ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Tingting Yu,Lei Tao,Zhiyi Liu,Xuge Zhang,Tao Gan,Wensheng Yan,Lirong Zheng,Ge Meng,Wei Chen,Shoujie Liu,Chenliang Ye,Jian Zhang
Unique active sites make single-atom (SA) catalysts promising to overcome obstacles in homogeneous catalysis but challenging due to their fixed coordination environment. Click chemistry is restricted by the low activity of more available Cu(II) catalysts without reducing agents. Herein, we develop efficient, O-coordinated SA Cu(II) directly catalyzed click chemistry. As revealed by theoretical calculations of the superior coordination structure to promote the click reaction, an organic molecule-assisted strategy is applied to prepare the corresponding SA Cu catalysts with respective O and N coordination. Although they both belong to Cu(II) centers, the O-coordinated one exhibits a 5-fold higher activity than the other and even much better activity than traditional homogeneous and heterogeneous Cu(II) catalysts. Control experiments further proved that the O-coordinated SA Cu(II) catalyst tends to be reduced by alkyne into Cu acetylide rather than the N-coordinated catalyst and thus facilitates click chemistry.
研究领域:
化学
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催化
·
材料科学
✓ 已验证
DOI
高影响因子
Arabian Journal of Chemistry
·
2022
·
IF 6.212
Run Yuan,Yihe Qin,Can He,Zichen Wang,Lu Bai,Hong Zhao,Zijian Jiang,Lingyao Meng,Xuwen He
It is important to develop a catalyst that has high catalytic activity and can improve the degradation efficiency of refractory organic pollutants in the catalytic ozonation process. In this study, Fe-Mn-Cu-Ce/Al 2 O 3 was synthesised via impregnation calcination for catalytic ozonation of bio-treated coking wastewater. The physical and chemical characteristics of the catalysts were analysed using X-ray diffraction (XRD), X-ray fluorescence spectrometry (XRF), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and Brunauer–Emmett–Teller nitrogen adsorption–desorption methods. The effects of catalyst dosage, pH, and reflux ratio on the degradation efficiency of wastewater were examined in laboratory-scale experiments. The chemical oxygen demand (COD) removal rate of bio-treated coking wastewater was estimated to be 52.76 % under optimal conditions. The experiments on the catalytic mechanism demonstrated that the surface hydroxyl formed by the Lewis acid sites on the surface of the catalyst can react with ozone as the active site forming the active oxygen (·OH, ·O 2 – , and 1 O 2 ), thereby efficiently degrading the organic pollutants in coking wastewater. Furthermore, a pilot-scale experiment on the catalytic ozonation of bio-treated coking wastewater was carried out using an Fe-Mn-Cu-Ce/Al 2 O 3 catalyst, while the effects of the initial pollutant concentration, ozone concentration, and gas flow on the COD removal rate were studied on a pilot scale. It was found that the COD removal rate of the wastewater was ∼ 60 % under optimal parameters. After the treatment, the wastewater steadily reached the coking wastewater discharge standard (COD < 80 mg/L), while the operating cost of catalytic ozonation reached ∼ 0.032$/m 3 , thereby paving the way toward economic engineering applications. The COD degradation kinetics in the bio-treated coking wastewater followed pseudo-second-order kinetics. Three-dimensional fluorescence and gas chromatography–mass spectrometry revealed that macromolecular organic pollutants in the bio-treated coking wastewater were greatly degraded. In summary, Fe-Mn-Cu-Ce/Al 2 O 3 exhibited good reusability, high catalytic activity, and low cost and has a wide application prospect in the treatment of coking wastewater.
