BIOCHEMICAL ENGINEERING JOURNAL
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2022
·
IF 4.446
Ying Zhang,Yucui Jiang,Bin Wei,Mingming Su,Hao Liang
Enzyme is an efficient green catalyst, but its vulnerability and difficulties of separation from products limited the application in industry. Furthermore, a large number of oxidase enzymes rely on dihydronicotinamide adenine dinucleotide (NADH) or dihydronicotinamide adenine dinucleotide phosphate (NADPH) cofactors . These cofactors are too expensive to be used in industrial processes. Thus, cofactor regeneration is an important method to avoid the consumption of large quantities of oxidized cofactor NAD(P) + in enzyme-catalyzed reactions. In this paper, Cu based metal nucleotides coordination polymers (MNCPs) with NAD(P)H oxidase activity were constructed by self-assembly of copper ions and nucleotides. Cu 2+ /AMP and Cu 2+ /GMP showed high catalytic activity and high reusability. Then, Cu 2+ /AMP with NADH oxidase activity was combined with NAD + dependent alcohol dehydrogenase (ADH) to construct a bienzyme cascade system with circulating cofactor, which applied to the conversion of benzyl alcohol to benzaldehyde. In this system, ADH exhibited high activity due to the increase of substrate concentration and the inhibition of the diffusion of intermediate products. Besides, the bienzyme cascade system also showed high stability and reusability. After 8 cycles, the immobilized ADH remained more than 57% of the initial activity. The prepared bienzyme cascade system can extensively extended its application in industrial production.
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ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Tan Ke,Guangyu Guo,Junrong Liu,Chao Zhang,Yue Tao,Panpan Wang,Yanhong Xu,Lanzhou Chen
To explore a novel strategy for the remediation of soils polluted with Cu and Cd, three strains of plant-growth-promoting rhizobacteria (PGPRs) isolated from contaminated mines and two grass species (perennial ryegrass and tall fescue) were selected in this study. The performance of PGPR strains in metal adsorption, maintaining promotion traits under stress, and ameliorating phytostabilization potential was evaluated. Cd 2+ exerted a stronger deleterious effect on microbial growth than Cu 2+ , but the opposite occurred for grass seedlings. Adsorption experiment showed that the growing PGPR strains were able to immobilize maximum 79.49% Cu and 81.35% Cd owing to biosorption or bioaccumulation. The strains exhibited the ability to secrete indole-3-acetic acid (IAA) and dissolve phosphorus in the absence and presence of metals, and IAA production was even enhanced in the presence of low Cu 2+ (5 mg L −1 ). However, the siderophore-producing ability of the isolates was strongly suppressed under Cu and Cd exposure. Ryegrass was further selected for pot experiments owing to its higher germination rate and tolerance under Cu and Cd stress than fescue. Pot-experiment results revealed that PGPR addition significantly increased the shoot and root biomasses of ryegrass by 11.49%–44.50% and 43.53%–90.29% in soil co-contaminated with 800 mg Cu kg −1 and 30 mg Cd kg −1 , respectively. Metal uptake and translocation in inoculated ryegrass significantly decreased owing to the reduced diethylenetriamine pentaacetic acid-extractable metal content and increased residual metal-fraction percentage mediated by PGPR. Interestingly, stress mitigation was observed in these inoculated plants; in particular, their malondialdehyde content and superoxide dismutase activity were even significantly lower than those of ryegrass under normal conditions. Therefore, PGPR could be a promising option to enhance the phytostabilization efficiency of Cu and Cd in heavily polluted soils.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Yongqing Wang,Zhiqiang Lan,Hong Fu,Haizhen Liu,Jin Guo
MgTM/ZIF-67 nanocomposites were prepared by the deposition-reduction method using ZIF-67, MgCl 2 , and TMCl x (TM = Ni, Cu, Pd, Nb) as raw materials. The dehydrogenation activation energies of MgTM/ZIF-67 (TM = Ni, Cu, Pd, Nb) nanocomposites were calculated to be 115.4 kJ mol −1 H 2 , 115.7 kJ mol −1 H 2 , 113.6 kJ mol −1 H 2 , and 75.8 kJ mol −1 H 2 , respectively; hence, the MgNb/ZIF-67 nanocomposite manifested the best comprehensive hydrogen storage performance. The hydrogen storage capacity of the MgNb/ZIF-67 nanocomposite was hardly attenuated after the 100th hydrogen absorption-desorption cycle. The dehydrogenated enthalpies of MgH 2 and CoMg 2 H 5 in MgNb/ZIF-67 hydride were calculated to be 72.4 kJ mol −1 H 2 and 81.0 kJ mol −1 H 2 , respectively, which were lower than those of additive-free MgH 2 and Mg/ZIF-67. The improved hydrogen storage properties of MgNb/ZIF-67 can be ascribed to the CoMg 2 –Mg(Nb) core-shell structure and the catalytic effects of NbH and niobium oxide nanocrystals .
