Small
·
2023
·Vol. 19
·期 49
·2304644
·
IF 13.3
Ping Lu,Zhaoyang Qi,Jie Chen,Changshen Ye,Ting Qiu
High-efficiency adsorption of aromatic sulfur-containing compounds from liquid hydrocarbon fuels over metal-organic frameworks (MOFs) is challenging because of inert metal sites. A new method, the Ce-enhanced modulation of MOFs’ microenvironment, is proposed to modulate the –COO···Cu(II)– coordination microenvironment of Hong Kong University of Science and Technology (HKUST-1) using Ce(III) as a molecular scalpel for fabricating abundant high-efficiency Cu(I) and Cu-coordination-unsaturated sites and improving the pore structures around adsorptive sites. The optimal CH-250 thus exhibits adsorptive capacities for 20.2, 28.0, and 58.3 mg S g –1 of thiophene, benzo-thiophene, and dibenzothiophene, respectively, which are superior to most reported MOFs, zeolites, and nanoporous carbons. The constructed Cu(I) sites show stronger affinity for dibenzothiophene (−0.86 eV) than the initial Cu(II) (−0.74 eV) for out-of-plane adsorption. Further, they are far stronger in-plane adsorption interactions in DBT/CH-250 (−0.90 eV) than those in DBT/HKUST-1 (−0.37 eV). Thus, molecular engineering for modulating the coordination microenvironment of MOFs shows great potential for adsorption desulfurization.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Jianguo Yu,Zehui Yu,Yunling Jia,Ting Ran,Ming Song,Yanshuang Zhang,Qing Wang,Yuning Qu,Lili Wang
Direct alcohol fuel cells' performance is significantly affected by the phase and composition of the catalyst, thereby the development of high-performance alcohol oxidation catalysts is essential. In this study, PVA preparation was used for the first time to create PdCu core-shell nanoflowers with a high electrochemically active surface area and a potent synergistic effect. Notably, the presence of PVA causes Pd and Cu nanoparticles with different reduction rates to form a core-shell structure, and the Pd nanoparticles continue to migrate regularly under the action of PVA, forming a flower-like morphology with a high degree of branching. Cu@Pd 22.3 catalyst exhibited 13 times higher catalytic performance (4353.04 mA mg Pd −1 ) than Pd/C (334.09 mA mg Pd −1 ) in ethylene glycol oxidation reaction. The Cu@Pd 22.3 catalyst also exhibits higher stability than commercial Pd/C in stability tests lasting up to 20,000 s. This core-shell combination and highly branched structural design result in more active sites for fast ion adsorption/desorption,offering an original method to improving the activity and endurance of polyol oxidation.
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Catalysts
·
2023
·Vol. 13
·期 7
·1066
·
IF 3.9
Xi’an Guan,Yehong Wang,Xiumei Liu,Hong Du,Xinwen Guo,Zongchao Zhang
As clean energy, methane has huge reserves and great development potential in the future. Copper zeolites are efficient in the oxidation of methane to methanol. Water has been confirmed as a source of oxygen to regenerate the copper-zeolite active sites to enable selective anaerobic oxidation of methane to methanol. In this work, we report that the methanol yield increased from 36 μmol/g (Cu-MOR1) to 92 μmol/g (Cu-MOR1-water) as a result of water enhancing the activity of copper ion-exchange mordenite catalyst. We show for the first time that water could convert inactive copper species into active copper species during catalyst activation. A combination of the XPS, FTIR, and NMR results indicates that water dissociates and then converts ZCuIIZ into ZCuII(OH) (where Z indicates framework O (Ofw) bonded to one isolated Al in a framework T-site, i.e., 1Al) and simultaneously produces a Brönsted acid site during catalyst activation. This finding can be used to tune the state of copper species and design highly active copper-zeolite catalysts for methane oxidation to methanol.Keywords:Cu-MOR;water;methane to methanol;ZCuIIOH;XPS
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Jingpi Gao,En Li,Kena Song,Tongtong Ma,Ran Yang,Yi Zhang,Nan Li,Xiaoran Liu,Jinghua Li
The dye degradation method based on Fenton-like heterogeneous nanostructures has gained significant attention in recent years. We have developed a Copper-Stannum-Polypyrolle-Heterogeneous (Cu–Sn oxide-PPy Heterogeneous, CSPHGs) catalytic system. The system uses a PN junction formed by two oxide semiconductors (Cu 2 O and SnO 2 ) as the core, which is then coated with polypyrolle (PPy) on the outer layer. Under near-infrared (NIR) light irradiation (500.0 μg ml −1 , 1.2w·cm −2 ), the temperature rapidly reached approximately 45 °C within 5 min, demonstrating excellent photothermal performance. We have overcome the limitation of traditional Fenton reactions that require weak acidic conditions for effective operation. Moreover, we have increased the photostability of Cu 2 O monomers by incorporating them into a three-layer heterostructure . The Rhodamine B (RhB) degradation experiment revealed that the generated reactive oxygen species (·OH), effectively catalyze the decomposition of dyes. Within 120 min, the degradation rate exceeded 99%. This research provides a new option for environmental remediation through the combination of photo-Fenton and photothermal processes.
