JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Xiaofeng Wang,Zuyi Zhang,Ziyi Yan,Qingbo Li,Chengcheng Zhang,Xinhua Liang
The efficient hydrodeoxygenation (HDO) of biomass derivatives to yield specific products is a significant yet challenging task. In the present study, a Cu/CoO x catalyst was synthesized using a facile co-precipitation method, and subsequently used for the HDO of biomass derivatives. Under optimal reaction conditions, the conversion of 5-hydroxymethylfurfural reached 100% with a selectivity of ∼99% to 2,5-diformylfuran. In combination with the experimental results, systematic characterizations revealed that CoO x , as the acid site, tended to adsorb C O bonds, and the metal sites of Cu + were inclined to adsorb C O bonds and enhance C O bond hydrogenation. Meanwhile, Cu 0 was the main active site for 2-propanol dehydrogenation . The excellent catalytic performance could be attributed to the synergistic effects of Cu and CoO x . Further, by optimizing the ratio of Cu to CoO x , the Cu/CoO x catalysts exhibited notable performance in HDO of acetophenone, levulinic acid, and furfural, which verified the universality of the catalysts in the HDO of biomass derivatives.
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ANALYTICAL CHEMISTRY
·
2023
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IF 7.4
Yue Mou,Peng Yin,Meiyun Chen,Chonghui Wei,Yanfei Zhang,Jiaheng Zhang,Yujie Zhao,Xingyu Luo,Yilin Wang
Copper ions play vital roles in regulating life processes and being closely involved in several diseases such as cancer. Although detection methods based on fluorescent sensors or other strategies have been developed, it still remains a challenge to simultaneously realize the convenience, specificity, and accuracy in intracellular copper ion analysis. Herein, we propose an aptamer-functionalized DNA fluorescent sensor (AFDS) for accurate and specific detection of Cu(II) both in vitro and in cells by engineering the linkage of two DNA aptamers, namely, Lettuce aptamer and AS1411 aptamer, to achieve the manner of recognition response. Taking advantage of the functions of each aptamer, the tumor cell recognition capability and the high-contrast detection performance are simultaneously equipped in the AFDS. Furthermore, the AFDS shows high specificity and selectivity in Cu(II) response to avoid interference from common metal ions, chelators, and reactants by being associated with the irreversible interaction between nucleobases and Cu(II), which can destroy the topological structures and switch off the fluorescence of the AFDS. It also enables a sensitive in vitro detection of Cu(II) with a detection limit as lower as 0.1 μM and a wide detection linear range from 0.1 to 300 μM. The feasibility and superiority of the AFDS provide an opportunity to reveal both concentration-dependent and time-dependent intracellular Cu(II) responses in living cells. Therefore, the AFDS has achieved the novel detection performance of Cu(II) to exhibit great potential in exploring copper-related biological and pathological research.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 18
·12754-12766
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IF 3.3
Qixiao Gai,Shoutian Ren,Xiaochun Zheng,Wenjun Liu
Cu nanoparticles (NPs) are low-cost surface plasmonic resonance (SPR) metal nanostructures, and their SPR properties can be used to enhance the photocatalytic hydrogen evolution performance of carbon nitride (C3N4). But their actual performance is usually limited, and one key factor is their poor interfacial quality. In this work, a highly conductive reduced graphene oxide (RGO) interlayer is introduced between protonated C3N4 (PCN) nanosheets and Cu NPs, which can act as an efficient sink for photogenerated electrons from C3N4 and hot electrons from Cu NPs, and simultaneously serve as reaction sites for the hydrogen evolution reaction, and accelerate the charge transport by the formed C–O–C and C–O–Cu bonds. The optimal hydrogen evolution rate of the optimized PCN/RGO/Cu is 1.30 mmol g−1 h−1, which is 6.76, 2.47 and 2.41 times that of PCN, PCN/RGO and PCN/Cu, respectively, and it can further reach up to 13.22 mmol g−1 h−1 by loading moderate Pt NPs. Meanwhile, the introduced RGO can effectively anchor Cu NPs to enhance the stability of the photocatalyst. In addition, due to the broad SPR response of Cu NPs, a near-infrared photocatalytic performance is realized for PCN/RGO/Cu with an apparent quantum efficiency of 0.46% at 765 nm.