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2019
·Vol. 411
·期 25
·6645-6653
·
IF 3.286
Ma Xin,Lin Shijun,Dang Yunfei,Dai Yu,Zhang Xiaojin,Xia Fan
Carbon dot (CD)-based fluorescent probes have been widely exploited; however, multi-component detection using CDs without tedious surface modification is always a challenging task. Here, we develop a convenient and simple CD-based “on-off-on” fluorescent probe for detection of copper(II) ion (Cu 2+ ), ascorbic acid (AA), and acid phosphatase (ACP). Cu 2+ leads to the fluorescence quenching of CDs. The limit of detection (LOD) for Cu 2+ is 2.4 μM. When AA is added into the CDs + Cu 2+ solution, Cu 2+ is reduced by AA to Cu + , causing the fluorescence recovery of CDs. The fluorescent intensity linearly correlates with the concentration of AA in the range of 100–2800 μM with LOD of 60 μM. Besides, the probe has potential application for detection of AA in real samples such as VC tablets, orange juice, and fresh orange. The probe can also indirectly detect ACP that enzymatically hydrolyzes ascorbic acid-phosphate (AAP) to produce AA. This work expands the application of CDs in the multi-component detection and provides a facile fluorescent probe for detection of AA in real samples.
Graphical abstract
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Catalysts
·
2026
·Vol. 16
·期 10
·857
·
IF 4.5
Piaoyin Zhang,Peiyuan Li,Yingchun Sun,Xin Sun,Ye Jiang,Zhengda Yang,Yang Yang
The control of CO emissions from iron and steel sintering flue gas has received increasing attention. In this work, Pt-loaded Mn–Cu catalysts were prepared by a redox precipitation method to investigate the effects of Pt loading and calcination temperature on low-temperature CO oxidation activity and SO2-induced deactivation behavior. Among the tested catalysts, 1Pt/MnCu-300, containing 1 wt.% Pt and calcined at 300 °C, exhibited the highest low-temperature CO oxidation activity and achieved complete CO conversion at 75 °C. Under the specified SO2-containing test conditions, all catalysts eventually underwent severe and largely irreversible deactivation, whereas Pt loading and calcination temperature altered the transient CO-conversion decay profiles. Pt/MnCu-450 retained high CO conversion for a longer initial period during SO2exposure than the other catalysts in the calcination-temperature series; however, this observation does not by itself demonstrate superior intrinsic SO2tolerance because the present experiments did not quantify SO2breakthrough, sulfur uptake, or active-site-normalized deactivation rates. Characterization results show that Pt modification increased the specific surface area, altered the Mn3+/Mn4+ratio and surface oxygen species, promoted oxygen-vacancy formation, and enhanced CO adsorption and redox properties. These physicochemical changes are correlated with the improved low-temperature CO oxidation activity of Pt-modified Mn–Cu catalysts. This work clarifies the effects of Pt loading and calcination temperature on CO oxidation performance and on the transient response to SO2exposure.
