International Journal of Environmental Research and Public Health
·
2019
·Vol. 16
·期 8
·1439
·
IF 2.468
Yue Teng,Ke Yao,Wenbin Song,Yongjun Sun,Haoliang Liu,Zhiying Liu,Yanhua Xu
Cu-Mn-Ce@γ-Al2O3was prepared by incipient wetness impregnation and used to catalyze ozonation in a coal chemical wastewater-biotreated effluent. The preparation factors that considerably affected the catalytic performance of Cu-Mn-Ce@γ-Al2O3, specifically metal oxide loading percentage, calcination temperature, and calcination time, were examined. The catalyst was characterized by scanning electron microscopy, energy dispersive spectrometry, X-ray diffraction, and Brunauer-Emmett-Teller analysis. The optimal catalytic ozonation operating parameters, such as ozone dosage, catalyst dosage, pH, and reaction time, were also investigated. Results showed that an optimized catalyst consisted of 17.0% CuO, 3.0% MnO2, and 2.0% CeO2(wt.%). The optimal calcination temperature and calcination time were 600 °C and 5 h. The optimal catalytic ozonation operating parameters, including ozone dosage, catalyst dosage, pH, and reaction time, were 7, 80.0 mg/L, 20.0 mg/L, 7 and 50 min, respectively. The COD removal of biotreated effluent increased to 61% under these optimal operating conditions. Meanwhile, ozonation alone resulted in only 20% removal. This work proposes the use of easily available Cu-Mn-Ce@γ-Al2O3catalyst and might drive the advancement of catalytic ozonation for chemical wastewater purification.Keywords:catalyst;catalytic ozonation;coal chemical wastewater;advanced treatment
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高影响因子
MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 7
·1-12
·
IF 5.3
Gu Yaohong,Li Qiulan,Yang Dezhi,Yang Yaling
A phosphomolybdate nanozymes doped with copper and iron particles (Cu,Fe-PMs) with excellent peroxidase (POD)-like activity was prepared by one-step microwave digestion method. It can oxidize the positively charged substrates such as 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H₂O₂, resulting in the formation of a blue compound. It is noteworthy that the POD-like activity of Cu,Fe-PMs was significantly boosted upon the incorporation of sodium dehydroacetate (DHA). This was attributed to the formation of complex between the Cu,Fe-PMs and DHA. On the one hand, DHA enhances the affinity of Cu,Fe-PMs for the substrate and exhibits superior catalytic properties. On the other hand, DHA also accelerated the valence state transformations between Fe 3+ /Fe 2+ and Cu + /Cu 2+ , increased catalytic active sites and facilitate the generation of more reactive oxygen species (ROS) such as •OH with strong oxidation. Therefore, the current study successfully established a highly sensitive and reliable colorimetric sensor for detecting the DHA content in foods. The results indicated that the absorbance at 652 nm exhibited a linear relationship with DHA concentration within the range of 0.0017—2.5 μg mL −1 , achieving a minimum limit of detection (LOD) as low as 0.83 ng mL −1 . The sensor was successfully applied to detect DHA in actual samples, with recoveries ranging from 91.59% to 103.35% and a relative standard deviation (RSD) not exceeding 3.64%. This demonstrates the reliable performance and consistent reproducibility of the analytical approach. Graphical
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Mengjie Cao,Shuangde Li,Shikun Wang,Xin Zhou,Guangxin Ma,Yunfa Chen
The catalytic decomposition of CH4 offers a promising route to obtain pure H2, which is significant for mitigating greenhouse gas emissions and enhancing methane utilisation. Nickel-based catalysts are the most prevalent for methane cracking. However, catalyst deactivation can occur due to coking and sintering. Therefore, stabilising the active sites of Ni-based catalysts by enhancing metal–support interactions is essential for designing methane cracking catalytic systems. This study investigates the effects of adding Co, Cu and Zn on the performance of a hydrotalcite-derived NiCrAl catalyst. The results showed that Cu increased the specific surface area, decreased the electron density around Ni atoms, facilitated the reduction of NiO, and produced strong interactions between the metal and support. This improved methane decomposition at the Ni active sites and enhanced catalytic stability. The strong interaction between the metal and support suppressed nickel sintering during methane cracking. The Ni2.4Cu0.3Cr0.3Al catalyst retained 50% H2 yield for 400 min at 650 °C. Online mass spectrometry analysis demonstrated that the catalyst did not generate CO and CO2 during the methane cracking reaction. XRD and TEM results showed that Cu maintained the balance between CH4 dissociation and carbon diffusion by stabilising the size of nickel, promoting the transition of deposited carbon from carbon particles to carbon nanotubes. This work provides a reference for designing high-performance nickel-based catalysts for methane cracking.
