LANGMUIR
·
2025
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IF 3.9
Yue Cao,Yanping Wang,Lirong Guo,Zhiyue Han,Haining Liu,Kaipeng Zhong,Shaoju Bian,Naicai Xu
A novel composite adsorbent, AMP@MIL-101(Cr), has been successfully synthesized by integrating ammonium phosphomolybdate (AMP) with the metal–organic framework MIL-101(Cr) for the efficient adsorption of rubidium ions (Rb+) from aqueous solutions. The results of structural characterizations confirmed that the crystalline framework of the adsorbent remained intact after Rb+ adsorption, indicating excellent structural stability. Adsorption kinetics, isotherm, and thermodynamics studies revealed that the adsorption process followed a single-layer chemisorption mechanism and was an endothermic reaction and spontaneous adsorption process with negligible influence from solution pH. The adsorbent exhibited a remarkable Rb+ adsorption capacity, reaching 69.4 mg·g–1 within 5 min in a solution containing 250 mg·L–1 Rb+ at 45 °C. In the Nanyi Mountain Oilfield, the adsorption rate of adsorbent for Rb+ (10.69%) exceeded that of other ions (Li+: 0.75%; Na+: 0; K+: 0.95%; Mg2+: 0.67%). Furthermore, the adsorbent still maintained 86.72% of its initial adsorption capacity after 5 consecutive adsorption–desorption cycles. These findings highlighted the great potential of AMP@MIL-101(Cr) as an efficient and stable adsorbent for the selective recovery of rubidium from aqueous environments.
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PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2025
·
IF 9
Chengyu Yang,Jie Wei,Yixuan Li,Yuanhao Peng,Xuan Wu,Xianrui Zhang,Yingxin Ding,Shumi Lu,Chongling Feng,Chao Huang
Aging-induced surface passivation of nano zero-valent iron (nZVI) significantly diminishes its reactivity for Cr(VI) reduction, thereby impeding its practical application in environmental remediation. Herein, we propose a novel system integrating aged nZVI (AnZVI), Shewanella oneidensis MR-1, and the endogenous electron shuttle riboflavin (RF) to overcome the passivation limitations and enhance Cr(VI) removal. Remarkably, the AnZVI/MR-1/RF system achieved complete removal of 20 mg L − 1 Cr(VI) within 3 h, outperforming AnZVI/MR-1 and AnZVI alone by 23.8 % and 36.6 %, respectively. Mechanistic investigations revealed that RF mediated direct interfacial contact between AnZVI and MR-1, promoting microbial reduction of the AnZVI passivation layer. Electrochemical analyses confirmed RF’s critical role as an electron mediator in accelerating charge transfer between AnZVI and MR-1. Three-dimensional fluorescence mapping (3D-EEM) analysis revealed microbial extracellular polymeric substances (EPS) contributions to chromium immobilization processes. The immobilization of chromium is primarily attributed to the reduction of Cr(VI) to insoluble Cr(III) species, in conjunction with adsorption and surface complexation mechanisms. TEM validated a significant reduction in the thickness of the iron passivation layer, resulting in the exposure of the underlying Fe⁰ core and a resultant enhancement in reductive capacity. This work provides a robust strategy to overcome AnZVI’s limitations by coupling microbial activity with electron shuttling, offering new insights into sustainable remediation via biotic-abiotic synergies.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Bing Li,Qian Zuo,Zhiyi Deng,Jianhua Cheng,Ping Li,Jinhua Wu
Surface passivation caused by Fe-Cr precipitates limits the application of milli-sized zero-valent iron (mFe 0 ) in filter tanks for Cr(VI) removal. A mFe 0 -based column was established using sand as dispersing media, coupled with a micro-electric field (MEF, 1.2 mA/cm 2 ), to accelerate iron corrosion and enhance Cr(VI) sequestration. A control column without MEF was employed for comparison. Surface analysis verified that the MEF induced mFe 0 particles into three-electrodes with bipolar charges and facilitated electron transfer from iron-core to surrounding O 2 /H 2 O. Ferrous ions from iron corrosion afterwards reduced Cr(VI) and precipitated into secondary minerals (e.g., magnetite, lepidocrocite, and green rust). These minerals effectively sequestered Cr(VI) in their matrices through adsorption-reduction/precipitation on Fe 0 and sand surfaces. Compared to the mFe 0 column, the MEF-mediated mFe 0 (MEF-mFe 0 ) column demonstrated a 2.5-fold increase in kinetic rate constant and a 10-fold decrease in Cr(VI) migration rate, leading to a 9.5-fold augment in Cr(VI) sequestration capacity and a 3.7-fold extension in longevity. Under different hydraulic retention times and influent concentrations, the MEF-mFe 0 column outperformed the mFe 0 column with 6.0 to 9.6-fold higher Cr(VI) sequestration and 3.5 to 5.7-fold longer lifespan. Our study revealed that MEF-assistance represented a promising approach to enhance mFe 0 activation for subsequent Cr(VI) sequestration from water.
