APPLIED ORGANOMETALLIC CHEMISTRY
·
2022
·Vol. 36
·期 4
·e6587
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IF 4.072
Dan Mo,Xun Song,Jiri Wu,Yogini Jaiswal,Yifu Guan,Yuzhen Zhang,Yunjun Shen,Hedong Bian
Metal complexes have been reported to possess excellent free radical scavenging and antimicrobial properties. In the present study, seven linear trinuclear complexes were synthesized based on bis Schiff base ligand and complexes 1 , 3 – 7 are reported for the first time. Their structure was characterized by IR spectroscopy and single crystal diffraction. BSA was used as carrier to hybridize the synthesized complexes to construct hybrid proteins. The interaction between metal complex and BSA was studied by UV–Vis spectrophotometry and fluorescence spectroscopy. Static quenching was the main mechanism identified for the interaction between metal complex and BSA. In the superoxide dismutase (SOD) activity test, IC 50 values of complexes and hybrid proteins range between 2.89 and 26.53 μM, with hybrid proteins demonstrating a stronger activity than the complexes. Among all the complexes studied, complex 5 exhibited the strongest inhibition against Candida albicans (MIC 12.5 μg ml −1 ) and Cryptococcus neoformans (MIC 6.5 μg ml −1 ).
研究领域:
无机化学
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生物化学
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药学
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微生物学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
·
IF 9.229
Wenyang Fu,Xuedong Du,Pei Su,Qizhan Zhang,Minghua Zhou
As nitrate contamination causes serious environmental problems, it is necessary to develop stable and efficient electrocatalysts for efficient electrochemical nitrate reduction reaction (ENRR). Here, a nonprecious Co3O4/carbon felt (CF) electrode with a 3D structure was prepared by integrating electrodeposition with calcination methods. This 3D structured Co3O4/CF electrode exhibits a high-rate constant of 1.18 × 10–4 s–1 cm–2 for the ENRR, surpassing other Co3O4 electrodes in previous literature. Moreover, it also has an excellent stability with a decrease of 6.4% after 10 cycles. Density functional theory calculations, electron spin resonance analysis, and cyclic voltammetry were performed to study the mechanism of the ENRR on the Co3O4/CF electrode, proving that atomic H* (indirect pathway) plays a prominent role in NO3– reduction and clarifying the synergistic effect of Co(III) and Co(II) in the Co(II)–Co(III)–Co(II) redox cycle for the ENRR: Co(III) prefers the adsorption of NO3– and Co(II) favors the production of H*. Based on this synergy, a relatively large amounts of Co(II) on the surface of the Co3O4/CF electrode (1.3 Co(II)/Co(III) ratio) was maintained by controlling the temperature of calcination to 200 °C with a lower energy barrier of H* formation of 0.46 eV than other ratios, which is beneficial for forming H* and enhancing the performance of the ENRR. Thus, this study suggests that building 3D structure and optimizing Co(II)/Co(III) ratio are important for designing efficient Co3O4 electrocatalyst for ENRR.
研究领域:
环境科学
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电化学
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材料科学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Jiaying Zhang,Fan Fan,Wei Zhu,Wenqing Yao,Fupeng Zhao,Zhuang Yang,Cong Wang,Yajun Wang
The low regeneration rate of Co(II) is a major obstacle to the efficient activation of peroxymonosulfate (PMS) by Co in advanced oxidation technology. Herein, a Co(II)/oxygen-defect monoclinic monazite BiPO4 (Co(II)/BiPO4−x) photocatalyst was prepared. The degradation efficiency of tetracycline hydrochloride (TCH) and polyethylene terephthalate (PET) in the 25%Co(II)/BiPO4−x/PMS/UV system is up to 99.0% (within 30 min) and 40.4%, which was 1.9 and 6.5 times that of the BiPO4/PMS/UV system, respectively. The loading of Co(II) increases the oxygen defect concentration of BiPO4−x, therefore more photogenerated electrons can involve in the Co cycling to promote PMS activation. Meanwhile, simultaneous illumination X-ray photoelectron spectroscopy (SI-XPS) indicates that the electrons are transferred from BiPO4−x to Co, accelerating the regeneration rate of Co(II). DFT calculation reveals that 25%Co(II)/BiPO4−x exhibits much lower reaction energy barrier. This novel work demonstrates a new perspective to modulate the free radical and nonradical dual-pathway for treating refractory contaminants through defect engineering.
