SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yu Guan,Guolang Zhou,Lin Li,Yexin Jiang,Jingzhou Yin,Cheng Liu,Lili Zhang,Qiaofeng Han,Edison Huixiang Ang
This research focused on creating oxygen vacancy-enriched copper-doped LaFeO 3 perovskite using a Prussian blue MOF template. This new material, LFO-Cu, showed outstanding Bisphenol A (BPA) degradation with 98 % efficiency in just 30 min, ten times faster than pure LaFeO 3 (LFO). Moreover, the LFO-Cu/peroxymonosulfate (PMS) system worked effectively at pH levels from 4 to 10, breaking down various pollutants (TC, PhOH, MV, MB), and removing 85 % TOC in BPA and 50 % in TC. Density Functional Theory (DFT) calculations revealed that copper strengthened the catalyst-PMS interaction, leading to the generation of highly reactive oxygen species (ROS), primarily singlet oxygen ( 1 O 2 ) and superoxide radicals (O 2 – ·). A degradation pathway was proposed, showing less toxic intermediates than BPA. In summary, copper-doped oxygen-rich vacancy MOFs-derived perovskite has significant potential for improving refractory organic mineralization.
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高影响因子
Journal of Environmental Chemical Engineering
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2026
·Vol. 14
·期 5
·125118
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IF 7.5
Jinzhuo Wang,Yonggang Zhang
Sulfurization-induced in situ surface reconstruction generates a Ni³⁺-rich NiOOH active phase for enhanced AOR activity. • Ni–Cu interaction optimizes interfacial electron transfer and promotes ammonia oxidation kinetics. • Cu/NF cathode promotes NO₃⁻/NO₂⁻ intermediate reduction and improves N₂ selectivity. • Anode–cathode synergistic catalysis integrates active phase reconstruction with intermediate regulation. • The integrated electrocatalytic system achieves > 98% NH₄⁺-N removal with high N₂ selectivity under mild conditions. Electrocatalytic ammonia oxidation (AOR) is a promising strategy for efficient ammonia removal and recovery; however, its practical application remains limited by sluggish reaction kinetics and low N₂ selectivity, while the structure–activity relationship between catalyst surface reconstruction and catalytic performance remains poorly understood. Herein, a sulfurization-modified NiCu layered double hydroxide (S-NiCu-LDH/NF) anode coupled with a Cu/NF cathode was rationally constructed to establish an anode–cathode synergistic electrocatalytic system for efficient NH₄⁺-N oxidation and selective nitrogen conversion. The optimized system achieved over 98% NH₄⁺-N removal within 90 min with an N₂ selectivity exceeding 82%. Electrochemical analyses reveal that sulfurization improves interfacial charge-transfer kinetics, while the Cu/NF cathode further facilitates electron transport through reduced charge-transfer resistance. XPS and Raman analyses suggest that sulfurization induces in situ surface reconstruction during electrolysis, accompanied by the formation of a Ni³ ⁺-rich NiOOH active phase. The reconstructed active phase is proposed to facilitate NH₃ activation and the adsorption and conversion of key reaction intermediates, thereby promoting multi-electron transfer during AOR. Meanwhile, the Cu/NF cathode promotes the electrochemical conversion of NO₂⁻ and NO₃⁻ intermediates, suppressing their accumulation and consequently improving N₂ selectivity through an anode–cathode synergistic process. Download: Download high-res image (232KB) Download: Download full-size image
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ACS Catalysis
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2026
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IF 13.6
Wang Kaixin,Dang Shanshan,Tong Qi,Gao Peng,Ni Xiaolu,Zhang Zhenzhou,Tu Weifeng
