Small
·
2020
·Vol. 17
·期 27
·1907114
·
IF 11.459
Qinzhen Li,Jinsong Chai,Sha Yang,Yongbo Song,Tao Chen,Cheng Chen,Hui Zhang,Haizhu Yu,Manzhou Zhu
Thiolate-protected nanoclusters with different charge states usually show similar structure frameworks but different electronic configurations, which are proved to dramatically affect their properties such as magnetism, photoluminescence, and catalytic activity. Until now, few nanoclusters with alterable charge states have been reported and only some of them are structurally solved, limiting the in-depth studies on their interesting properties. Here, a new Au Cu alloy nanocluster [Au 18 Cu 32 (SPhCl) 36 ] 2− (HSPhCl = 4-chlorophenylthiophenol) is synthesized and structurally solved by X-ray crystallography. Interestingly, it is found that this nanocluster can be reduced to another nanocluster with a different charge state, that is, [Au 18 Cu 32 (SPhCl) 36 ] 3− . This change in charge states is clearly proved by X-ray crystallography, electrospray ionization mass spectrometry, thermogravimetric analysis, and electron paramagnetic resonance. Furthermore, several redox methods are carried out to realize the reversible interconversion between these two nanoclusters, including electrochemical redox, introduction of H 2 O 2 /NaBH 4 , and oxidation with silica under air atmosphere. This work offers new insight into the transform progress of charge states with Au Cu alloy nanoclusters which contributes to the understanding of the relationship between electronic structure and properties of nanoclusters and further development of Au Cu nanoclusters with excellent performance.
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高影响因子
JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Zhi-Feng Jiao,Ya-Ming Tian,Xiao-Ning Guo,Udo Radius,Holger Braunschweig,Todd B. Marder,Xiang-Yun Guo
A highly efficient photocatalytic protocol for borylation of alkyl bromides and chlorides with graphene supported Cu/Pd alloy nanoparticles as a heterogeneous catalyst is reported. This photocatalytic system operates with visible light in air, providing a wide range of primary and secondary alkyl halides with B 2 pin 2 or B 2 neop 2 in high yields at low temperatures, thereby demonstrating its broad utility and functional group tolerance. The high performance is attributed to a synergistic effect of localized surface plasmon resonance (LSPR) of Cu and charge transfer from Cu to Pd due to the alloy surface charge heterogeneity. Transfer of energetic electrons from Pd to electrophilic alkyl halides lead to the formation of the alkyl radicals, which quickly react with a nucleophilic adduct of a diboron compound with base adsorbed on the positively charged Cu sites to form the corresponding borylation product.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 33
·80817-80827
·
IF 5.8
Huang Guofu,Wang Mianmian,Sun Xinying,Liu Haijian,Liu Fangfang
In this work, pomegranate peel extracts were used as the green reducing agent to synthesize Cu/Fe nanoparticles (P-Cu/Fe nanoparticles) and removed tetrabromobisphenol A (TBBPA) in aqueous solution. P-Cu/Fe nanoparticles were amorphous and irregularly spherical. The surfaces of nanoparticles contained Fe 0 , Fe 3+ oxides (hydroxides), and Cu 0 . The bioactive molecules from pomegranate peel were extremely important for the synthesis of nanoparticles. P-Cu/Fe nanoparticles had excellent removal performance for TBBPA, and 98.6% of TBBPA (5 mg L −1 ) was removed within 60 min. The removal reaction of TBBPA by P-Cu/Fe nanoparticles was well-fitted with the pseudo-first-order kinetic model. The Cu loading was critical for TBBPA removal with an optimum value of 1.0 wt%. A weakly acidic condition (pH 5) was more favorable for the removal of TBBPA. The removal efficiency of TBBPA increased with the rise of temperature and decreased with increasing initial TBBPA concentration. The activation energy ( E a ) was 54.09 kJ mol −1 , indicating that the removal of TBBPA by P-Cu/Fe nanoparticles was mainly surface-controlled. Reductive degradation was the main mechanism of TBBPA removal by P-Cu/Fe nanoparticles. In conclusion, green synthesized P-Cu/Fe nanoparticles using pomegranate peel waste show great potential for the remediation of TBBPA in aqueous solution.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yi Yang,Minyi Liu,Xintong You,Ying Li,Haowen Lin,J. Paul Chen