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Nanomaterials
·
2022
·Vol. 12
·期 21
·3844
·
IF 5.719
Zhenlan Xu,Qing Tang,Aimei Hong,Lingxiangyu Li
Along with the development of nanotechnology, nanomaterials have been gradually applied to agriculture in recent years, such as Cu(OH)2-nanorods-based nanopesticide, an antibacterial agrochemical with a high efficacy. Nevertheless, knowledge about physical stability of Cu(OH)2nanopesticide in soil solutions is currently scarce, restricting comprehensive understanding of the fate and risk of Cu(OH)2nanopesticide in the soil environment. Herein we investigated aggregation, sedimentation and dissolution of Cu(OH)2nanopesticide in soil solutions extracted from three different soil samples, wherein commercial Cu(OH)2nanopesticide formulation (NPF), as well as its active ingredient (AI) and laboratory-prepared Cu(OH)2nanorods (NR) with similar morphology as AI, were used as model Cu(OH)2nanopesticides. We found that NPF compared to AI showed less extents of aggregation in ultrapure water due to the presence of dispersing agent in NPF. Yet, moderated aggregation and sedimentation were observed for Cu(OH)2nanopesticide irrespective of NPF, AI or NR when soil solutions were used instead of ultrapure water. The sedimentation rate constants of AI and NPF were 0.023 min−1and 0.010 min−1in the ultrapure water, whereas the rate constants of 0.003–0.021 min−1and 0.002–0.007 min−1were observed for AI and NPF in soil solutions, respectively. Besides aggregation and sedimentation, dissolution of Cu(OH)2nanopesticide in soil solutions was highly dependent on soil type, wherein pH and organic matter played important roles in dissolution. Although the final concentrations of dissolved copper (1.08–1.37 mg/L) were comparable among different soil solutions incubating 48 mg/L of AI, NPF or NR for 96 h, a gradual increase followed by an equilibrium was only observed in the soil solution from acidic soil (pH 5.16) with the low content of organic matter (1.20 g/kg). This work would shed light on the fate of Cu(OH)2nanopesticide in the soil environment, which is necessary for risk assessment of the nanomaterials-based agrochemical.Keywords:soil solutions;aggregation;sedimentation;Cu(OH)2nanopesticide;dissolution
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MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Ping Yang,Xiuhong Meng,Penghu Guo,Rujin Zhou,Youhua Zhang,Shui Cao,Dan Zhang,Hongbing Ji,Linhai Duan
Two critical characteristics for gas adsorption and separation are the porosity and open metal sites of adsorbents. The Cu–BTC (BTC = benzene–1,3,5–tricarboxylate) structure was tailored using a template synthesis technique to increase the separation performance for C 3 H 6 /C 3 H 8 mixtures. The three hierarchical porous frameworks, Cu x O y @HP–Cu–BTC, synthesized using a cationic surfactant (cetyltrimethylammonium bromide (CTAB)), a neutral organic amine (N,N–dimethyltetradecylamine (N,N)), and an anionic surfactant (sodium dodecylbenzene sulfonate (SDBS)) as the template, Cu x O y @HP–Cu–BTC(SDBS) exhibited the best performance, with a C 3 H 6 adsorption capacity of 6.679 mmol g −1 , which was significantly greater than that of C 3 H 8 (5.721 mmol g −1 ). Cu x O y @HP–Cu–BTC(SDBS) has an ideal ultra–microporous structure that encloses C 3 H 6 molecules precisely while rejecting slightly bigger C 3 H 8 molecules, and C 3 H 6 interacts strongly with unsaturated metal sites through particular π–Cu bonds. According to the ideal adsorbed solution theory (IAST), the adsorption selectivity of C 3 H 6 /C 3 H 8 was 63.322, which is more than that of the reference adsorbent Cu–BTC. Additionally, the breakthrough studies shown that Cu x O y @HP–Cu–BTC(SDBS) has a good dynamic performance for the effective separation of the C 3 H 6 /C 3 H 8 mixture.