研究领域:
环境科学
·
催化材料
✓ 已验证
DOI
高影响因子
CRYSTENGCOMM
·
2020
·Vol. 22
·期 23
·4005-4013
·
IF 3.117
Baolin Liu,Yizhao Li,Shaojun Qing,Kun Wang,Jing Xie,Yali Cao
Highly dispersed surface Cu species and oxygen vacancies are important for CuOx–CeO2 catalysts in many reactions, but it is difficult to increase the concentrations of highly dispersed Cu species and oxygen vacancies simultaneously by only adding a Cu component. Herein, CuOx–ZrO2–CeO2 (CZC) nanocatalysts with different ratios of Cu/Zr have been effectively produced by a simple solvent-free synthetic strategy. The effect of Zr doping on the structure and reactivity of the CuOx–CeO2 catalysts has been investigated with the help of carbon monoxide (CO) oxidation and 4-nitrophenol (4-NP) reduction as model reactions. It is revealed that the introduction of Zr relieved the agglomeration of surface Cu species, produced more oxygen vacancies in the interior and Cu+ species on the surface of the catalyst, and increased the reducibility of CuOx–CeO2. The CZC catalysts show remarkably enhanced catalytic activity due to the abundant surface active sites and the improved redox properties provided by the suitable doping of Zr into CuOx–CeO2. This work not only offers a practicable way to reconstruct the distribution of active metals on the metal oxide support but also provides a high-efficiency strategy to prepare oxide catalysts with excellent catalytic performance.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2019
·Vol. 411
·期 17
·3801-3810
·
IF 3.286
Huang Yuanlin,Liang Guangzhao,Lin Tianran,Hou Li,Ye Fanggui,Zhao Shulin
The convenience of colorimetric sensors is useful for practical applications. In this work, we constructed a novel colorimetric sensor with magnetic separation ability that can be operated in nearly neutral conditions and achieve one-step detection of metabolites. Magnetic Cu doped Fe 3 O 4 @FeOOH magnetic nanocomposite (Cu/Fe 3 O 4 @FeOOH) with an oxygen vacancy was prepared by a one-step self-assembly hydrothermal method, and fully characterized by different methods. The oxygen vacancy generated by the incorporation of Cu 2+ cations into the Fe 3 O 4 @FeOOH structure was confirmed to be a vital reactive site for enhancing the catalytic activity, which opens up a new way of designing highly efficient enzyme mimics. Benefiting from its inherent horseradish-peroxidase-like activity, a simple and selective enzyme-based colorimetric sensor was developed for one-step detection of H 2 O 2 and cholesterol, and 3,3′,5,5′-tetramethylbenzidine was catalyzed by H 2 O 2 to generate a colored product of oxidized 3,3′,5,5′-tetramethylbenzidine for signaling. H 2 O 2 and cholesterol can be linearly detected in the same range from 0.01 to 0.4 mmol L -1 with detection limits of 0.0075 mmol L -1 and 0.0082 mmol L -1 , respectively. The proposed colorimetric sensor has satisfactory reusability, accuracy, and practicability in human serum samples, indicating its potential application for the detection of different metabolites in the fields of life science and analytical science.
Graphical abstract
研究领域:
分析化学
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生物传感
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材料科学
·
生命科学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2020
·Vol. 9
·期 3
·710-718
·
IF 5.344
Zhengdi Wang,Liyang Fu,Yu Zhu,Sa Wang,Guohong Shen,Lan Jin,Ruizheng Liang
The combination of chemodynamic therapy (CDT) with photothermal therapy (PTT) is an efficacious strategy in cancer treatment to acquire satisfactory therapy efficiency in the endogenous redox reaction and external laser induction. In this work, we have designed Ce doped Cu–Al layered double hydroxide (CAC-LDH) ultrathin them through a bottom-up synthesis method, and further loaded them with indocyanine green (ICG). The synthesized ICG/CAC-LDH was used as a Fenton-catalyst and photothermal agent. With the Fenton activity, the ICG/CAC-LDH nanosheets could decompose H2O2 and exhibit a low KM value (1.57 mM) and an ultra-high Vmax (4.88 × 10−6 M s−1) value. Due to the presence of oxidized metal ions, ICG/CAC-LDH could induce intracellular GSH depletion and reduce Cu2+ and Ce4+ to Cu+ and Ce3+, respectively. The generated Cu+ and Ce3+ further reacted with local H2O2 to generate toxic hydroxyl radicals (˙OH) via the Fenton reaction. Owing to the obviously enhanced absorption of ICG/CAC-LDH at 808 nm, the photothermal efficiency of ICG/CAC-LDH increased significantly compared with ICG (ΔT = 34.7 °C vs. 28.3 °C). In vitro studies substantiate the remarkable CDT/PTT efficacy, with complete apoptosis of HepG2 cancer cells (the cell viability is less than 2%) treated with 25 μg mL−1 of ICG/CAC-LDH. Furthermore, ICG/CAC-LDH could also act as a contrast agent for cancer magnetic resonance imaging (MRI) and photoacoustic imaging (PAI). These results demonstrate the potential of ICG/CAC-LDH as an integrated agent for dual-modal imaging and synergistic CDT/PTT.