Although industrial Cu/ZnO/Al 2 O 3 catalysts are highly promising for methanol synthesis from CO 2 hydrogenation, identifying the nature of the surface active structure and establishing a quantitative structure-activity relationship remain elusive. Herein, through integrated qualitative, titration, and isothermal adsorption characterizations, we elucidate how Zr species promotion tailors the electronic and structural properties of Cu/ZnO x interfacial sites—the primary active sites. A substantial methanol STY of 0.813 g g cat –1 h –1 is achieved over the Cu/ZnO/Al 2 O 3 -2Zr catalyst at 503 K and 3 MPa with an H 2 /CO 2 ratio of 4 and a GHSV of 40,000 mL g cat –1 h –1 , a 23.9% leap over the pristine benchmark. Mechanistically, a linear dependence of CO 2 conversion on the density of Cu/ZnO x interfacial sites is established, which originates from the improved dispersion of both ZnO and Cu induced by moderate ZrO 2 incorporation. Electronic analyses reveal that Zr species acts as an electron donor to ZnO x , enriching its electron density. This electronic modulation facilitates H 2 dissociation and the surface Zn-H-Zn species formation even at low temperature, selectively driving the intermediate hydrogenation to methanol. In situ spectroscopies identify a sequential HCOO* → CH 3 O* hydrogenation pathway for methanol synthesis. Ultimately, this work establishes a definitive quantitative structure-activity relationship, paving a clear path for designing advanced industrial methanol catalysts.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
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2023
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IF 3.1
Wang Yunlong,Sun Yue,Wang Le,Zhang Hao,Hu Jiakang,Li Yongxin
Phenolic compounds, classified as persistent organic pollutants, pose a significant threat to both human health and environmental safety. Therefore, the efficient removal of phenolic substances from water is of paramount importance. Laccase, a multicopper oxidase, is commonly utilized for the efficient removal of phenolic contaminants from water due to its highly effective catalytic activity towards phenolic compounds. However, natural laccase exhibits certain limitations that impede its practical implementation in industrial settings, including a restricted pH activity range, diminished enzymatic efficacy at elevated temperatures, and substantial cost implications. In this work, we prepared a nanozyme (MIZ-Cu, MIZ: 2-methylimidazole) with laccase-like activity by coordinating 2-methylimidazole and copper. This nanozyme overcomes the deactivation issues observed in natural laccase under high temperature and alkaline conditions. The catalytic activity of the MIZ-Cu towards phenolic compounds surpasses that of natural laccase across a wide range of temperature and pH conditions. Under pH=9, 80 °C, and 500 mmol/L NaCl conditions, the removal rate of four phenols (catechol, hydroquinone, resorcinol, and phloroglucinol) by MIZ-Cu was much higher than that of natural laccase. The results also demonstrate exceptional removal rates in natural aquatic environments, thereby presenting a promising approach for the treatment of phenol-containing wastewater originating from industrial facilities.
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Journal of Physical Chemistry C
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2023
·
IF 3.7
XiaoLin Liu,YinYi Ma,QianTong Song,Hao Huang,YuHan He,ShiGang Sun,ZhaoHui Wang
Interface-specific detection of adsorbed key intermediates and product species on the Cu electrode is critical for unraveling the electrocatalytic mechanism of CO2 reduction. In this study, Cu-catalyzed electrocatalysis of CO and CO2 reduction (COR and CO2R, respectively) is investigated using in situ broad-band sum-frequency generation (BB-SFG) spectroscopy. By analysis of the potential-dependent SFG spectra of surface-bound CO (*CO) and possible intermediates in the C–H stretching vibrational range, valuable insights into the electrocatalysis of CO2R are obtained. The SFG spectra of the C–H vibrations reveal two distinct adsorption configurations of surface-bound ethoxy (“standing” and “lying”) on Cu, which provides new molecular evidence to support the presence of C2 intermediates with the atoms of O and C at both ends attached to the Cu surface in the pathway leading to ethanol formation. Moreover, we observed distinct potential-dependent SFG features of *CO in COR and CO2R, while the ethoxy intermediates and product distributions are nearly identical, suggesting that the dimerization of *CO might not be the rate-determining step for the C–C coupling to form ethanol. With these findings, we present a mechanistic scheme for the formation of C1 and C2 products with surface-bound CO and ethoxy intermediates for the formation of ethanol.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jinjuan Xue,Jiaqian Zhang,Meng Yuan,Yiting Lv,Zhaoxia Chen,Mingxin Wang