研究领域:
环境科学
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材料科学
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化学
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DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Siyi Pan,Pingxiao Wu,Leiye Sun,Meiqing Chen,Bo Li,Tianming Wang,Zhongbo Shang,Jiangmin Fang,Nengwu Zhu,Zhi Dang
Green rust (GR), as a vital intermediate product during the formation of various iron oxides, exists with organic matters and metals contaminants in natural environments. Understanding the effects of these natural factors on the transformation process of GR into iron oxides and the environmental behaviors of heavy metals and organic matters during process are critical for environmental quality management, but the fundamental identification of the interaction mechanisms between them and GR is still challenging. In this study, the transformation mechanisms of Co-bearing green rust (GR-Co) synthesized by co-precipitation, and the redistribution behaviors of Co(II) in an environment containing oxalic acid (OA) and citric acid (CA) were clarified. The findings indicated that OA promoted the Fe(II) dissolution and the transformation of GR-Co to goethite, while CA decreased the Fe(II) dissolution and the proportion of non-extractable Co. Furthermore, in the presence of CA, the transformation products of GR-Co were ferrihydrite, magnetite, lepidocrocite and goethite instead of only lepidocrocite and goethite. Meanwhile, CA prohibited ferrihydrite from transforming into more highly crystalline iron minerals. The finding of this study improves the understanding of the interaction mechanisms between GR-Co and organic matter, and the environmental geochemical behaviors of Co and organic carbon during the transformation processes in nature.
研究领域:
环境科学
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矿物学
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DOI
PubMed
高影响因子
ACS ES&T Engineering
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2021
·
IF 0
Zihao Zhao,Xinhong Li,Hongchao Li,Jieshu Qian,Bingcai Pan
The combination of Co(II) and peracetic acid (PAA) is an important alternative advanced oxidation process (AOPs), in which R-O• radicals including acetyloxyl radicals (CH3C(O)O•) and acetylperoxyl radicals (CH3C(O)OO•) have been considered to be the primary reactive species for the oxidative degradation of contaminants. However, it is still unclear how the active Co species participates in this process. In this study, we conduct a series of experiments including chemical probing, radical quenching, electron paramagnetic resonance (EPR), and Co(III) oxidation to investigate the degradation mechanism of contaminants in the Co(II)/PAA process, using bisphenol A (BPA) as target pollutant. On the basis of these results, we propose a Co(II)-PAA complex (Co(II)-OO(O)CCH3) to be the primary reactive species, while R-O• radicals and Co(III) (available as dimeric Co-peroxide species) derived from the decomposition of Co(II)-PAA complex are the minor contributors for the oxidation of BPA. Factors, including PAA concentration, Co(II) concentration, solution pH, inorganic anions, and natural organic matters (NOM), that might affect the oxidation performance of the Co(II)/PAA process were also investigated systematically. This study sheds new light on the mechanistic understanding of the Co(II)/PAA process for the oxidation of contaminants in water.
研究领域:
环境科学
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化学
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产品关联
DOI
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Hongchao Li,Zihao Zhao,Jieshu Qian,Bingcai Pan
The catalytic activation of peroxymonosulfate (PMS) is under intensive investigation with potentials as an alternative advanced oxidation process (AOP) in wastewater treatment. Among all catalysts examined, Co(II) exhibits the highest reactivity for the activation of PMS, following the conventional Fenton-like mechanism, in which free radicals (i.e., sulfate radicals and hydroxyl radicals) are reckoned as the reactive species. Herein, we report that the primary reactive species (PRS) is proposed to be a Co(II)–PMS complex (Co(II)–OOSO3–), while free radicals and Co(III) species act as the secondary reactive species (SRS) that play a minor role in the Co(II)/PMS process. This Co(II)–OOSO3– exhibits several intriguing properties including ability to conduct both one-electron-transfer and oxygen-atom-transfer reactions with selected molecules, both nucleophilic and electrophilic in nature, and strongly pH-dependent reactivity. This study provides novel insights into the chemical nature of the Co(II)-catalyzed PMS activation process.
