaohong He
The diatomic catalysts (DACs) provide a new strategy for efficient catalysis of CO2 reduction reaction (CO2RR) owing to their maximum atomic utility and more flexible active sites. However, it is still challenging to precisely design heteronuclear diatomic active centers and understand the coordination mechanism of binary sites at the atomic level. Herein, a nitrogen-doped carbon matrix with precisely controlled Fe–Cu diatom sites is synthesized through a metal–organic framework. The as-obtained Fe/Cu–N–C catalyst exhibits an excellent CO faradaic efficiency (>95% over a wide potential range of −0.4 to −1.1 V vs. RHE, 99.2% at −0.8 V vs. RHE), a high turnover frequency (5047 h−1 at −1.1 V vs. RHE), and a low overpotential (50 mV), thus outperforming most reported atomically dispersed catalysts. Further density functional theory calculations indicate that the synergy between Fe–Cu diatoms causes rapid charge transfer and effectively adjusts the position of the d-band center, which reduces the energy barriers for *COOH formation and *CO desorption. This work provides a new approach for advancing universal synthesis strategies to construct heteronuclear diatomic catalysts and explore synergistic effects.
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Nature Communications
·
2025
·
IF 15.7
Ren Yuqi,Cheng Miao,He Hongbin,You Changjun,Duan Lunbo,Sun Zhenkun,Peng Ruoxuan,Zhu Yuan-Hao,Zhang Hongyang,Zhou Jiancheng,Huang Kai,Guan Jie,Li Naixu
CO 2 -to-hydrocarbon fuel conversion via artificial photosynthesis is limited by catalyst poisoning under high O 2 partial pressures and sluggish C 2 -product formation. Herein, Ru 0.6 Cu 1 (Cu 0 –Cu 1+ )/CeO 2 catalysts with adaptive O 2 tolerance are prepared by O 2 -mediated dynamic interfacial reconstruction. Single-atom Ru doping at Ce lattice sites creates a trigonal prismatic coordination configuration, enabling proton-coupled electron transfer and accelerating H 2 O dissociation. Photothermal effect promotes O 2 -driven self-assembly of Cu 0 –Cu 1+ charge-gradient interfaces within Ru/Cu alloy clusters, thereby optimizing the adsorption behavior of * CHOCO intermediates and restructuring the C–C coupling pathway. Interfacial charge cascade transfer and geometric site synergy thermodynamically shift the product selectivity from C 1 to C 2 , as determined by operando spectroscopy and electronic structure analysis. Under concentrated solar irradiation, the catalyst produces 549 ± 20 μmol·g −1 C 2 H 4 with 74.3% selectivity and 0.5% solar-to-chemical energy conversion efficiency—25-fold higher than that in non-concentrated systems. Dynamic interfacial regulation facilitates precise carbon chain synthesis in complex reaction networks.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
·
IF 4.6
Jianlong Gu,Yuchen Liu,Jieyun Cai,Jie Long,Jing Ma,Zilong Zhang,Bing Yang,Hongming Meng,Yaling Yang,Li Gao
In this study, a colorimetric detection system for Cr(III) was established by leveraging the laccase-mimicking activity of two-dimensional Cu-based metal-organic frameworks (Cu-MOFs) modified with polydopamine (PDA) nanomaterials (Cu-MOF@PDA), through which Cr(III) specifically inhibits the catalytic performance. The Cu-MOF@PDA composite exhibited significant laccase-mimicking activity, enabling the oxidation of 2,4-dichlorophenol (2,4-DP) and 4-aminoantipyrine (4-AP), leading to the generation of a red-colored compound. Notably, the laccase-like activity of Cu-MOF@PDA was substantially enhanced under ultrasonic (US) stimulation. Free-radical trapping experiments revealed that the levels of singlet oxygen ( 1 O 2 ) and hydroxyl radicals ( OH) were markedly increased, while the electron transfer rate was accelerated, thereby boosting catalytic efficiency under US exposure. The research confirmed that Cr(III) binds to Cu-MOF@PDA, leading to the suppression of its catalytic activity. A strong linear correlation (R 2 = 0.995) was observed between the absorbance at 505 nm and Cr(III) concentrations ranging from 0.67 to 54.17 μg/L, with a low detection limit (LOD) of 0.26 μg/L (S/N = 3). The developed approach was effectively utilized for the analysis of Cr(III) and total Cr in cigarette tipping paper samples, yielding highly satisfactory results.