The development of novel photocatalytic platform for efficient water purification and sterilization is of utmost importance due to the significant threat of chronic diseases resulting from water pollution and bacterial contamination. Herein, a high-efficiency, easy-recyclable, and environment-friendly photocatalytic fabric was developed as a water disinfection and organic pollutant degradation platform. In which, microamounts of Au nanoparticles (2 wt%) and Cu(II) clusters (2.5 wt%) co-decorated porphyrinic MOF (Au/PCN-224/Cu(II)) coating was applied as photocatalytic surface, and flexible cotton fabric served as stable support. Au/PCN-224/Cu(II) composite photocatalyst was prepared via a facile photo-deposition procedure followed by impregnation method, and further immobilized onto polydopamine (PDA) pre-treated cotton fabric through catechol-amine reaction. The fabricated photocatalytic platform exhibited excellent ability to generate reactive oxygen species (ROS) by multiple routes under low-power visible light irradiation, and achieved efficient photodisinfection effects for causative organism including Gram-negative Escherichia coli ( E. coli ) and Gram-positive Staphylococcus aureus ( S. aureus ) without the obvious leakage of metal ions from the potocatalyst during the reaction. Additionally, the reaction rate constant for organic dye MB photodegradation achieved by Au/PCN-224/Cu(II)@Fabric was 3.73 times higher than that of PCN-224@Fabric, and the degradation intermediates analysis was also conducted. The band alignments of PCN-224, Au/PCN-224, Au/PCN-224/Cu(II) photocatalysts were determined, and the charge transfer mechanism within Au/PCN-224/Cu(II) photocatalyst was elucidated through the utilization of DRS, Mott − Schottky, ESR, EIS, and photocurrent analyses. It is suggested that the deposition of Au and doping of Cu(II) both with small amounts enhanced the light absorption capacity, and also improved the charge separation ability through the surface plasmon resonance (SPR) effect and interfacial electron transfer (IFCT) mechanism. Moreover, Au SPR and Cu doping exhibited a substantial enhancement in photothermal conversion effect, thereby synergistically reinforcing the sterilization performance. This work provides an approach for the development of effective photocatalytic platform based on porphyrinic MOFs combined with trace metal co-catalysts in the application of water disinfection and purification.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Tingting Zhu,Jinhang Yang,Yuxiang Shen,Ting Liang,Songyu Fan,Shiming Zhang,Zebin Yu,Shuangfei Wang,Yanping Hou
Z-scheme heterojunction photocatalysts can restrain carriers’ recombination while retaining high redox capacity. Herein, a novel ZnTe/rGO/WO 3 (ZRW) Z-scheme heterojunction was constructed for simultaneous removal of TC and Cu (II) from wastewater. The highly conductive rGO served as a bridge connecting the ZnTe and WO 3 whereby forming a tight interaction interface, beneficial to carriers transfer and separation. The removals of TC and Cu (II) using the optimized ZRW-10% achieved 90.6% and 89.5% within 150 min of light exposure, which were much higher than those from the ZnTe and WO 3 . Results of free radical trapping experiments and electron spin resonance analysis suggested that·O 2 - and·OH were the key active species for TC oxidation while e - dominated Cu (II) reduction. Based on the identified TC degradation intermediates, two possible degradation pathways for TC were proposed, and the ecotoxicity of most intermediates were less than TC. This study can advance research development of designing efficient Z-scheme photocatalyst and elimination of complex pollutants.