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Biosensors-Basel
·
2022
·Vol. 12
·期 10
·881
·
IF 5.743
Pei Dai,Xianzhi Huang,Yaqian Cui,Lihua Zhu
Tetrabromobisphenol A (TBBPA) was one of the most widely used brominated flame retardants. However, it easily contaminates nature and harms the environment and human health during its production and use. Therefore, it is necessary to strictly control the content of TBBPA in electronics. Surface-enhanced Raman spectroscopy has the advantages of being fast and sensitive, but it is difficult to obtain the SERS spectra of TBBPA because the hydrophobic TBBPA molecule is difficult to approach with the hydrophilic surface of common noble metal SERS substrates. In the present work, a hydrophobic Cu-Ag chip was developed for the SERS detection of TBBPA. The integration of the hydrophobic interaction and the Ag-Br bonding promoted the adsorption of TBBPA on the Cu-Ag chip, allowing for SERS detection. It was observed that both the hydrophobicity and bimetallic composition of the Cu-Ag chip played important roles in the SERS detection of TBBPA. Under the optimized conditions, the low limit of detection of the established SERS method for TBBPA was 0.01 mg L−1, within a linear range of 0.1–10 mg L−1. Combined with ultrasonic-assisted extraction, the substrate could be used for the quantitative determination of TBBPA in electronic products. Compared with the HPLC-UV method used as a national standard, the relative error of the SERS method for quantifying the TBBPA content in a mouse cable and shell was ±3% and ±7.7%, respectively. According to the SERS results, the recovery of TBBPA in the spiked mouse shell was 95.6%.Keywords:tetrabromobisphenol A;surface-enhanced Raman scattering;hydrophobic interaction;bi-metal chips;synergistic coupling
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Jing Huang,Jiawei Dai,Jiannan Zhu,Rong Chen,Xiaoqi Fu,Hongfang Liu,Guangfang Li
Electrocatalytic reduction of CO 2 (CO 2 RR) represents a promising approach to reduce CO 2 emission and generate value-added chemicals. Herein, we developed bimetallic Au-Cu gradient alloy nanostructures (AuCu-g) comprising of ultrathin Cu-rich alloy surface and Au-rich alloy core as electrocatalyst via a facial solvothermal method. Impressively, the AuCu-g can stably generate a considerable amount of C 2 H 4 with faradaic efficiency (FE) ∼20 % at a low limiting potential of −0.4 V versus reversible hydrogen electrode (RHE) due to its unique gradient structure and multi-component tandem effect. The potential-dependent in situ Raman spectrum indicated an enhanced *CO adsorption strength and a remarkable CO intermediate generation over Au-Cu gradient alloy at low overpotentials during CO 2 reduction process. This work shines a light for developing mutilmetallics toward efficient CO 2 RR.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Hongai Zheng,Meilin Zhu,Derui Wang,Yao Zhou,Xin Sun,Shuangyan Jiang,Mengyao Li,Cunzheng Xiao,Daquan Zhang,Lizhi Zhang
Membrane fouling is one of the main impediments that limit the wide application of Polyvinylidene fluoride (PVDF) membrane. In this study, for the first time, we incorporated the cellulose nanocrystal (CNCs) onto Cu-MOF-74 by physical stirring and then coated the composites on the PVDF membrane to ameliorate the antifouling performance. The PVDF membrane with the addition of CNC/Cu-MOF-74 composite showed enhanced hydrophilicity compared with the pristine membrane, which significantly promoted the permeability and antifouling performance. The Bovine serum albumin (BSA) multiple-cycle antifouling results revealed that the flux recovery ratio (FRR) value (76.9 %) was much higher than that of the pristine membrane (60.8 %). The enhancement of recovery flux was correlated with the increased electrostatic repulsion and hydrophilicity of the modified membrane according to the contact angle test and Zeta-potential measurement. Meanwhile, the CNC/Cu-MOF-74 modified membrane showed improved antibacterial efficiency (96.3 % at 4 h) due to the predominant antibacterial efficacy of Cu-MOF-74. The efficiently antibacterial achievement of modified membrane was attributed to the release of Cu 2+ and the generation of •OH. This study proposed a novel modified membrane with excellent antifouling properties and provided new insights into the fabrication of antifouling membranes with outstanding performance.