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2025
·
IF 3.5
Hu Lan,Zhao Qiuyue,Zhang Xinling,Li Huipeng,Bian Cheng,Zeng Yiqing
Redox sites and acidic sites are the main active sites of bimetallic oxide catalysts used for selective catalytic oxidation of NH 3 (NH 3 -SCO). In this work, three MMoO x (M = Cr, Fe, and Mn) bimetallic oxides catalysts were prepared by simple grinding and calcination to investigate the effect of redox sites (M sites) on the NH 3 -SCO performance. The NH 3 -SCO test results showed that the activity of MMoO x is in the order of CrMoO x > MnMoO x > FeMoO x . The characterization results of H 2 -TPR, O 2 -TPD, NH 3 -TPD, and in situ DRIFTS proposed that the NH 3 -SCO reaction on MMoO x catalysts is proceed via i-SCR mechanism, and the formation of the intermediates of NH 3 -SCR reaction is the decisive reaction step. Owing to the excellent ability in promoting the formation of nitrate/nitrite species, CrMoO x and MnMoO x samples show much higher NH 3 -SCO activity than FeMoO x sample . CrMoO x can facilitate the formation of a large amount of –NH 2 species, which together with nitrate/nitrite species enhance the NH 3 -SCO reaction via i-SCR reaction route. Therefore, CrMoO x shows the highest NH 3 -SCO activity among the MMoO x catalysts. Through this work, the redox sites of bimetallic oxide catalysts are demonstrated as a vital role in inducing the formation of reaction-active intermediates, which highlight the importance of choosing the redox sites in designing NH 3 -SCO catalyst.
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高影响因子
ACS Omega
·
2020
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IF 2.87
Chunmei Xiao,Jianming Lin
The contamination of water systems by heavy metals greatly threatens human health and ecological safety. An efficient adsorbent is critical for the removal of these contaminants. In this work, magnetic Ni3Si2O5(OH)4 nanotubes (NTs) have been synthesized via in situ hydrothermal reduction and further functionalized by grafting poly(4-vinyl pyridine) (P4VP) brushes on its surface via atom transfer radical polymerization. Characterizations by Fourier transform infrared, X-ray diffraction, thermogravimetric analysis, transmission electron microscopy, and X-ray photoelectron spectroscopy proved that P4VP was successfully grafted on the surface of magnetic Ni3Si2O5(OH)4 NTs. The resultant Ni3Si2O5(OH)4-g-P4VP NTs are efficient nanosorbents for removing Cr(VI) anions from water. The Cr(VI) adsorption capacity of Ni3Si2O5(OH)4-g-P4VP NTs reaches 1.49 mmol/g at a pH of 3. The pseudo-second-order kinetic model and the Freundlich isothermal model are suitable to describe the adsorption process. The analysis using Weber–Morris and Boyd models indicates that both intraparticle diffusion and external film diffusion affect the Cr(VI) adsorption process. The adsorption enthalpy is estimated to be 18.37 kJ/mol. More than 90% of the Cr(VI) adsorption capacity of the Ni3Si2O5(OH)4-g-P4VP NTs remains after eight adsorption and desorption cycles.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Zhiping Zhang,Xuejiao Li,Huanyan Xu
Layered perovskite-related GdBaFe 2 O 5+ δ (GBF) and GdBaFeCoO 5+ δ (GBFC) oxides are systematically studied as advanced air electrodes for intermediate-temperature solid oxide fuel cells (IT-SOFCs). The characterizations of the samples are gauged with the assistance of a variety of techniques, involving X-ray diffractometer (XRD), O 2 -temperature programmed desorption (O 2 -TPD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and Fourier transform infrared spectrometry (FT-IR). Results of XRD demonstrate that GBFC has the exact same crystal structure as that of GBF, which displays slight lattice shrinkage. Substitution of Co for Fe increases the TEC from 9.87 × 10 −6 K −1 and 16.6 × 10 −6 K −1 at 150–700 °C. GBFC shows the highest conductivity of 500 S cm −1 at 520 °C, which complies with the requirement for the cathode of the fuel cell. The polarization resistance ( R p ) values of GBF and GBFC are 0.33 Ω cm 2 and 0.07 Ω cm 2 at 650 °C, respectively. Moreover, a single cell based on Sm 0.8 Ce 0.2 O 1.9 (SDC) electrolyte-supported is indicative of a peak power density of 0.28 W cm −2 for GBFC cathode at 700 °C. This single cell also exhibits a superior operational stability utilizing dry hydrogen fuel at 600 °C during the tested 220 h. Electrochemical impedance spectroscopy (EIS) and relaxation time distribution (DRT) results are suggestive of the slowly decreasing oxygen reduction kinetics of GBFC cathode with the introduction of CO 2 or gaseous Cr species, which may be connected with the formation of carbonate or Cr depositions. Compared to classic materials, GBFC cathode shows very good electrochemical stability and CO 2 /Cr tolerance.
