MICROCHIMICA ACTA
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2024
·Vol. 191
·期 12
·1-13
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IF 5.3
Wang Xue,Zhao Zixuan,An Long,Wang Tianxiang,Yang Xiaojing,Shan Jiajia
An unlabeled electrochemical sensing strategy based on electroactive copper-centered metal–organic framework (Cu-MOF) film coupled with multiwalled carbon nanotubes (MWCNTs) was proposed for the rapid assessment of nanoplastic concentration. The sensing interface was fabricated via the electro-deposition of Cu-MOF on the pre-modified MWCNTs using the cathodic reduction method. The exposed copper active sites in Cu-MOF showed excellent electrochemical activity, which was further enhanced due to rapid electron transfer induced by highly conductive MWCNTs. Through the adsorption functionality of Cu-MOF film towards polystyrene (PS) nanoplastics, the rapid recognition for nanoplastics in aqueous solution was achieved, thereby causing the inhibition of the current response. The results showed a robust dependence of the inhibition rate on the PS mass concentration. The proposed detection method was used for the quantitative determination of PS nanoplastics with the sizes of 100 nm, 500 nm, and 1 μm. The applicability of this electrochemical sensing platform was successfully validated in real-world water sample analysis. Graphical abstract
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Journal of Water Process Engineering
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2024
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IF 6.3
Xingping Deng,Hua Yang,Dongye Zhao,Jingchun Guan,Zhengxuan Gu,Liang Zhang
Graphitic carbon nitride (g-C 3 N 4 ), a nitrogen-rich polymeric semiconductor, has gained significant attention as a photocatalyst . However, its potential to activate permonosulfate (PMS) has been somewhat limited. Prior research has demonstrated that manganese-doped g-C 3 N 4 can effectively activate PMS to degrade pollutants, with Mn 3+ playing a pivotal role. Consequently, enhancing the Mn 3+ content within the system is of paramount importance. In this study, we developed a novel class of manganese‑copper doped g-C 3 N 4 materials using a hydrothermal-calcination process. The optimized material, denoted as Mn 5 Cu 5 -CN, was synthesized at a Mn/Cu molar ratio of 1:1. When applied to degrade a model contaminant, acetaminophen (ACP), the Mn 5 Cu 5 -CN/PMS system demonstrated remarkable efficiency, degrading nearly 20 mg/L of ACP within 30 min (material dosage = 0.4 g/L, PMS concentration = 2.0 mM). The Mn 5 Cu 5 -CN exhibited favourable performance across a broad pH range. Singlet oxygen ( 1 O 2 ) was identified as a major player in the degradation of ACP. X-ray photoelectron spectroscopy (XPS) analyses revealed that the cyclic redox reactions of Mn 3+ /Mn 4+ and Cu + /Cu 2+ led to the abundant generation of 1 O 2 . Superoxide (O 2 •- ) was identified as an important intermediate product in these processes. Additionally, the g-C 3 N 4 present in the material also facilitated the generation of reactive oxygen species (ROS). This study provides a fresh perspective on the utilization of g-C 3 N 4 for pollutant degradation, highlighting the potential of Mn Cu doped g-C 3 N 4 materials in environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Shuang Wu,Yangli Cui,Lan Liang,Wenjie Gao,Zhen Yu,Zhanjun Cheng,Beibei Yan,Guanyi Chen,Ning Li
Heterogeneous catalyst reuse and the effectiveness of hydrogen peroxide (H 2 O 2 )-based advanced oxidation processes under near-neutral conditions remain an obstacle in wastewater remediation. Herein, we put forward a versatile catalytic membrane with Cu-doped MnO active layer anchoring on the polydopamine-modified electrospinning polyvinylidene fluoride (PDA@PVDF) base. The Cu-MnO@PDA@PVDF membrane was conferred admirable sulfamethoxazole (SMX) reduction (over 90% within 90 min) and clogging alleviation (relative flux recovery to 0.98) capabilities via in situ H 2 O 2 activation at pH 8, which was slightly affected by actual water background. Electron paramagnetic resonance (EPR) and trapping tests unveiled the joint contribution of • OH, O 2 •− and 1 O 2 , with • OH exerting the supreme role in SMX oxidation. The inherent characteristics of dual Mn-Cu centers on the membrane surface for facilitation of electron transfer, H 2 O 2 adsorption and barrierless dissociation to • OH were further elucidated by electrochemical measurements and density functional theory (DFT) computation. Comprehensively, this study proposes a facile procedure and insights into engineering catalytic membrane coupled H 2 O 2 strategy for refractory organic treatment at ambient conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Cui Zhang,Saiyu Dong,Zhaoli Liu,Nairu Liu,Xi Zhang,Jie Dong,Xueping Zhou,Yirong Guo,Jianxiang Wu