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ACS Omega
·
2022
·
IF 4.132
Lian-Jiao Zhou,Yu-Ying Wang,Shu-Lan Li,Ling Cao,Feng-Lei Jiang,Thomas Maskow,Yi Liu
Cu-modified nanoparticles have been designed to mimic peroxidase, and their potent antibacterial and anti-biofilm abilities have been widely investigated. In this study, novel core–shell polydopamine (PDA)/Cu4(OH)6SO4 crystal (PDA/Cu) nanometer rods were prepared. The PDA/Cu nanometer rods show similar kinetic behaviors to chloride-activated peroxidases, exhibit excellent photothermal properties, and are sensitive to the concentrations of pH values and the substrate (i.e., H2O2). PDA/Cu nanometer rods could adhere to the bacteria and catalyze hydrogen peroxide (H2O2) to generate more reactive hydroxy radicals (•OH) against Staphylococcus aureus and Escherichia coli, Furthermore, PDA/Cu nanometer rods show enhanced catalytic and photothermal synergistic antibacterial activity. This work provides a simple, inexpensive, and effective strategy for antibacterial applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Fan Gao,Zhuzhu Xiong,Yi Jia,Hong Li,Junbai Li
As a good alternative for natural enzyme, enzyme mimics with artificial functional materials have attracted considerable attention. However, it remains a great challenge to develop a facile method to design laccase mimic with high catalytic activity, long-term stability and reusability. In this report, we propose the one-pot synthesis of reusable paper filter templated Cu-doped polydopamine membranes (PF@PDA/Cu) with laccase-like activity. Compared with the natural laccase, the PF@PDA/Cu membrane exhibits enhanced catalytic activity for the chemical conversion of hydroquinone into benzoquinone . Interestingly, these membranes present good tolerance to high temperature and the catalytic activity increases with the increase of temperature. Moreover, these membranes could be stored for 7 days and recycled for 5 times with negligible loss of catalytic activity. This work provides a promising paradigm for rational design and practical applications of metal-loading PDA materials based on one-pot synthesis methodology.
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Small
·
2022
·Vol. 18
·期 34
·2202405
·
IF 15.153
Hong Li,Zhuzhu Xiong,Yi Jia,Fan Gao,Chenlei Wang,Qi Li,Junbai Li
The development of high-efficiency enzyme mimics is of great significance in the field of biocatalysis. However, it remains challenging to design novel enzyme mimics with multiple enzyme-like activities, excellent stability, and good reusability. Herein, a facile molecular assembly strategy to construct dialdehyde cellulose (DAC) templated Cu-doped polydopamine (DAC@PDA/Cu) membrane with dual enzyme-like activities is presented. The Schiff base bonds formed between polydopamine (PDA) and DAC can not only accelerate the adhesion of PDA thin layer but also contribute to Cu-loading and high stability of DAC@PDA/Cu membrane. Importantly, the assembled DAC@PDA/Cu membrane exhibits a remarkable catalytic activity that is superior to the natural laccase along with high stability and excellent reusability. Moreover, the DAC@PDA/Cu membrane also demonstrates peroxidase-like activity, and it is successfully applied in the sensitive detection of ascorbic acid (AA). This work will provide a new paradigm methodology for rational design and practical applications of enzyme mimics based on bioinspired molecular assemblies.
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