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MOLECULES
·
2022
·Vol. 27
·期 15
·4712
·
IF 4.927
Yu Lei,Bin He,Shujun Huang,Xinyan Chen,Jian Sun
Facile construction of functional nanomaterials with laccase-like activity is important in sustainable chemistry since laccase is featured as an efficient and promising catalyst especially for phenolic degradation but still has the challenges of high cost, low activity, poor stability and unsatisfied recyclability. In this paper, we report a simple method to synthesize nanozymes with enhanced laccase-like activity by the self-assembly of copper ions with various imidazole derivatives. In the case of 1-methylimidazole as the ligand, the as-synthesized nanozyme (denoted as Cu-MIM) has the highest yield and best activity among the nanozymes prepared. Compared to laccase, theKmof Cu-MIM nanozyme to phenol is much lower, and thevmaxis 6.8 times higher. In addition, Cu-MIM maintains excellent stability in a variety of harsh environments, such as high pH, high temperature, high salt concentration, organic solvents and long-term storage. Based on the Cu-MIM nanozyme, we established a method for quantitatively detecting phenol concentration through a smartphone, which is believed to have important applications in environmental protection, pollutant detection and other fields.Keywords:laccase;phenolic oxidation;nanozyme;intelligent detection;self-assembly synthesis
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Sijia Tian,Chi Zhang,Mincong Yu,Yunchao Li,Louzhen Fan,Xiaohong Li
Laccase mimics are multicopper oxidase highly important for biotechnology and environmental evaluation/remediation. However, buffer species-dependent catalytic activity is rarely investigated. Herein, through Cu 2+ coordinating with adenine (A), gram-scale Cu-Adenine nanosheets are synthesized. As a laccase mimic, Cu-Adenine exhibits excellent catalytic performance in 10 mM Tris-HAc, and greatly decreases in 10 mM MES (4-morpholine ethanesulfonic acid) and further decreases in 10 mM HEPES (N-2-hydroxyethyl piperazine- N ′-2-ethanesulfonic acid) (pH = 7, 25 °C). Moreover, upon gradually increasing NaCl to 500 mM, the catalytic activity further enhances. Such the buffer species/NaCl concentration-dependent catalytic activity is explained with the help of K m (Michaelis constant) and V max (maximum rate value) Based on the fact that Cu-Adenine could differentially catalyze phenolic substrates (2,4-dichlorophenol (2,4-DP), o-chlorophenol (o-CP), m-chlorophenol (m-CP), p-chlorophenol (p-CP), phenol and catechol), a colorimetric sensor array with three buffer solutions as sensing channels is designed for simultaneously discriminating 2,4-DP, o-CP, m-CP, p-CP, phenol and catechol as low as 10 μM, even quantifying 2,4-DP (as a model analyst). The performance is further validated through accurately identifying binary and ternary mixtures , and even 18 blind samples containing one of six phenols and ternary mixtures. Finally, the designed sensor array is successfully applied for identifying six representative phenols in various simulated water samples, presenting great potential and valuable applications for large-scale scanning levels of phenols in water samples.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Zanling Huang,Shuqi Zhu,Abebe Reda Woldu,Wenhua Gao,Jing-Xin Jian,Paul K. Chu,Qing-Xiao Tong,Liangsheng Hu
Electrochemical glucose detection co-catalyzed by bimetallic ions is carried out by introducing Co(II) and Cu(II) into the alkaline solution. The technique avoids the complicated electrode design and catalyst poisoning. By using nitrogen-doped carbon nanotubes (NCNT) loaded on carbon cloth (CC) as the working electrode, the bimetal co-catalytic system achieves a sensitivity of 6,909 mA M −1 cm −2 , a detection limit of 0.4 μM (S/N = 3), as well as good selectivity and stability. By performing systematic electrochemical and structural analysis, the mechanism of Co(II) and Cu(II) co-catalysis for glucose detection in the solution is elucidated. Co(II) supplies the dynamic reaction sites and source of active intermediate (CoOOH), while Cu(II) promotes the formation of CoOOH. The results provide mechanistic insights into bimetal co-catalysis of glucose detection and other electrochemical reactions .
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhicheng Xu,Yuran Li,Yuting Lin,Yan Wang,Qiang Wang,Tingyu Zhu
To strengthen the CO oxidation activity of activated carbon for flue gas purification, AC was modified through acid treatment and metal loading. AC-supported Cu shows excellent catalytic oxidation activity compared with other metal-modified AC samples. To investigate the action modes of Cu loaded on activated carbon and the mechanism of CO oxidation, various samples were characterized by XRD, N 2 O titration, SEM, N 2 physisorption, TPD, H 2 -TPR, XPS, in situ DRIFTS and EPR. The results show that oxygen-containing functional groups increase the loading amount and dispersion of Cu. Moreover, Cu species strongly bound to oxygen-containing functional groups are the main contributors to CO oxidation. The roles of oxygen-containing functional groups are further revealed: carboxyl groups are the anchoring sites of Cu, and hydroxyl groups supply oxygen to restore the active structure. Similarly, Ce indirectly promote the oxidation activity of CO by re-oxidizing Cu + to Cu 2+ , which accelerates the catalytic cycle. The reaction mechanism on AC-supported Cu samples has been proposed to follow the double-site Langmuir–Hinshelwood mechanism, with Cu 2+ as oxidation sites, Cu + as adsorption sites and the formation of oxygen vacancies on Cu + during the reaction. AC-Cu performs the highest oxidation activity at a proportion of Cu + of 0.5–0.6. SO 2 causes irreversible chemical poisoning to CO oxidation, while NO leads to reversible poisoning due to competitive adsorption with CO. The novel AC-supported Cu catalyst with Ce improves the resistance against SO 2 and NO, and the reason is explained. These findings provide theoretical guidance for the preparation and application of metal-modified activated carbon.