Immunochromatographic test strip (ITS) has been widely employed for point-of-care diagnoses. However, how to significantly enhance the analytical sensitivity of device-free ITS remains a challenge. Here, we synthesized a Cu single-atom anchored Co 3 O 4 (CuSA/Co 3 O 4 ) nanozyme that possesses ultrahigh peroxidase-mimicking catalytic activity owing to d -band center upshift mediated by Cu single-atom. Molecular orbital analysis demonstrated that d orbitals in CuSA/Co 3 O 4 have stronger orbital hybridization affinity than Co 3 O 4 to H 2 O 2 ′s π* orbitals. This reinforces hydroxyl radical ( OH) production and provides a stronger catalytic colorimetric signal, which is beneficial for improving the sensitivity of ITS. Moreover, we applied the CuSA/Co 3 O 4 to ITS as a signal reporter for monitoring Xanthomonas oryzae pv. oryzicola (Xoc) , the pathogen of rice bacterial leaf streak. The visual limit of detection (LOD) of the developed CuSA/Co 3 O 4 -based ITS was as low as 6.4 × 10 2 CFU mL −1 , which is 25-fold more sensitive than the traditional Au nanoparticles (AuNP)-based ITS. Taken together, this work demonstrates the great potential of CuSA/Co 3 O 4 nanocomposite as a signal reporter to improve the sensitivity of ITS for on-site Xoc detection.
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Nano Today
·
2024
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IF 13.2
Hui Huang,Wendi Xuan,Jiakang Hai,Xue Wang,Meng Chen,Guobing Hong,Xinyue Dai,Lili Xia,Wei Feng,Yu Chen
Bioorthogonal reaction refers to chemical reactions that occur within a biological system without interfering the normal biochemical process, offering the unprecedented versatility in engineering chemical reactions within cells. However, the precise regulation of bioorthogonal reaction in living systems is mired by the complexity of the physiological environment and the toxicity of catalysts. Herein, considering the deeper tissue penetration and reduced phototoxicity compared to visible light and ultraviolet, a second near infrared (NIR-II) light-activated Cu-based bioorthogonal reaction is developed to achieve precise spatiotemporal control and effective switching for Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) mediated chemical transformations in tumor, reducing the off-target effects. The catalytic activity of Cu catalyst through valence state interconversion between Cu(II) and Cu(I) can be precisely regulated in a reversible manner under NIR-II light irradiation-induced photoelectron transfer, which controls the extent of desired drug synthesis in bioorthogonal reaction. Meanwhile, the adverse effects of Cu(I) can be substantially mitigated within normal tissues due to their oxygen-rich condition. By utilizing NIR-II light and oxygen level, the Cu bioorthogonal catalyst achieves a balance between catalytic activity and biocompatibility. The ability to achieve precise spatiotemporal control and reversible catalysis makes this NIR-II light-mediated CuAAC platform an efficient and adaptable tool for bioorthogonal chemistry in living systems.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Xiangxue Zhang,Nina Fei,Qianhong Wang,Ali Raza Khan,Wenyao Chen,Gang Qian,Jing Zhang,De Chen,Xuezhi Duan,Xing-Gui Zhou,Weikang Yuan
Oxygen vacancy regulation in metal catalysts has emerged as a crucial strategy for efficiently degrading volatile organic compounds (VOCs), while the acquisition of kinetics and mechanistic insights into the oxygen vacancy roles remains highly desirable yet challenging. Herein, we conduct a combined kinetics and mechanistic investigation into the oxygen vacancy effects of Cu catalysts on toluene oxidation. Cu catalysts with varying oxygen vacancy contents are prepared using three representative metal oxide supports, including reducible ZrO2 with strong oxygen storage capacity, reducible ZnO, and unreducible Al2O3. The toluene oxidation as well as CO oxidation are tested for these catalysts, revealing the superior catalytic activity of Cu/ZrO2 catalyst. Multiple charactrizations demonstrate that the strong reducibility and abundance of oxygen vacancies within the Cu/ZrO2 catalyst are the key factors for these reactions. A redox-based kinetics strategy is further applied to decouple the reduction and oxidation steps, thus affording a rate diagram to elucidate the promotional effects of oxygen vacancies on toluene decomposition. Additionally, in-situ DRIFTS study unveils the reaction pathway, showing the transformation from toluene to benzyl alcohol, benzaldehyde, benzoate, phenol, anhydride, carbonate, and ultimately to CO2. As a result, the oxygen vacancy-tuned rate-relevant step is disclosed, shifting from C-H bond cleavage for the Cu/Al2O3 catalyst with limited oxygen vacancies to the C=O and C=C bond cleavage for the Cu/ZnO and Cu/ZrO2 catalysts with more oxygen vacancies. The kinetics and mechanistic insights gained here would help guide the design of highly efficient oxidative catalysts by tuning the oxygen vacancies of support.