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WATER RESEARCH
·
2019
·
IF 7.913
Wei Xiang,Tao Zhou,Yifan Wang,Mingjie Huang,Xiaohui Wu,Juan Mao,Xiejuan Lu,Beiping Zhang
This study has demonstrated that hydroxylamine (HA) could greatly enhance Cu nanoparticles (nCu) in activating molecular oxygen and significantly elevate the diclofenac (DCF) degradation rate about two orders of magnitude in neutral circumstances. Effects of several important parameters on the DCF degradation such as nCu loading, HA dosage, pH and reaction temperature were investigated in the nCu/HA/O 2 system. Multiple examinations revealed that the reactive Cu(III) species instead of OH• would be predominant in the nCu/HA/O 2 system, despite their similar DCF degradation pathways. Based on a HA-enhanced copper cycle depending on the pristine Cu 0 @Cu(I) (hydro)oxides core-shell structure, the heterogeneous-homogeneous reaction mechanism was proposed. It included solid-liquid interfacial and bulk reactions, e.g. heterogeneous activation of O 2 by Cu(I) to produce H 2 O 2 and homogeneous Cu(I)-catalytic generation of Cu(III) from H 2 O 2 . Further quantitative investigation of the main reactive species in the cycle revealed that the Cu(I) regeneration instead of the O 2 activation would be rate-limited. Besides, nCu could be recycled to effectively degrade DCF in four consecutive cycles in the raw neural nCu/HA/O 2 system. It suggested that the nCu/HA/O 2 system with a more efficient copper cycle would be a good alternative Fenton-like system in treating neutral recalcitrant organic wastewaters.
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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.
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CELLULOSE
·
2018
·Vol. 25
·期 10
·5831-5842
·
IF 3.809
Zhang Yan-Jie,Ma Xiao-Zhou,Gan Lin,Xia Tao,Shen Jun,Huang Jin
Abstract Fluorescent cellulose nanocrystals (fCNCs) have shown a great potential as optical probe for the applications of bioimaging or metal ion detection. In this work, by a controllable esterification strategy, the cellulose nanocrystal (CNC) surface was modified with ethylenediaminetetraacetic dianhydride (EDTAD) to achieve highly carboxylation degree, and, meanwhile, keep surface integration and crystalline structure in comparison with the TEMPO oxidation method. Then, the controllability of carboxylation degree was applied to produce a series of fCNCs with various conjugating densities of fluorescent 7-amino-4-methylcoumarin (AMC). The steric effect of AMCs on the fCNC surface could inhibit self-quenching, resulting in a more stable fluorescence intensity independent upon the change of fCNC concentration and a relatively high quantum efficiency in the solid state. Moreover, the fluorescence signals of fCNC can be selectively affected by Cu 2+ , and even high Cu 2+ concentration resulted in the visualized color change from blue to purple under ultraviolet radiation. Hence, two linear correlations with the Cu 2+ concentration, i.e. the fluorescence attenuation ratio at 390 nm in 0.5–16 ppm of Cu 2+ concentration and the fluorescence intensity ratio of 440 nm versus 390 nm in 16–160 ppm of Cu 2+ concentration, contributed to a potential of quantitative Cu 2+ detection. Especially, the on–off behavior of the fCNC fluorescence at the critical Cu 2+ concentration of 0.5 ppm was well consistent with the requirement of the Guideline of Drinking-Water Quality (GDWQ) administrated by World Health Organization (WHO), and hence might be used to rapid and visualized evaluation of drinking water quality. This work provides a new fluorescent nanomaterial that can be used in metal ion detection. Furthermore, the nontoxicity, biodegradability and environment-friendliness of cellulose nanocrystals might also contribute to the additional advantages for the application of environmental surveillance. Graphical abstract
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CATALYSIS LETTERS
·
2018
·Vol. 148
·期 8
·2348-2358
·
IF 2.911
Lin Jin,Guo Yafei,Li Changhai,Lu Shouxiang,Chen Xiao,Liew Kim Meow
A series of supported and bulk Cu–Mn–Ce ternary oxide catalysts was synthesized by wet-impregnation (IM), deposition–precipitation (DP), traditional co-precipitation (CP), co-precipitation with cetyltrimethyl ammonium bromide (CC), and sol–gel (SG) methods. The supported catalysts (CuMn/Ce-IM, CuMn/Ce-DP) exhibited significantly higher activity for CO oxidation than the bulk catalysts (CuMnCe-CP, CuMnCe-CC and CuMnCe-SG). The improved performance could be attributed to the presence of more isolated CuO and MnO x entities on the surface of supported catalysts, which contributed to the efficient utilization of both lattice oxygen from CeO 2 and spillover oxygen from surface MnO x . For bulk catalysts, major Cu–Mn species were doped to form \({\text{C}}{{\text{u}}_{\text{x}}}{\text{M}}{{\text{n}}_{\text{y}}}{\text{C}}{{\text{e}}_{1 - {\text{x}} - {\text{y}}}}{{\text{O}}_{2 - {\text{z}}}}\) solid solutions and a part of them were coated by ceria mechanically. Lowest 50% CO conversion temperature were achieved at 76.9 °C for CuMn/Ce-IM catalyst. Low-temperature CO oxidation activities of all catalysts were in the sequence of CuMn/Ce-IM > CuMn/Ce-DP > CuMnCe-SG > CuMnCe-CC > CuMnCe-CP. Graphical Abstract
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Ting Chen,Zhiliang Zhu,Zeyu Wang,Hua Zhang,Yanling Qiu,Daqiang Yin,Guohua Zhao
To develop an efficient catalyst with novel structure and limited metal release for enhanced PMS activation, a 3D hollow sphere like Cu-incorporated LaAlO 3 perovskite was synthesized based on soft chemical process with template-free. It was evaluated as the heterogeneous catalyst firstly to activate peroxymonosulfate (PMS) for the oxidative degradation of several typical pharmaceuticals in water. The mechanism study indicated a coaction of electron transfer and oxygen defects in this system. The obtained catalyst can promote electron transfer efficiency of Cu + /Cu 2+ cycle and provide abundant oxygen defects for catalytic oxidation, which is responsible for the generation of OH, SO 4 − and 1 O 2 . These active species played crucial roles in efficient degradation of thiamphenicol (TAP), diclofenac sodium (DCF), ibuprofen (IBF) and paracetamol (PR), achieving more than 95% removal within 30 min. The catalyst kept high removal efficiency over pH range from 5.0 to 9.1 and suppressed copper leaching in reaction process. Besides, the catalyst exhibited good performance for TAP degradation and mineralization in raw water matrixes from Taihu Lake Basin, which showed a possible practical application to the remediation of water pollution.