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CELLULOSE
·
2022
·Vol. 29
·期 15
·8353-8370
·
IF 6.123
Mo Liuting,Zhang Shifeng
Aerogels, as attractive absorbents, have played essential roles in water treatment due to their light weight, high porosity, and exceptional absorption capacity. Nevertheless, conventional synthetic aerogel usually shows isotropic architectures, unsatisfactory mechanical performance, complex preparation process, and scale-limited fabrication, greatly limiting its applications in water remediation. In this study, inspired by the anisotropic architecture of natural wood, a biomimetic strategy was reported to prepare anisotropic, robust and environmental resistant aerogel composites via assembling semi-interpenetrating polymer networks (semi-IPNs) into the delignified wood template. The anisotropic structure endows the aerogel with excellent anisotropic mechanical behavior. The intermolecular hydrogen bonds of the cellulose microfibrils, the strong interfacial hydrogen bonds between cellulose chains and PI polymer networks, as well as the covalent bonds of semi-IPNs systems enable the aerogel composites to have a high yield strength of 566 kPa and Young’s modulus of 56.335 MPa. The resulting aerogel composite exhibits a high saturation adsorption capacity of 296 mg g −1 at about 100 min for Cu(II) ions. The composite is easily regenerated and recycled five cycles without apparent removal efficiency loss. This study presents a promising, eco-friendly, low-cost, and feasible strategy for scalable fabricating anisotropic, robust, highly efficient, and environmental resistant aerogel composites for heavy metal ions removal. Graphical abstract
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Fang Zhou,Yan Zhu,Longlai Yang,De-Quan Yang,Edward Sacher
Aqueous dispersions of AgCu nanoparticles (NPs), with enhanced antibacterial efficacy, have been prepared through the catalyzed reduction of Cu ions by PVP/PVA-stabilized Ag nanoparticles at 85 °C. The effects of Cu concentration and heating time on NP morphology and antibacterial efficacy were investigated, using TEM, UV-Vis and FTIR spectroscopies , and antibacterial evaluations. The enhanced antibacterial performance of these NPs was correlated with Ag ion release. We propose a simple model of AgCu NP formation, and an enhanced antibacterial efficacy mechanism involving Ag ion release, in which AgCu NPs formation plays a role to control of Ag ion release.
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Journal of Physical Chemistry C
·
2020
·
IF 4.189
Abubakar Yusuf,Yong Sun,Yong Ren,Colin Snape,Chengjun Wang,Hongpeng Jia,Jun He
Defect engineering is an effective strategy to enhance the activity of catalysts for various applications. Herein, it was demonstrated that in addition to enhancing surface properties via doping, the influence of dopants on the surface–intermediate interaction is a critical parameter that impacts the catalytic activity of doped catalysts for low-temperature formaldehyde (HCHO) oxidation. The incorporation of Co into the lattice structure of δ-MnO2 led to the generation of oxygen vacancies, which promoted the formation of surface active oxygen species, reduced activation energy, and enhanced catalytic activity for low-temperature oxidation of HCHO. On the contrary, Cu doping led to a drastic suppression of the catalytic activity of δ-MnO2, despite its enhanced redox properties and slight increase in the surface concentration of active oxygen species, compared to pristine δ-MnO2. Diffuse reflectance infrared Fourier transform analysis revealed that in the presence of Cu, carbonate intermediate species accumulate on the surface of the catalysts, leading to partial blockage of active sites and suppression of catalytic activity.
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