研究领域:
环境科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Crystals
·
2019
·Vol. 9
·期 9
·477
·
IF 2.061
Qian-Jun Deng,Min Chen,Dong-Chu Chen,Chang-Ai Chen
The organic ligand (1-methyl-1H-benzo[d]imidazol-2-yl)methanol (HL) was used to react with CoX2·6H2O (X = Cl and Br) under solvothermal conditions to obtain the complex [Co4(L)6(X)2] (1, X = Cl; 2, X = Br). The butterfly-shaped structure of complex 1 and 2 suggest that Co(II) ions have two different coordinated modes, which are five coordination with O3NX environment and six coordination with O4N2environment. In addition, the electrospray ionization mass spectrometry (ESI-MS) analysis indicated that the ion molecular fragment of highest intensity was [Co4(L)6]2+, and there existed a high nuclear fragment peak of [Co7(L)12]2+. Interestingly, it was basically completely transformed into [Co7(L)12]2+two days later, so those two complexes were relatively stable in CH3OH. Magnetic characterization exhibited that complex 1 and 2 display field-induced single-molecule magnetic behavior, of which the energy hillsUeff/kBwere 28 and 20 K under direct-current field of 0.1 T, respectively.Keywords:tetranuclear;butterfly shaped;mass spectrometric;single-molecule magnet (SMM)
研究领域:
无机化学
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材料科学
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DOI
高影响因子
NUCLEAR TECHNOLOGY
·
2022
·
IF 1.667
Yanhui Wang,Qiao Jiang,Yexin Yang,Jianfeng Cheng,Chenyang Bao,Yuelong Pan,Yu Liu,Gang Yang,Yangchun Leng,Xianguo Tuo
The alteration of the morphology of bentonite, a key barrier to isolating high-level radioactive waste in deep geological repositories under long-term interaction with groundwater, was studied. Bentonite colloids were prepared from Gaomiaozi bentonite, and its various properties were analyzed by various characterization methods. The effects of various factors on the adsorption of Cs(I) and Co(II) on bentonite colloids were investigated by batch static adsorption experiments. The results showed that the colloids were mainly composed of montmorillonite and were lamellar in shape, with a zeta potential of −enton mV and an average size of approximately 209.10 nm. The adsorption of Cs(I) and Co(II) by the colloids was a rapid process, and 31.78 and 88.24 mg/g, respectively, were adsorbed at equilibrium. Pseudo-second-order kinetic fitting showed that chemisorption plays a dominant role and acid-base interactions affect adsorption by influencing the stability of colloids and the chemical form of simulated nuclides. This work can be helpful for evaluating the safety of waste repositories.
研究领域:
环境科学
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放射性废物管理
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DOI
高影响因子
HYDROMETALLURGY
·
2022
·
IF 4.217
Yu Deng,Yi Zhang,Yigang Ding
Recovery and separation of rare earth elements was highly crucial but difficult. In this study, a well-designed new ionic liquid named as benzyltributylammonium decanedioate ([N 444Bn ] 2 [SA]) was developed to extract rare earths and separate Sm(III) from the spent SmCo magnets in acetate medium for the first time. To exhibit the superiority of acetate medium, the extraction of Nd(III) and La(III) in three different media were comparatively investigated under different conditions, including equilibrium time, initial pH of aqueous solution, rare earth concentration, extractant concentration, salting-out agent concentration and extraction temperature. The results revealed that the better extractabilities of La(III) were observed in acetate medium rather than those in chloride medium (i.e., 97.6% versus 78.6%), which may be attributed to the low-hydrated nature of acetate ions. Importantly, the back-extraction experiments indicated that 91.4% Nd(III) can be stripped from [N 444Bn ] 2 [SA] by using 1.5 mol/L HOAc, revealing the outstanding reusability of ionic liquid in the industrial separation-stripping cycles. Furthermore, the ion association mechanism was proposed to describe the extraction behavior and confirmed by the slope analysis and FT-IR characterizations in three media. In terms of the SmCoCu mixture separation, the maximal separation factor of Sm(III)/Co(II) was calculated as 3078 in simulated solution. Impressively, the recovery of Sm(III) from the actual SmCo magnets by our dicarboxylate-type ionic liquid was also successfully achieved with a recycling rate of 96.8% and a Sm(III)/Co(II) selectivity of 148, which exhibited the potential application in the separation of Sm(III) from the spent SmCo magnets.