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JOURNAL OF CATALYSIS
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2018
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IF 6.759
Bing Hu,Yazhi Yin,Guoliang Liu,Shengli Chen,Xinlin Hong,Shik Chi Edman Tsang
Surface modification with Pd is an effective way for improved activity in CO 2 hydrogenation to methanol over commercial Cu-ZnO catalysts via a so-called hydrogen spillover mechanism. However, there still lacks a quantitative analysis of hydrogen spillover effect and the nature of active sites after Pd modification remains unclear. In this work, we prepared a series of Pd-doped Cu-ZnO catalysts (Pd-CZ-x) with tunable Pd loading by using a facile polyol reduction method for a deep study of the promotion effect of Pd. With the increase of Pd/Cu molar ratio (x) from 0 to 0.04, there emerges a volcano-shaped relationship between methanol space time yield (STY) and Pd loading. 1% Pd doping can increase the methanol STY by 2.5 times and the methanol turnover frequency (TOF) by 3.5 times at 543 K, when compared to undoped Cu-ZnO. Kinetic studies show the activation energy required for methanol synthesis is greatly reduced from 59 kJ mol −1 over Cu-ZnO to 31 kJ mol −1 over Pd-CZ-0.01. Behind the volcano-shaped relationship is a balance between the hydrogen spillover effect of Pd and the reduced surface Cu area caused by Pd blocking. Chemisorption gives a quantitative analysis of an important type of activated Cu sites enabled by hydrogen spillover (Cu hs ). Importantly, it is found that the methanol STY correlates linearly with Cu hs surface area, suggesting that the activated Cu sites with the assistance of ZnO are real active sites for methanol synthesis from CO 2 hydrogenation.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2017
·
IF 3.671
Shaojun Yuan,Ping Zhang,Zhenyi Yang,Li Lv,Shengwei Tang,Bin Liang
Cross-linked chitosan (CCS) microspheres tethered with melamine-conjugated poly(hydroxyethyl methacrylate) (PHEMA) brushes were synthesized by combination of surface-initiated atom transfer radical polymerization (ATRP) of HEMA and subsequent covalent immobilization of melamine onto the chain ends of PHEMA brushes. The as-synthesized CCS microsphere was used as a novel adsorbent for effective uptake of Cu(II) ions from aqueous solution. Success in each functionalization step was ascertained by SEM, ATR-FTIR and XPS characterization. Batch adsorption experimental results demonstrated that the adsorption equilibrium of Cu(II) ions on the melamine-grafted CCS microsphere was rapidly established within 20 min, and the adsorption process was found to be governed by intra-particle diffusion and chemisorption processes. The Langmuir-fitted maximum adsorption capacity of Cu(II) ions on the as-synthesized CCS microspheres was as high as circa 4.67 mmol L −1 (299 mg g −1 ). The calculated thermodynamic parameters revealed an endothermic and spontaneous adsorption process of Cu(II) ions on the melamine-grafted CCS microspheres. XPS spectra revealed that the adsorption mechanism was attributed to coordination (or chelation) interactions between amino (or hydroxyl) groups with cationic Cu(II) ions.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2018
·
IF 3.779
Liang Liu,Rui Bao,Jianhong Yi,Dong Fang
Mono-dispersed and homogeneous carbon nanotube (CNT)/copper (Cu) composite powders were fabricated by spraying pyrolysis (SP) method successfully. Subsequently, CNT/Cu composites were obtained by spark plasma sintering (SPS) at sintering temperature ranged from 1023 to 1223 K (70–90% melting point of pure Cu). The mechanical properties , micro-morphology and interface microstructure of CNT/Cu composites were measured and characterized. The results reveal that Cu nano-particles (NPs) coated on the CNT surface are conducive to improving the wettability of CNT within matrix and reducing the interface energy between matrix and CNT, and finally stable interface structure is established. The traditional trade-off tendency between strength and ductility is balanced in the CNT/Cu composites, which are sintered at 1223 K. The ultimate tensile strength (UTS) shows 344 MPa and the elongation is 19.6%, which owing to the improvement of CNT–Cu interface bonding. At last, the role of interfacial bonding extent played in determining the load transfer efficiency of CNT is discussed.