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MICROCHEMICAL JOURNAL
·
2023
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IF 4.8
Yuting Hao,Hao Zhang,Xizhuang Yue,Zhen Zhao,Shuang Zhao
Herein, a novel, simple prepared and robust electrochemical sensor based on the copper-containing metal organic framework (CuBTC) has been developed for the determination of metformin (MET), a first-line drug for type 2 diabetes mellitus. CuBTC was synthesized by hydrothermal method. The morphology and structure of CuBTC were characterized by scanning electron microscopy, X-ray powder diffraction and infrared spectroscopy. The electrochemical behavior of MET at the glassy carbon electrode modified with CuBTC/Nafion mixture was deeply explored by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The electrochemical studies showed that CuBTC had excellent electrocatalytic ability towards the redox reaction of MET. Under the optimal conditions, the linear range of MET on the modified electrode was 0.5–280 μmol/L, and the detection limit was 0.19 μmol/L. Additionally, the proposed sensor exhibited good long-time stability, reproducibility and selectivity, which was successfully applied to detect MET in tablets, serum and urine samples.
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CARBON
·
2023
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IF 10.9
Yonghui Zhao,Xiaoli Yang,Xiang Meng,Rui Hu,Xiaoliu Duan,Zhengya Gan,Jianjun Ding,Yi Gong,Xingyou Tian
Encapsulation of Cu nanoparticles by carbon chain mail is a promising approach to extend the service endurance. However, the diffusion of oxygen across the surfaces and interfaces of Cu nanoparticles (NPs) may induce obvious changes to their surface compositions, thereby dramatically altering catalytic properties . Here we reported an unanticipated boosting catalytic activity of graphitic chain mail-encapsulated Cu nanocatalysts (1.3- to 6.8-fold enhancement from initial 1.6–13.4 s −1 g −1 to stable 6.6–21.5 s −1 g −1 ) for the reduction of 4-nitrophenol by simply immersing these NPs in water for 10 days without any further treatment. The graphitic shells were arc-converted from sixteen types of biomass residuals and polymeric wastes. The rising catalytic activity was attributed to the temporal formation of Cu 2 O at the interface of Cu core and graphite shell, which was derived from the diffusion of dissolved oxygen across the defective graphitic chain mail. The increment of catalytic activity was linearly related with the rising content of Cu 2 O. The monotonous relations of initial and enhanced activities with shell thickness and interfacial composition of NPs were also well established. This work provides a new insight into the interfacial manipulation of core/shell nanocatalysts, and paves a versatile path for the high value-added utilization of carbon wastes.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 26
·12117-12122
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IF 3.3
Chaoqun Huang,Yinan Li,Fan Cai,Hongbin Zhong,Fengling Zhang,Weimin Zhong,Lin Yao,Jiyi Huang
This research put forward an electrochemical immunoassay based on an atomically Cu dispersed nitrogen-doped carbon (Cu-CN) modified disposable screen-printed carbon electrode (Cu-CN/SPCE) for sensitive screening of carcinoembryonic antigen (CEA) with a split-type strategy. Atomic-level Cu–CN can be obtained after pyrolysis of a metal–organic skeleton encapsulated with copper acetylacetone, which can realize significant electrochemical signal amplification of ascorbic acid. Using alkaline phosphatase (ALP) catalytic chemistry to in situ generate ascorbic acid from a sandwich immunoassay, an exquisite protocol was successfully constructed for the CEA bioassay due to the dependence of differential pulse voltammetry (DPV) peak current signals of the Cu–CN/SPCE on the concentration of ascorbic acid. Under optimal conditions, this electrochemical immunoassay is capable of assaying the CEA biomarker sensitively, from which a linear range of 0.01 to 50 ng mL−1 was derived along with a low limit of detection (LOD) of 2.4 pg mL−1. In addition, this method shows good stability and high specificity in the detection process. Compared with the commercial ELISA detection method, the proposed sensing mode exhibits satisfactory accuracy in actual detection samples. Such enhanced analytical performance through atomic level dispersed metals provides a path for the future development of electrochemical immunoassay in the field of tumor biomarkers.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Hongshuai Cao,Yijing Dang,Zhonghai Zhang,Fengping Chen,Jingyao Liu,Qian Sun,Yangchun Xie,Zhiai Xu,Wen Zhang