Treatment of organic wastewater is of great importance and can be carried out by catalysis technologies such as catalytic wet peroxide oxidation (CWPO). A novel bimetallic Fe-Cu-CNT catalyst was first developed by a facile hydrothermal method; Fe species (Fe (Ⅱ) and Fe (Ⅲ)) and Cu species (Cu (Ⅰ) and Cu (Ⅱ)) were used to fabricate the catalyst with the CNTs, which was stable during testing. Methylene blue (MB) was chosen as model compound for the study; the optimization for treatment by the Box-Behnken design indicated that a combination of low pH, high MB concentration and intermediate temperature led to better treatment performance. The CWPO reaction obeyed the 2 nd -order kinetic equation and the catalyst activity increased with an increase in the Cu content. The reaction induction period was shortened with decreasing Fe:Cu ratio. The cycling reaction between Fe 3+ /Fe 2+ and Cu 2+ /Cu + pairs generated a large number of oxidative radicals and improved the pollutant degradation efficiency. Finally, the reaction rate equation of CWPO over Fe-Cu-CNT was derived, and it was experimentally illustrated that hydroxyl radicals played a crucial role in the treatment. This study demonstrates that the optimized Fe-Cu-CNT has great potentials for treatment of organic wastewater with higher efficiency and lower cost.
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高影响因子
Journal of Materiomics
·
2020
·
IF 5.797
Xinrui He,Yalin Hu,Hanqing Tian,Zhipeng Li,Pei Huang,Jing Jiang,Chao Wang
For pursing high-performance supercapacitors, both of the design strategy and structural characteristic of electrode materials are crucial. Herein, we report the in-situ growth of flexible self-assembled 3D hollow tubular Cu 2 S nanorods on Cu foam substrate (Cu 2 S@Cu). The Cu substrate is simultaneously acted as a copper source and a collector, which reduces the contact resistance. Moreover, the highly ordered 3D unique structure increases the redox reactive sites and enhances the ion transmission effectively, resulting in greatly improved electrochemical performance. Based on the Cu 2 S@Cu electrode, the supercapacitor exhibits high areal capacitance of 1000 mF cm −2 at a current density of 2 mA cm −2 , and great cycle stability, maintaining 96.9% capacitance after 10,000 cycles. Furthermore, the supercapacitor also shows an excellent flexibility with no significant decrease in the twisting or bending state. The capacity retention rates are 99.8% and 86.1%, respectively, and finally recover to 99.3%, confirming its great potential in practical application for portable electronic devices.
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高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jiayu Feng,Fei Wang,Chi Wang,Kai Li,Xin Sun,Ping Ning
In this study, an NH3 plasma-treated Cu/HZSM-5 sorbent was introduced to simultaneously remove H2S and PH3 in low-temperature and low-oxygen environments. The effects of the Cu loading amounts, modification methods, and plasma-treatment conditions on the adsorption–oxidation performance of the sorbents were investigated. From the performance test results, the sorbent treated by NH3 plasma with the specific energy input (SEI, electrical input energy to the unit volume of gas) value of 1 J·mL–1 (Cu/HZSM-5-[S1]) was identified as having the highest breakthrough capacities of 108.9 mg S·g–1 and 150.9 mg P·g–1 among all of the materials tested. After three times of regeneration, the sorbent can still maintain the ideal performance. The results of Fourier transform infrared (FT-IR) spectroscopy and CO2 temperature-programmed desorption (CO2-TPD) indicated that the NH3 plasma treatment can introduce amino groups (functional groups) onto the sorbent surface, which greatly increases the number and strength of the basic sites on the sorbent surface. Results of N2 adsorption/desorption isotherms and scanning electron microscopy–energy dispersive spectroscopy (SEM–EDS) showed that the morphology of the sorbent changed after the plasma treatment, which exposed more active sites (copper species). In situ IR spectra showed that the amino groups are continuously consumed during the reaction process, indicating that these amino groups can help sorbents to capture gas molecules. Moreover, X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses indicated that CuO is the main active species and the consumption of CuO and accumulation of the reaction products on the surface and inner pores of the sorbent are the primary reasons for the deactivation of the sorbent.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2018