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JOURNAL OF POROUS MATERIALS
·
2024
·
IF 2.5
Zhang Wenhui,Wu Xinbo,Wang Dazhi,Cai Weijie
As the frequency range of electronic devices gradually expands, exploring frequency insensitive electromagnetic wave adsorption (EWA) materials that can achieve effective absorption in all bands has aroused great interest. A series of Fe 1 − x S@C composite materials with three-dimensional conductive networks were successfully prepared in this work. In the preparation process, poly (aryl ether sulfone) with branched carboxylic (PAES-C) was selected as the skeleton and Fe 3+ ions were introduced via chemical adsorption. The main purpose of this work was to develop array porous composite materials with good EWA property. The work proposed a novel controllable method for preparing metal sulfides to explore the electromagnetic wave absorption. This routine was also developed to prepare other M x S@C composites (M = Fe, Cu, Mn). Compared to Mn x S@C and Cu x S@C composites, the RL min value of Fe 1 − x S@C-4 was − 40.6 dB at 13.52 GHz, and at a thickness of 1.5 mm the effective bandwidth reached 3.12 GHz. Furthermore, its effective absorption band covered Ku, X, and C radar bands at different thicknesses.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Jie Song,Lijun Chen,Yingnan Zhou,Zhiwen Yuan,Yuhua Niu,Zhiqiang Wei
With the rapid development of industrialization, the removal of heavy metal ions and small organic molecules from wastewater has triggered a hot debate. ZIF-8 was grown on a sodium alginate backbone using an in situ growth technique, the core-shell P-SMG@ZIF-8 was synthesized. It was also characterized by FTIR, XRD, SEM, UV–Vis and XPS, and the optimal conditions and mechanism of adsorption were explored. At pH 2.0, a contact time of 200 min, and 298 K, removal of Cu(II) and Ph up to 80.2 %, 65.6 % by P-SMG@ZIF-8, adsorption behavior consistent with Langmuir model for pseudo-secondary rates, the saturated adsorption of Cu(II) and Ph could reach up to 83.5812 mg/g and 78.1779 mg/g, respectively. And the adsorbed P-SMG@ZIF-8 is easy to separate and reusable, which is a cost-effective and efficient natural product-based adsorption material.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yi Fang,Shoubing Chai,Zhiwei Chu,Zirui He,Yingjie Li
In the calcium looping CO 2 capture process, using CO in the flue gas to reduce NO at a high molar ratio of CO to NO (e.g., above 10:1) can achieve efficient removal of NO. However, the lots of unreacted CO causes secondary pollution. In this study, a novel Cu/Ce co-modified CaO was proposed for cyclic CO 2 capture and the catalytic NO reduction at a low CO:NO molar ratio (e.g., 2:1). The experimental findings indicate that Cu/Ce modification improves the performance of CaO in both catalytic NO reduction and carbonation. The Cu/Ce co-modified CaO contained the optimal Cu/Ce/Ca molar ratio of 1:5:100 possesses both NO removal and CO conversion efficiencies of above 99 %, along with CO 2 removal efficiency exceeding 88%. Microscopic analysis determines that the electron transfer between Cu and Ce facilitates the conversion of lattice oxygen into surface oxygen, mitigating the competition between CO 2 and CO for surface oxygen. Furthermore, density functional theory calculations demonstrate that CO/NO/CO 2 exhibits non-competitive adsorption behavior on Cu/Ce co-modified CaO. Consequently, Cu/Ce-modified CaO possesses superior catalysis for efficient NO reduction by CO at low CO:NO molar ratio in calcium looping process.
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