The real-time detection of nitric oxide (NO) in living cells is essential to reveal its physiological processes. However, the popular electrochemical detection strategy is limited to the utilization of noble metals. The development of new detection candidates without noble metal species still maintaining excellent catalytic performance has become a big challenge. Herein, we propose a spinel oxide doped with heteroatom-Cu-doped Co3O4 (Cu-Co3O4) for the sensitive and selective detection of NO release from the living cells. The material is strategically designed with Cu occupying the tetrahedral (Td) center of Co3O4 through the formation of a Cu–O bond. The introduced Cu regulates the local coordination environment and optimizes the electronic structure of Co3O4, hybridizing with the N 2p orbital to enhance charge transfer. The CuTd site can well inhibit the current response to nitrite (NO2–), resulting in a high improvement in the electrochemical oxidation of NO. The selectivity of Cu-Co3O4 can be markedly improved by the pore size of the molecular sieve and the negative charge on the surface. The rapid transmission of electrons is due to the fact that Cu-Co3O4 can be uniformly and densely in situ grown on Ti foil. The rationally designed Cu-Co3O4 sensor displays excellent catalytic activity toward NO oxidation with a low limit of detection of 2.0 nM (S/N = 3) and high sensitivity of 1.9 μA nM–1 cm–2 in cell culture medium. The Cu-Co3O4 sensor also shows good biocompatibility to monitor the real-time NO release from living cells (human umbilical vein endothelial cells: HUVECs; macrophage: RAW 264.7 cells). It was found that a remarkable response to NO was obtained in different living cells when stimulated by l-arginine (l-Arg). Moreover, the developed biosensor could be used for real-time monitoring of NO released from macrophages polarized to a M1/M2 phenotype. This cheap and convenient doping strategy shows universality and can be used for sensor design of other Cu-doped transition metal materials. The Cu-Co3O4 sensor presents an excellent example through the design of proper materials to implement unique sensing requirements and sheds light on the promising strategy for electrochemical sensor fabrication.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Li Feng,Xiaoyun Lin,Junhui Feng,Xiaoqin Min,Yongnian Ni
This study presents the preparation of a novel electrochemical non-enzymatic sensor for the detection of glucose in natural saliva based on a metal organic framework (MOF) derivative (Cu-MOF-C) and nickel nanoparticle (NiNP) composite modified glassy carbon electrodes (GCE). The morphology and structural evolution were thoroughly characterized using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), ultraviolet and visible spectrum (UV) and Fourier transform infrared spectrum (FTIR). Moreover, the electrocatalytic activity of the NiNPs/Cu-MOF-C/GCE for glucose was investigated using cyclic voltammetry (CV) and the amperometric i-t technique. The NiNPs/Cu-MOF-C/GCE sensor exhibits a wide linear range of 0.3–1150 μM and low detection limit (DL) of 0.090 μM at a signal/noise ratio (S/N) of 3. The average recovery rate of this method is satisfactory between 97.3% and 108.4%. Furthermore, the sensor exhibited excellent repeatability, good stability and reproducibility for glucose detection. Compared with traditional invasive measurement, the detection of glucose in natural saliva can reduce the pain caused by continuous blood collection, which is an ideal method for patients requiring continuous monitoring of glucose.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Shiyao Lu,Jian Zhang,Hao Meng,Xiaoyuan Qin,Jianbin Huang,Yehao Liang,Feng-Shou Xiao
The direct dehydrogenation of ethyl lactate (EL) to produce ethyl pyruvate (EP) over non-precious heterogeneous catalysts is highly desirable, but challenging. Herein, we report a highly efficient silica-supported copper catalyst prepared via a hydrolysis-precipitation method (Cu/SiO 2 -HP) for the dehydrogenation of ethyl lactate, which exhibited an 85.4 % EL conversion with 91.1 % selectivity toward EP at 320 °C. XAFS, in situ XPS, and CO-adsorption FT-IR spectra revealed that the Cu/SiO 2 -HP catalyst had abundant Cu 0 /Cu + interfaces. In situ FT-IR spectra, kinetic studies , and theoretical calculations also demonstrated that the Cu 0 /Cu + interfaces synergistically activate the O−H and C−H bonds in the adsorbed EL for direct dehydrogenation into EP. The H/D kinetic isotope effect for model reaction confirmed that C−H bond activation is the key step in the dehydrogenation reaction. This study offers a new approach toward the selective conversion of EL into EP, which is of great significance for biomass conversion .