·
IF 3.525
Yu Zhang,Chenliang Ye,Cuili Guo,Changna Gan,Xinmeng Tong
A series of indium oxide-modified Cu/SiO 2 catalysts were synthesized and used to produce ethanol via methyl acetate hydrogenation. In-Cu/SiO 2 catalyst containing 1.0 wt% In 2 O 3 exhibited the best catalytic activity and stability. The physicochemical properties of the synthesized catalysts were investigated using several characterization methods and the results showed that introducing suitable indium to Cu/SiO 2 increased the copper dispersion, diminished the copper crystallite size, and enriched the surface Cu + concentration. Furthermore, the Cu/SiO 2 catalyst gradually deactivated during the stability test, which was mainly attributed to copper sintering and the valence change in surface copper species. In contrast, indium addition can inhibit the thermal transmigration and accumulation of copper nanoparticles to stabilize the catalyst.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Qiao Wang,Wei Wang,Boyin Yan,Wenxin Shi,Fuyi Cui,Ce Wang
The present development gives an insight into the effect of the distribution of bimetallic sites in denitrification. A highly-dispersed Pd-Cu bimetallic catalyst supported by titanium dioxide nanofibers (Pd-Cu/TiO 2 ) was in situ fabricated by electrospinning and subsequent calcination and chemical reduction, and then applied in the catalytic reduction of water phase nitrate (NO 3 − ) to nitrogen gas (N 2 ). Compared with ex situ Pd-Cu impregnated catalyst, the in situ Pd-Cu/TiO 2 nanofibers exhibited the high nitrate removal efficiency, selectivity and fast kinetics (about twice that of impregnated ones). These good catalytic performances are mainly benefited from increased active sites and raised ratio of nitrogen to hydrogen on them, which are brought about by the well-dispersed and closely connected Pd-Cu bimetallic nanoparticles in TiO 2 nanofiber matrix. Moreover, the in situ nanofiber matrix provides a physical barrier to inhibit bimetallic nanoparticles movement, aggregation and leakage from the support into water, and hence significantly enhances the recyclability for nitrate reduction.
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高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Zhuo Zhang,Liying Tian,Hongyu Zhang,Hai Xu,Panpan Dong,Yayun Zhang,Donghui Long
Solid-state lithium batteries using solid composite polymer electrolytes (CPEs) with great thermal and mechanical stabilities are believed to be the next-generation advanced electrochemical devices, but they suffer from low ionic conductivity at room temperature and a poor interface between the electrode and the electrolyte. Herein, we present a poly(ethylene oxide) (PEO)-based CPE allowing rapid Li+ migration enabled by coordinating the anions on the exposed metal sites of a metal–organic framework (MOF). The CPE contains MOF-74 fillers, a PEO matrix, and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). Owing to the strong anchoring effect of MOF-74 fillers on TFSI– verified by calculations and measurements, the CPE exhibits a high ionic conductivity (5.5 × 10–5 S·cm–1 at 30 °C), a wide electrochemical stability (4.8 V), and an improved Li+ transference number (0.36). Besides, the adjusted local current density promotes the interfacial stability against the Li anode in a Li symmetric battery, which performed well at a current density of both 0.2 and 0.4 mA cm–2. With these advantages, the all-solid-sate LiFePO4 battery fabricated exhibited stable cycling performances (161 mA h g–1 and maintained 152 mA h g–1 after 300 cycles at 0.5 C). This strategy gives fresh reference to the utilization of different MOFs and polymers in building high-performance solid-state lithium batteries.