研究领域:
纳米技术
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癌症治疗
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生物医学工程
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材料科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Zhang Minghao,Sun Chenxi,Chen Guanhong,Kang Yuanhong,Lv Zeheng,Yang Jin,Li Siyang,Lin Pengxiang,Tang Rong,Wen Zhipeng,Li Cheng Chao,Zhao Jinbao,Yang Yang
Rechargeable aqueous zinc-metal batteries, considered as the possible post-lithium-ion battery technology for large-scale energy storage, face severe challenges such as dendrite growth and hydrogen evolution side reaction (HER) on Zn negative electrode. Herein, a three-dimensional Cu-In alloy interface is developed through a facile potential co-replacement route to realize uniform Zn nucleation and HER anticatalytic effect simultaneously. Both theoretical calculations and experimental results demonstrate that this bifunctional Cu-In alloy interface inherits the merits of low Zn-nucleation overpotential and high HER overpotential from individual copper and indium constituents, respectively. Moreover, the dynamical self-reconstruction during cycling leads to an HER-anticatalytic and zincophilic gradient hierarchical structure, enabling highly reversible Zn chemistry with dendrite-free Zn (002) deposition and inhibited HER. Moreover, the improved interface stability featured by negligible pH fluctuations in the diffusion layer and suppressed by-product formation is evidenced by in-situ scanning probe technology, Raman spectroscopy, and electrochemical gas chromatography. Consequently, the lifespan of the CuIn@Zn symmetric cell is extended to more than one year with a voltage hysteresis of 6 mV. Importantly, the CuIn@Zn negative electrode is also successfully coupled with high-loading iodine positive electrode to fabricate Ah-level (1.1 Ah) laminated pouch cell, which exhibits a capacity retention of 67.9% after 1700 cycles.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
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.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
En-Hui Yuan,Meng Li,Ming-Hui Yang,Xiaosheng Huang,Kun Zhang,Weiliang Han,Zhicheng Tang,Zhong-Wen Liu
A direct hydrothermal synthesis strategy is developed to prepare the Cu–Fe-ZSM-5 zeolites by using the ethylenediaminetetraacetic acid disodium dihydrate (EDTA-2Na·2H 2 O) chelated Cu 2+ and Fe 3+ precursors as metal sources. During the crystallization, the metal chelates were spontaneously embedded into the ZSM-5 crystals and subsequently transformed to the zeolites encapsulated copper and iron species after removing the chelating agent via the high-temperature calcination . Rigorous characterizations indicate that the resulted Cu 2+ /Cu + and Fe 3+ /Fe 2+ species are formed ultra-small nano-composites with an average diameter of ∼2.2 nm and highly dispersed in the ZSM-5 zeolite crystals. The acidity of the ZSM-5 zeolites is subtly modulated by the encapsulated Cu–Fe nano-composite. As expected, the as-prepared Cu–Fe-ZSM-5 exhibits outstanding catalytic performance for the selective catalytic reduction of NO x with ammonia (NH 3 -SCR) in the broad reaction temperature ranges of 220–480 °C, which is much better than the Cu–Fe/ZSM-5 prepared with the conventional wetness impregnation method. Furthermore, the resultant zeolites show high stability and good tolerance to H 2 O and SO 2 , and it is very competitive for practical application to eliminate NO x . The developed one-pot hydrothermal synthesis route by using EDTA-2Na·2H 2 O as chelating agent is very convenient and easily reproducible, providing a general guideline to design and fabricate the superior transition metal modified zeolite catalysts for NH 3 -SCR and the related reactions.