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FUEL
·
2021
·
IF 6.609
Yuewen Shao,Qingyin Li,Xinyi Dong,Junzhe Wang,Kai Sun,Lijun Zhang,Shu Zhang,Leilei Xu,Xiangzhou Yuan,Xun Hu
The production of γ-valerolactone (GVL) receives increasing attention due to its extensive applications as a promising fuel and fuel additive. In this study, the direct conversion of biomass-derived furfural to GVL with a unprecedent yield of 90.5% was achieved via consecutive hydrogenation and acid-catalyzed reactions over CuAl for hydrogenation and a co-catalyst (i.e. H-ZSM-5) for acid-catalysis in ethanol. The relative abundance of the hydrogenation sites and acidic sites determines the reaction network and the transfer of the main products from furfuryl alcohol (FA) to ethyl levulinate (EL) or GVL, as the acidic sites, especially the Brønsted acidic sites, not only catalyze the formation of EL from FA, but also affect the hydrogenation activity of CuAl. However, the Lewis acidic sites facilitate the opening ring of FA to 1,4-pentanediol, preventing the GVL formation. The acid catalyst and hydrogenation catalyst deactivate via varied mechanisms in the conversion of furfural to GVL, which is required to be considered in the further development of the robust catalysts.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Mingyue Xie,Yong Wu,Hao Gu,Yuhao Peng,Shan Zhang,Feng Ryan Wang,Wei Xiao,Dong Gu
Deuterated compounds have broad applications across various fields, with dehalogenative deuteration serving as an efficient method to obtain these molecules. However, the diverse electronic structures of active sites in the heterogeneous system and the limited recyclability in the homogeneous system significantly hinder the advancement of dehalogenative deuteration. In this study, we present a catalyst composed of copper single-atom sites anchored within an ordered mesoporous nitrogen-doped carbon matrix, synthesized via a mesopore confinement method. The Cu1/OMNC-1100 catalyst, characterized by Cu–N4 sites, demonstrates exceptional performance, high functional group tolerance, and remarkable durability in the deuteration of 2-bromo-6-methoxynaphthalene under relatively mild conditions (80 °C, 2 MPa of CO). Experimental results combined with X-ray absorption fine structure analysis reveal that Cu–N3 sites can be converted into more stable Cu–N4 counterparts at higher pyrolysis temperatures, resulting in enhanced catalytic activity. This work demonstrates a strategy for designing single-atom site catalysts with tunable coordination environments, providing a promising approach to improving catalytic performance in selective dehalogenative reactions under relatively mild conditions.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Jinjing Du,Yu Zhou,Xinhai Liu,Xinxin Cui,Xuan Zhang,Bin Wang,Xiao Feng,Jun Zhu,Heng Zuo,Qian Li,Xihong He,Ping Hu
The development of a hydrogen evolution catalyst with both catalytic activity and stability is critical for hydrogen production from electrolytic water. Herein, a V-based porous alloy was prepared via high-energy ball milling and solid-state sintering. Then, the V-based porous alloy was modified with a Ni-Cu-Mo ternary alloy coating by direct current electrodeposition to obtain a composite hydrogen evolution cathode with high hydrogen evolution activity. The substrate has a certain hydrogen storage capacity combined with a high-activity Ni-Cu-Mo coating. The composite hydrogen evolution cathode exhibited high electrocatalytic activity toward the HER. It can afford a lower overpotential of 93 mV and a smaller Tafel slope of 97.4 mV/dec with a current density of 10 mA/cm 2 in 1.0 M KOH. The composite hydrogen evolution cathode demonstrated outstanding stability after 2000 cycles and good durability after intermittent electrolysis for 20 h. Hydrogen protons can protect the components of the cathode composite from dissolution during discontinuous constant potential electrolysis. The composite hydrogen evolution cathode also exhibited a strong catalytic capacity for hydrogen evolution during intermittent electrolysis under alkaline conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yanhu Han,Zhaowei Jia,Wenxue Gong,Xuechun Wei,Yu Zhang,Mengying Tao,Yaofei Ren,Zuyi Lu,Yutong Wu,Jianhua Chen,Zhongfeng Shi,Zhenxia Zhao,Zhongxing Zhao
Developing photocatalysts with high activity and selectivity remains a significant challenge in the field of CO 2 photoreduction for producing valuable chemical or fuel products under mild conditions. Herein, photonic crystal (PC) GDY-Cu/ZnO was constructed through the in-situ induced growth of graphdiyne (GDY) on PC Cu/ZnO surface via H 2 -reduction for efficient photoreduction of CO 2 to CH 4 . With the aid of photonic crystal structure, PC GDY-Cu/ZnO exhibits a distinctive red-edge slow light region which can significantly improve the utilization efficiency of visible light and intensify photo-catalysis. Additionally, the formed all-solid-state Z-scheme system efficiently accelerates photoelectron migration, facilitating e - /h + separation. Thirdly, the surface GDY, along with the enrich oxygen vacancies generated during H 2 reduction, enhances the adsorption and activation toward CO 2 and H 2 O on PC GDY-Cu/ZnO interface. In consequence, PC GDY-Cu/ZnO demonstrates highly photocatalytic conversion of CO 2 to CH 4 , achieving a CH 4 yield of 33.67 μmol·g −1 ·h −1 with 93.3 % selectivity via slow-light-driven photocatalysis CO 2 reduction. This work provides an efficient strategy to modify ZnO for the efficient photoreduction of CO 2 to CH 4 .
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