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Zhimin Lv,Yifeng Zhang,Ming Fang,Xiaoli Tan
Exploring high-efficiency and low-cost catalysts for reducing Cr(VI) is one of the key problems in solving Cr(VI)-containing wastewater. In this paper, bimetallic Ni- and Co-based carbon sphere (Ni x Co y @NCS) was prepared by a simple hydrothermal-pyrolysis route, in which Ni-Co nanoalloys were uniformly dispersed on N -doped carbon sphere with average nanoparticles of 37.5 nm. The catalytic reduction performance of the hybrid catalyst Ni x Co y @NCS for Cr(VI) can be optimized by manipulation stoichiometry, and the catalytic ability of the Ni 1 Co 1 @NCS was much higher than that of other samples. This is because the synergy between Co and Ni NPs promotes the dehydrogenation efficiency of formic acid and the N doping improves the electron transport efficiency of the catalyst, and the strong protection of N -doped carbon for NPs ensured its excellent recycling ability and durability. In the existence of coexisting ions, the catalytic efficiency of the Ni 1 Co 1 @NCS is not affected at all. The reduction mechanism is mainly because of the active hydrogen during the dehydrogenation pathway of formic acid. This paper demonstrates that bimetallic Ni-Co-based materials have higher catalytic capacity than monometallic Ni or co-based materials.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Li Guo,Kai Lai Zhang,Huidong Shen,Chan Wang,Qiang Zhao,Danjun Wang,Feng Fu,Yucang Liang
Exploiting highly efficient and stable photocatalysts for treating Cr(VI)-containing wastewater is of great importance. Herein, a robust core-shell structurally magnetic Fe 3 O 4 @SiO 2 /Bi 2 WO 6−x F 2x photocatalyst was successfully fabricated and used to photocatalytic Cr(VI) reduction, in which an inert protective layer (SiO 2 )-coated micro/nanostructured Fe 3 O 4 particles can not only improve the chemical stability but also retain magnetic advantage of catalyst. The optimized 55% Fe 3 O 4 @SiO 2 /Bi 2 WO 6− x F 2 x exhibited the highest catalytic activity in a reaction system of pH = 3, the apparent rate constant (k app /min −1 ) of 55% Fe 3 O 4 @SiO 2 /Bi 2 WO 6−x F 2x for photocatalytic reduction of Cr(VI), as high as 0.027 min −1 , is approximately 5.4 and 2.6 times higher than that of Bi 2 WO 6 and Fe 3 O 4 @SiO 2 /Bi 2 WO 6 , respectively. After being illuminated for 90 min, nearly 100% percentage of Cr(VI) has been reduced to Cr(III) by using 55% Fe 3 O 4 @SiO 2 /Bi 2 WO 6−x F 2x as photocatalyst, which can be attributed to the synergistic effect of magnetic Fe 3 O 4 @SiO 2 support – “core”, Bi 2 WO 6 – “shell” and the successful introduction of F − ions. A readily magnetic separation of Fe 3 O 4 @SiO 2 /Bi 2 WO 6−x F 2x catalyst enabled it to reuse conveniently for practical industry application. Finally, the enhanced photocatalytic mechanism of catalyst was proposed for Cr(VI) reduction. The present study not only provides a new mean to solve the recovery of the Bi 2 WO 6 -based photocatalyst, but also presents a promising candidate for Cr(VI) reduction in the field of the industrial wastewater treatment.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
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IF 7.312
Fenglei Liu,Anjie Wang,Miao Xiang,Qingyuan Hu,Baowei Hu