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CHEMOSPHERE
·
2022
·
IF 8.943
Zhiyu Wei,Jie Chen,Hongjin Tong,Mingchao Sun,Jing Tian,Lu Fan
CNTs-Al was prepared by ball milling combined with sintering process and then used for CNTs-Al-Cu synthesis with chemical deposition method. The obtained CNTs-Al-Cu composite was systematically characterized and its NO 3 − -N reduction performance under alkaline condition was also evaluated. As indicated by the reduction batch experiment, 80.2% of NO 3 − -N removal efficiency was obtained in 90 min at pH of 9. The product of the reduction process was dominated by NO 2 − -N, which was further reduced to harmless N 2 . The reusability of CNTs-Al-Cu composite was evaluated, and the experiment results showed that 68.1% of NO 3 − -N removal efficiency was maintained after 3 cycles of regeneration. Finally, based on the characterization results and kinetic analysis, it was concluded that micro-electrolysis was mainly responsible for the removal of NO 3 − -N by CNTs-Al-Cu.
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Materials Today Communications
·
2023
·
IF 3.8
Zhuo Xing,Juhai Weng,Chi Ma
A series of Zn 2- x Cu x GeO 4 ceramics were prepared by the solid-phase sintering method. Cu 2+ substitution for Zn 2+ facilitated the single-phase formation and benefited densification via lowering the sintering temperatures , hence thereby the microwave dielectric properties were largely improved. A representative composition with x = 0.08 revealed a homogenous Zn 2 GeO 4 phase with good microwave dielectric properties: ε r ∼ 7.47, Q × f ∼ 56,980 GHz, and τ f ∼ −13.9 ppm/°C when sintered at 1000 °C. To evaluate the potential application of low-temperature cofired ceramics (LTCC), sintering aids (B 2 O 3 ) were added to the x = 0.08 sample to reduce its sintering temperature to below 960 °C. A dramatic improvement in Q × f ∼ 107,415 GHz was observed with only 0.5 wt % B 2 O 3 addition. Chemical compatibility was confirmed via cofiring with silver electrodes at 940 °C. All the merits show promising potential for advanced substrates.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xinxin Yuan,Zhiling Huang,Jinhua Li,Yue Meng,Zhenhai Gu,Bo Xie,Zheming Ni,Shengjie Xia
The steric effect caused by the lattice mismatch between the two phases hinders the separation and transfer of photogenerated carriers, which is one of the important factors limiting the activity of heterojunction photocatalysts. In this paper, semi - coherent interface Cu2O/Cu7S4 heterojunction was successfully constructed based on the epitaxy growth method of anion exchange. The degradation of tetracycline by semi - coherent interface Cu 2 O/Cu 7 S 4 -30 heterojunction under simulated visible light reached 95.3 % at 60 min, which is a significant improvement compared with single-phase catalysts and ordinary heterojunction catalysts (Cu 2 O/Cu 7 S 4 -mix). The experimental characterization and theoretical calculations confirmed the existence of unique S-Cu-O chemical bonds in the semi - coherent interface Cu 2 O/Cu 7 S 4 heterojunction. On the basis of heterojunction energy band bending and the formation of built-in electric fields, the S-Cu-O bonds can act as a specific bridge to further facilitate the separation, transfer and delivery of photoelectrons and holes, which contributes to the generation of more oxidatively active species (mainly superoxide radicals and holes). In addition, based on experimental characterization and theoretical calculations, the intermediates, degradation pathways and photodegradation mechanisms of the degradation process have also been discussed in detail.
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