研究领域:
化学工程
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材料科学
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环境科学
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DOI
高影响因子
MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 7
·1-8
·
IF 5.479
Zhou Jiao,Ling Yu,Li Nian Bing,Luo Hong Qun
The authors describe a fluorometric and resonance Rayleigh scattering dual-mode scheme for detection of the activity and inhibition of alkaline phosphatase (ALP). The method utilizes (a) CoOOH nanoflakes, which have high resonance Rayleigh scattering activity and can strongly adsorb ssDNA, and (b) Co(II)-dependent DNAzyme assisted signal amplification. ALP specifically catalyzes the hydrolysis of ascorbic acid-2-phosphate to produce ascorbic acid which reduces CoOOH nanoflakes to Co(II) ion. The Co(II)-dependent DNAzyme is then activated by Co(II) ion, and this results in the cleavage of a substrate labeled with both a fluorophore and a quencher. Following hydrolysis, fluorophore and quencher become separated and the fluorescence measured at excitation/emission wavelengths of 490/518 nm recovers, while the RRS signal at 405 nm decreases. The method works on the 0.2 to 2000 U L −1 ALP activity range, and the detection limit is 0.05 U L −1 . The method was used to validate the mechanism of the action of two classical ALP inhibitors (EDTA and Na 3 VO 4 ). Conceivably, it can also be applied to screen for ALP inhibitors.
A bioprobe composed of cobalt oxyhydroxide (CoOOH) nanoflakes as the substrate and carrier, and Co 2+ -dependent DNAzyme containing guanine ribonucleotide (rG) and uracil ribonucleotide (rU) for circularly signal amplification is used for fluorometric determination of alkaline phosphatase (ALP) activity.
研究领域:
分析化学
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生物化学
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纳米技术
·
酶学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Surfaces and Interfaces
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2024
·
IF 5.7
Ting Pan,Chuang Chen,Li Yu,Cong Yin,Mi Zhou,Huidong Qiu,Guoyuan Yuan,Wei Xiong,Xiaoqin Pu
In addressing the crucial need for separating cobalt ions from leachate solutions of spent ternary lithium batteries (TLBs), this study focuses on the development of an innovative molecular sieve (MS)-based MOFs material, MS-MIL-53(Al), synthesized by combining MS with 2,5-dihydroxyterephthalic acid. Since the powdered MS-MIL-53(Al) material presents a granular powdery form, which is difficult to recover during the adsorption process, electrospun nanofibers denoted as MS-MIL-53(Al)/PAN, were fabricated and functionalized with hydroxylamine hydrochloride to create MS-MIL-53(Al)/AOPAN. Static adsorption experiments conducted with MS-MIL-53(AL)/AOPAN as the adsorbent in cobalt-containing wastewater revealed a maximum adsorption content of 65.3 mg/g for Co(II). Moreover, the material exhibited a tensile strength at the breaking point of 0.077 kPa, indicating its excellent mechanical properties. The adsorption process followed pseudo-second-order kinetics and the Langmuir isotherm model, showcasing a spontaneous, endothermic monolayer chemical adsorption behavior. XPS analysis highlighted the influence of hydroxy and amidoxime functional groups on Co(II) adsorption. Notably, MS-MIL-53(Al)/AOPAN displayed exceptional stability, retaining over 90 % of its adsorption capacity after five cycles, demonstrating its potential for efficient Co(II) separation in wastewater treatment. This study is the first to synthesize MOFs material using MS as the base material, showing potential cost reduction and enhanced adsorption capabilities, with implications for advancing the innovative use of MOFs.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Polymers
·
2024
·Vol. 16
·期 9
·1239
·
IF 4.7
Cong Yin,Yang Luo,Ting Pan,Liting Ding,Chenghuang Wang,Guoyuan Yuan,Chongxiong Duan
Recovering cobalt from waste batteries is crucial for resource recycling and environmental protection. Here, MOF-OH, a Zr-based MOF, was synthesized and merged into a polyacrylonitrile (PAN) matrix to create MOF-OH-PAN nanofibers (NFs). These NFs showed a high cobalt ion adsorption capacity of 33.1 mg/g, retaining over 90% of the capacity after six cycles. The adsorption mechanism involves Co(II) surface diffusion followed by strong bonding with functional groups. This technology enables efficient cobalt recovery from waste batteries, supporting reuse and reducing resource depletion and environmental pollution. The study provides insights into waste battery resource management, highlighting environmental and economic benefits and contributing to green resource recovery and circular economy initiatives.
研究领域:
材料科学
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环境科学
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资源回收
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）