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Journal of Materials Chemistry B
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2023
·Vol. 11
·期 48
·11519-11531
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IF 7
Shuhui Chen,Yu Yan,Yixuan Chen,Kaili Wang,Yawen Zhang,Xinlong Wang,Xurui Li,Jian Wen,Yue Yuan
Non-invasive cancer therapies, especially those based on reactive oxygen species, including photodynamic therapy (PDT), have gained much interest. As emerging photodynamic nanocarriers, metal–organic frameworks (MOFs) based on porphyrin can release reactive oxygen species (ROS) to destroy cancer cells. However, due to the inefficient production of ROS by photosensitizers and the over-expression of glutathione (GSH) in the tumor microenvironment (TME), their therapeutic effect is not satisfactory. Therefore, herein, we developed a multi-functional nanoparticle, HN@Cu-MOF, to enhance the efficacy of PDT. We combined chemical dynamic therapy (CDT) and nitric oxide (NO) therapy by initiating sensitization to PDT and cell apoptosis in the treatment of tumors. The Cu2+-doped MOF reacted with GSH to form Cu+, exhibiting a strong CDT ability to generate hydroxyl radicals (˙OH). The Cu-MOF was coated with HN, which is hyaluronic acid (HA) modified by a nitric oxide donor. HN can target tumor cells over-expressing the CD44 receptor and consume GSH in the cells to release NO. Both cell experiments and in vivo experiments showed an excellent tumor inhibitory effect upon the treatment. Overall, the HN@Cu-MOF nanoparticle-integrated NO gas therapy and CDT with PDT led to a significant enhancement in GSH consumption and a remarkable elevation in ROS production.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Mei-Mei Wang,Yun-Ke Cui,Jia-Tai Wen,Yan-Shan Wang,Meng-Hui Jia,Shu-Zhen He,Wei-Kang Wang,Juan Xu
Radical and nonradical dominated persulfate activation processes have pros and cons in the degradation of pollutants. It is challenging to flexibly tune the contribution ratios of radicals and nonradicals in a persulfate activation process for improved pollutant degradation. Herein, we successfully synthesize copper oxide catalysts derived from metal-organic frameworks. By varying the annealing temperature, valence states of copper can be regulated in the catalyst, thereby enabling the switching between radical and nonradical mechanisms for persulfate activation. Copper oxides annealed at 300 °C (CuBTC-300) demonstrate high performance in peroxydisulfate (PDS) activation for the degradation of bisphenol A (BPA), with the synergy of radical and nonradical mechanisms. The surface activated PDS-catalyst complex and OH are identified as the reactive oxidative species involved in this process. On one hand, PDS undergoes a one-electron transfer reaction with Cu(I) sites in Cu 2 O, generating SO 4 − , which subsequently converts into OH for BPA degradation. On the other hand, the combination of PDS molecules with CuO forms surface-activated complexes, depriving electrons from BPA. The increased content of Cu(II) in the catalyst gradually directs PDS activation towards the nonradical pathway. As the annealing temperature increases from 300 °C to 500 °C, the contribution of nonradical oxidation to BPA degradation increases from 58.65 % to 100 %. This work provides new insights into flexibly regulating persulfate activation mechanisms via rational catalysts design.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Jie Ding,Zisu Xu,Hongjun Fang,Xinzhen Feng,Weijie Ji
The aim of this study is to achieve a high fraction of monoene in biomass-derived cardanol to manipulate a well-balanced potential of cross-linking and coupling between resin and curing agent for heavy-duty coating. We reported a heterogeneous nonprecious trimetallic catalyst for selective hydrogenation of polyenes in cardanol for the first time. By cointroducing the second and third metal constituents (Cu and Co), and particularly facet controlling as well as Zn doping of Al2O3 substrate, we can accomplish the highly selective hydrogenation of triene/diene into monoene with variable ratio. The larger sized Ni entities with higher electron density on the Al2O3 hexagonal plates are more favorable for activating triene/diene responsible for a high potential of selective hydrogenation. On the other hand, the Ni0 fraction is comparatively lower, while the mean particle size of Ni0 is the smallest with lower electron density on the commercially obtained γ-Al2O3 spherules. The latter kind of Ni entities is more favorable for activating hydrogen to generate highly reactive H species accounting for a strong potential of full hydrogenation. Over a fine-tuned 10% Ni-5% Co-3% Cu/3% Zn-Al2O3-hexagonal plate under the optimized conditions (7.5% cardanol in n-butanol, 2.5 MPa H2, 80 °C, and 3.5 h), as high as 76% monoene can be obtainable. It is worth noting that not only the current catalyst system is more economic but also the reaction becomes kinetically much faster (within 3.5 h). This catalyst system is operational to a large-scale application in the modification of cardanol via selective hydrogenation. Ni–Co–Cu synergism and low-content Zn modification of the Al2O3 (110) facet are essential to achieve the aim of this study.