研究领域:
催化
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Jinhua Lai,Feng Cheng,Shuolin Zhou,Sha Wen,Dongwen Guo,Wenguang Zhao,Xianxiang Liu,Dulin Yin
Nitrogen-containing polymer-supported Cu-doped MnO 2 (Cu-MnO 2 @PDVTA) nanowires were prepared and their catalytic performances were evaluated via oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). The Cu-MnO 2 @PDVTA catalysts were characterized by Fourier-transform infrared spectroscopy, X-ray diffraction, N 2 physical adsorption, transmission electron microscopy, and X-ray photoelectron spectroscopy. Both the Cu 2+ and MnO 2 nanoparticles were found to synergistically promote HMF oxidation to FDCA via 2,5-furandicarbaldehyde and 5-formyl-2-furancarboxylic acid intermediates. The Cu-MnO 2 @PDVTA-3 catalyst demonstrated the highest catalytic activity, providing FDCA with an excellent yield of 96.8% after 12 h at 80 °C. The time course of HMF oxidation revealed that oxidation of the hydroxyl group in HMF was easier than that of the aldehyde group. Cu-MnO 2 @PDVTA-3 could act as a reusable heterogeneous catalyst for HMF oxidation.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2017
·
IF 3.671
Yuvaraja Gutha,Yaping Zhang,Weijiang Zhang,Xu Jiao
Metal ions cause a serious public health problem. It is a great challenge to find an effective and efficient adsorbent to remove heavy metals from wastewater. Chitosan-based adsorbents are potential and effective for heavy metal ion removal. Hence a novel m-ECCSB was synthesized, characterized and utilized as an adsorbent for the removal of Cu(II) ions from aqueous solution. Various factors affecting the uptake behavior such as pH, adsorbent dosage, contact time, initial concentration of Cu(II) and temperature effect were investigated. Maximum adsorption capability (123.10 mg/g) was obtained at pH = 6, adsorbent dose of = 250 mg, rotational speed = 200 rpm, contact time = 60 min, and temperature of 323 K. The result of the kinetic study shows that the adsorption of Cu(II) could be described by the pseudo-second-order equation. Equilibrium data were analysed with the Langmuir, Freundlich and Dubinin-Radushkevich isotherms and Langmuir model was found to provide the best fit of the experimental data. The thermodynamic parameters showed that the adsorption of Cu(II) onto m-ECCSB was spontaneous (ΔG° = −8.990, −10.00 and −10.593 kJ/mol), endothermic (ΔH° = 15.674, 15.478 and 15.699 kJ/mol) and ΔS° (0.0814 J/mol K) suggests an increased randomness at the solid/solution interface under the studied conditions.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Hao Zhang,Junyan Wang,Minjie Liu,Di Liu
Cu/Al 2 O 3 catalyst was developed by a double hydrolysis precipitation. Over the Cu/Al 2 O 3 catalyst, a continuous mode of N-methylations of nitroarenes with methanol was successfully achieved under the exogenous base- and H 2 - free condition. Methylation process of nitroarenes could be controlled just by adjusting reaction conditions, affording the desired N-monomethylanilines or N, N-dimethylanilines, respectively. The characterization displayed that the double hydrolysis precipitation method made active metal Cu surface enrichment and high dispersion, meanwhile endow Cu/Al 2 O 3 with more developed pore system, which were responsible for the higher performance of our catalyst relative to Cu/Al 2 O 3 -CP. Compared with the reported batch mode, our procedure possessed the merits of low cost, environment-friendliness, better controllability and wide universality.
研究领域:
催化化学
·
绿色化学工程
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 150
·期 12
·3394-3401
·
IF 2.482
Qiao Chenxia,Jia Wenlan,Zhong Qiming,Liu Bingyu,Zhang Yifu,Meng Changgong,Tian Fuping
Abstract Novel Cu-nanoparticles (NPs) embedded in porous carbon materials (Cu@C-x) were prepared by one-pot pyrolysis of metal–organic frameworks (MOF) HKUST-1 at different temperatures. The obtained material Cu@C-x was used as a cost-effective catalyst for the hydrogenation of nitrobenzene using NaBH 4 as the reducing agent under mild reaction conditions. By considering the catalyst preparation and the catalytic activity, a pyrolysis temperature of 400 °C was finally chosen to synthesize the optimal catalyst. When the aromatic nitro compounds with reducible groups, such as cyano, halogen, and alkyl groups, were tested in this catalytic hydrogenation, an excellent selectivity approaching 100% was achieved. In the recycling experiment, a significant decrease in nitrobenzene conversion was observed in the third cycle, mainly due to the very small amount of catalyst employed in the reaction. Hence, the easily prepared and cost-effective Cu@C-400 catalyst fabricated in this study demonstrates potential for the applications in selective reduction of aromatic nitro compounds. Graphic Abstract The catalyst Cu@C-400 exhibited 100 % conversion and high selectivity for the hydrogenation of industrially relevant nitroarenes.
研究领域:
材料科学
·
化学工程
·
催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）