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JOURNAL OF NON-CRYSTALLINE SOLIDS
·
2023
·
IF 3.5
Kun Lei,Jinyang Feng,Yuna Sun,Donghua Wu,Xiujian Zhao,Xiao Ma
Doped Cu + glass was prepared by ion exchange method. It was found that the accumulation zone of copper ions would be formed on the glass surface during the process of ion exchange, and there was an extreme point of copper ion distribution concentration about 10 µm inside the glass surface after ion exchange. The exchange depth of copper ions in the sample increased with the increase of ion exchange time. At low ion exchange temperatures, the Cu elements exchanged into the vitreous body exists in the form of Cu + and Cu 2+ . With the exchange of Cu + into the glass, the degree of polymerization of the glasses continued to increase. By raising the ion exchange temperature, a large number of spherical Cu 2 O grains formed on the surface of the sample, continuing to raise the temperature, these spherical grains agglomerated and adhered to form lamellae structure, mainly composed of oxides of Cu 2 O and CuO. The PL spectra showed that the ion-exchanged glass exhibited broadband blue-green emission light with a central wavelength of 468 nm and half-height width of 154 nm under 290 nm excitation. The luminescence intensity appeared to increase firstly and then decrease with increasing the ion exchange time. Dispersed spherical Cu 2 O grains were generated on the surface of the sample exchanged at 410 °C for 16 h. Co-composite luminescence of the spherical Cu 2 O semiconductor and the Cu + doped in the glass effectively increased the luminescence intensity of the samples. In addition, the samples showed a favorable thermal stability of luminescence.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Danqing Shu,Miao Wang,Fengyu Tian,Honglei Zhang,Chuang Peng
Electroreduction of CO 2 to high value-added products such as hydrocarbons provides a promising way to create a carbon neutral circular economy. Copper (Cu) is the most effective metal catalyst with selectivity towards hydrocarbons but Cu catalyst alone generally produces hydrocarbons at low selectivity and yield. Operando surface enhanced infrared absorption spectroscopic (SEIRAS) analysis reveals that the low hydrocarbon yield is attributed to the poor ability of Cu to produce carbon monoxide (CO), which is a crucial intermediate for hydrocarbon formation. In the current study, an Ag-Cu dual-cathode CO 2 RR device is developed, which allows separate control of electrode potential. This dual-cathode cell shows increased hydrocarbon yield (83 % for methane and 106 % for ethylene) and a 200 mV lower onset potential for C 2 H 4 , compared to electrolysis with a single Cu cathode. The CO produced by the Ag cathode transfers to Cu and increase its CO coverage, facilitating methane formation as well as promoting C C coupling to form ethylene. This study also reveals a mismatch of optimum electrode potential between Ag and Cu, which results in compromised performance of the two components in an Ag-Cu bimetallic electrocatalyst, but poses no challenge in the dual-cathode cell. To optimize the performance of the dual-cathode cell, we propose the use of a single-pass dual-gas-diffusion-cathode reactor with enhanced mass transfer for maximum hydrocarbon production. This work verifies that splitting the complex CO 2 RR process into two separate steps is a feasible method to improve the overall efficiency and rate of advanced products while reducing the energy input.
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
L.J. Zhang,J.C. Yuan,L.J. Ma,Z.Y. Tang,X.M. Zhang
Zirconium-based porphyrinic MOFs (PMOFs, MOF = metal-organic framework) have gained considerable attention in the field of electric/thermo/photo-catalysis as heterogeneous single-site catalysts; however, the study on multisite synergistic catalysis of PMOFs are rare. Herein, we have successfully developed a highly regio- and stereo-selective synthetic method of ( E )- β -vinylboronates through hydroboration of alkynes using PCN-222 (Cu, PCN = porous coordination network) as multifunctional heterogeneous catalyst. Compared with homogeneous catalytic system, high TOF value is achieved in the developed method, originating from the synergistic effect of central Cu(II) ions, N atoms of porphyrin rings and terminal –OH groups on Zr-nodes. Notably, density functional theory (DFT) study reveals that five-membered “Cu-N-B-C-C” ring is the key species responsible for the hydroboration process with specific selectivity.
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Journal of Advanced Ceramics
·
2022
·Vol. 11
·期 3
·427-442
·
IF 11.534
Zhang Yu,Han Shuai,Wang Mingyuan,Liu Siwei,Liu Guiwu,Meng Xianfeng,Xu Ziwei,Wang Mingsong,Qiao Guanjun
One-dimensional nanofibers can be transformed into hollow structures with larger specific surface area, which contributes to the enhancement of gas adsorption. We firstly fabricated Cu-doped In 2 O 3 (Cu-In 2 O 3 ) hollow nanofibers by electrospinning and calcination for detecting H 2 S. The experimental results show that the Cu doping concentration besides the operating temperature, gas concentration, and relative humidity can greatly affect the H 2 S sensing performance of the In 2 O 3 -based sensors. In particular, the responses of 6%Cu-In 2 O 3 hollow nanofibers are 350.7 and 4201.5 to 50 and 100 ppm H 2 S at 250 °C, which are over 20 and 140 times higher than those of pristine In 2 O 3 hollow nanofibers, respectively. Moreover, the corresponding sensor exhibits excellent selectivity and good reproducibility towards H 2 S, and the response of 6%Cu-In 2 O 3 is still 1.5 to 1 ppm H 2 S. Finally, the gas sensing mechanism of Cu-In2O3 hollow nanofibers is thoroughly discussed, along with the assistance of first-principles calculations. Both the formation of hollow structure and Cu doping contribute to provide more active sites, and meanwhile a little CuO can form p–n heterojunctions with In 2 O 3 and react with H 2 S, resulting in significant improvement of gas sensing performance. The Cu-In 2 O 3 hollow nanofibers can be tailored for practical application to selectively detect H 2 S at lower concentrations.
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ACS Nano
·
2024
·
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
·
2024
·
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
·
2025
·
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
·
2024
·
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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