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Journal of Physical Chemistry C
·
2023
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IF 3.7
Yuanbo Gao,Chi Zhang,Man Fang,Yunchao Li,Louzhen Fan,Xiaohong Li
Oxidase-mimicking nanozymes are some of the most important nanozymes, which are investigated in various buffer concentrations. However, buffer concentration-dependent catalytic performance is rarely investigated. Herein, with o-phenylenediamine (OPD) as a substrate, the catalytic performance of Cu-Adenine oxidase mimic (fabricated with Cu2+ as an active center and adenine as a ligand) gradually decreases upon Tris–HCl buffer concentration (CTris–HCl) increasing from 10 to 200 mM, exhibiting buffer concentration-dependent catalytic activity. Such buffer concentration-dependent catalytic activity is believed to be because Tris–HCl and OPD competitively bind with Cu-Adenine, leading to differences in catalytic activity. Similarly, with 2,4-dichlorophenol (2,4-DP) as a substrate and 4-aminoantipyrine (4-AP) as a chromogenic agent, the same results are obtained. However, with 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) and 3,3′,5,5′-tetramethylbenzidine (TMB) as substrates, the catalytic oxidation cannot be observed at CTris–HCl ≥ 50 mM. Tris–HCl and substrate competitively binding with Cu-Adenine produces buffer concentration-dependent catalytic performance. Subsequently, substrates are successfully expanded to other aromatic amines (p-phenylenediamine (PPD), 1,5-naphthalenediamine (1,5-NDA), 1,8-naphthalenediamine (1,8-NDA)) and phenols (phenol, 3-cresol, 1-naphthol). Based on the results, with 50 and 150 mM Tris–HCl buffer solutions as sensing channels, a Cu-Adenine-based colorimetric sensor array is constructed for discriminating four representative aromatic amines (OPD, PPD, 1,5-NDA, 1,8-NDA) and four phenols (2,4-DP, phenol, 3-cresol, 1-naphthol) as low as 50 μM. The performance is further validated through accurately identifying binary, quaternary, and even senary and octonary mixtures. Finally, the designed sensor array is successfully applied for identifying eight representative aromatic amines and phenols in river water, seawater, and sewage water, presenting great potential and valuable applications for large-scale scanning levels of aromatic amines and phenols in water samples.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yanyan Zhang,Zhilin Jiang,Ruiqi Zhang,Kang Wang,Xitao Wang
The construction of metal–semiconductor heterojunction has been proven to be an effective way to improve the separation efficiency of photogenerated electrons and holes, thus enhancing photocatalytic activity of semiconductor with narrow band gap. Here, we construct a Cu-(Ga 0.2 Cr 0.2 Mn 0.2 Ni 0.2 Zn 0.2 ) 3 O 4 high entropy oxide (HEO) heterojunction by using Cu-containing HEO precursor, and the effect of Cu addition method on the photocatalytic performance was investigated. The results show that the addition method of Cu has a great influence on the size of Cu nanoparticles (NPs), heterojunction amount and photocatalytic activity of Cu-HEO catalysts. Cu-HEO samples prepared by direct introduction method possess much smaller Cu particles due to the uniform distribution and stronger diffusion hysteresis effect of Cu in HEO, and exhibit superior photocatalytic activity and CH 4 selectivity for CO 2 reduction. With the increase of Cu loading, the photocatalytic activity of Cu-HEO samples firstly increases and then decreases. Among these photocatalysts, Cu 0.5 -HEO obtained by the direct introduction method displays the highest CO 2 reduction activity, and the yields of CO and CH 4 reach to 5.66 and 33.84 µmol/h/g cat , respectively. This work innovatively uses HEO precursors with unique properties to construct metal-HEO heterojunctions with smaller metal particles and more active sites.
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