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高影响因子
WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 7
·1-13
·
IF 2.9
Chen Sheng nan,Gao Ying jun,Ming Hao,Ren Long long,Geng Cong,Shen Xin jun,Shen Chen guang,Guan Yin yan,Gao Wei chun
Non-thermal plasma (NTP) co-catalytic technology is a waste gas treatment technology with high energy efficiency and little by-product. Catalyst plays an important role in the process of NTP co-catalytic degradation of contaminants. However, the performance of the catalyst is not only directly related to active center but also closely related to carrier. In this study, we successfully prepared stable Cu-doped catalysts with bicontinuous structure, using Cu(NO 3 ) 2 , Al(NO 3 ) 3 , and tetramethoxysilane as precursors through sol–gel process accompanied by phase separation. Scanning electron microscopy (SEM), energy dispersion X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), temperature programmed desorption (TPD), Brunauer–Emmett–Teller method (BET), and mercury intrusion porosity (MIP) were used to investigate the structure, properties, and the role of Al. It was found that in this Cu-doped system, addition of Al can produce Brønsted acidic sites and facilitate the divalent Cu dope into neutral Si skeleton to form stable complexes. Then, it was used as catalyst in NTP system to study the performance of the system and degradation mechanism of H 2 S. When binary metal catalyst was used, synergistic NTP system creates a secondary electron emission to enhance the field strength, 20 mg·m −3 H 2 S has the best degradation efficiency, and Cu-doped catalysts can cyclic utilization. At the same time, selective oxidation occurs in the system; elemental sulfur is produced.
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高影响因子
ADVANCED POWDER TECHNOLOGY
·
2019
·
IF 3.25
Yuting Chu,Muhammad Asim Khan,Fengyun Wang,Mingzhu Xia,Wu Lei,Sidi Zhu
Arg-Mt, was fabricated by modifying sodium montmorillonite (Na-Mt) with Arginine monohydrochloride (Arg salt), to adsorb Pb(II) and Cu(II) in aqueous solution. The X-ray powder diffraction (XRD), Fourier transform infrared (FTIR) spectrum, thermal analysis (TG/DTG), Brunauer-Emmett-Teller (BET) and Scanning electron microscope (SEM) were employed to investigate the properties of Na-Mt and Arg-Mt. The effects of the amount of modifier, pH value, the initial concentration of M(II), temperature and contact time were tested in a single adsorption system. The isotherm model was well matched with the Langmuir curve and the kinetic adsorption fitted well with the pseudo-second-order rate equation. The saturated adsorption of Pb(II) and Cu(II) by Arg-Mt were 124.69 and 29.15 mg/g, respectively, which were higher than that of Na-Mt (89.08 and 23.93 mg/g). The thermodynamic equation indicated that the adsorption process was spontaneous, endothermic, and the randomness of the samples changed a little after adsorption. The adsorption capacity of heavy metal ions in the binary co-adsorption system was poor than single adsorption system. Furthermore, the adsorbed M(II) onto Arg-Mt can hardly be dissolved under weak acidic condition (pH > 4) according to the desorption experiments. High-efficiency and low-cost make Arg-Mt to be used in the removal of heavy ions in aqueous solution.
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高影响因子
JOURNAL OF POLYMER RESEARCH
·
2013
·Vol. 21
·期 1
·1-13
·
IF 2.019
Li Xing-Jian,Sun Dao-Xing,Zhang Yi-Heng
The Cu(I)-mediated azide–alkyne cycloaddition reaction, “click” chemistry, has been used to functionalize the waterborne polyurethane, by which a novel fluorinated waterborne polyurethane (FWPU) was synthesized. FWPU was confirmed by FT-IR and 1 H NMR. The structure and properties of FWPU were characterized by water contact angle, water absorption, surface energy, scanning electron microscope (SEM) equipped with energy dispersive X-ray spectrometry (EDS), thermogravimetric analysis (TGA) and X-ray diffraction (XRD), etc. From the research of the surface properties, it was found that the modified materials were endowed with a remarkable hydrophobicity and stain resistance. SEM results showed that the micro-phase separation of FWPU became increasingly apparent with the rise of fluorinated side chains in polyurethane backbone. XRD measurements reflected that the crystallinity of FWPU tended to decrease firstly and then increase with the change of fluorine content. TGA results demonstrated that FWPU possessed flame retardant performance to a certain extent due to the incorporated alkyne groups in the FWPU to improve the final char strongly.
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高影响因子
危险品化学品经营许可证（带存储）