Herein, a magnetic amine-functionalized mesoporous silica SBA-15 (Fe 3 O 4 @SBA-15-PDA/HBP-NH 2 ) adsorbent was fabricated by loading Fe 3 O 4 nano-particles on amino-terminated hyperbranched polymers (HBP-NH 2 ) functionalized SBA-15 and exploited for chromium (VI) and uranium (VI) elimination. The morphologies and microstructures of as-obtained materials were observed using different physicochemical and spectroscopic techniques. Meanwhile, batch experiments were performed to investigate the impacts of various water environment conditions on removal process including solution pH, equilibrium time and temperatures. The maximum adsorption capacities of U(VI) and Cr(VI) on Fe 3 O 4 @SBA-15-PDA/HBP-NH 2 reached up to 77.4 mg/g and 66.5 mg/g under optimal water environment conditions. Moreover, the characterization analysis manifested that removal of U(VI) was fulfilled through the surface complexation with amino and phenolic hydroxyl groups, while Cr(VI) were firstly electrostatically adsorbed, and subsequently reduced to less toxic Cr(III) by phenolic hydroxyl groups. These findings demonstrated that this new magnetic amine-functionalized SBA-15 could be considered as valuable materials in environmental cleanup.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Fei Xue,Hui He,Hang Zhou,Zongyan Quan,Zhiping Chen,Qi Wu,Hongxiang Zhu,Shuangfei Wang
To solve the problem that cellulose-based adsorbents cannot remove Cr(VI) from water to the drinking water standard (US EPA, 0.05 mg/L) within 5 min due to imbalance of the high amine density and high-efficiency diffusion dynamics. A cellulose-based hyperbranched adsorbent (MCC/HBPA-0.88) was designed and prepared via cross-linking with microcrystalline cellulose (MCC) and amino-terminated hyperbranched polymers (HBP-NH 2 ). This strategy for liquid–solid phase one-step rapid conversion could effectively increase the conversion rate of the reactants (above 99%). The cellulose-based hyperbranched adsorbent possessed high amino density (10.63 mmol/g), high swelling rate (341%) and three-dimensional hyperbranched structure. It could rapidly and completely remove Cr(VI) from water with a low level of Cr(VI) (1.02 mg/L), and the residual Cr(VI) concentration satisfied the safe drinking level standards within 1 min, which exceeds the absorption rates of cellulose-based adsorbents that have been reported in the literatures.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
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IF 7.489
Chengwei Sun,Gang Song,Lili Chen,Xuemei Ren,Changlun Chen
Magnetic Fe 3 O 4 nanoparticles were coated by polyethyleneimine (PEI), and then Fe 3 O 4 @PEI was further modified with MoS 2 by the hydrothermal method to fabricate 3D flower-like structured magnetic polyethyleneimine@MoS 2 (MP@MoS 2 ) composites, and the composites were served as efficient adsorbents to capture Cr(VI) and Pb(II) from aqueous solution. The effects of temperature, pH, shaking time and environmental conditions on adsorption performance of MP@MoS 2 towards Cr(VI) and Pb(II) have been conducted by batch adsorption experiments. The prepared MP@MoS 2 exhibited high adsorption capacities (192.30 mg/g for Cr(VI) at pH 3.0 and 256.41 mg/g for Pb(II) at pH 6.0) and the adsorption equilibrium could be achieved in a short time. Moreover, MP@MoS 2 composites with high saturation magnetization could be simply separated under an external magnet. Combined experiments and spectral analysis, the underlying adsorption mechanism for Cr(VI) on MP@MoS 2 was mainly attributed to the reduction of Cr(VI) to Cr(III), and the removal of Pb(II) was due to the complexation with sulfur groups and amino-groups. Consequently, the prepared 3D flower-like structured MP@MoS 2 has a great potential for the practical application in removing Cr(VI) and Pb(II) from the aquatic environment.
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高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Wen Lu,Chen Wang,Wenhui Song,Zhixiong Zhang,Chengde Xie,Jianjun Wang
The heavy metal ion hexavalent chromium (Cr(VI)) in wastewater significantly threatens public health. Heterojunction photocatalysts typically demonstrate high reduction efficiency in water for Cr(VI) contamination. Overcoming the drawbacks of single metal organic frameworks (MOFs) or covalent organic frameworks (COFs), MOF@COF heterostructures inherit the advantages of large porosity, high surface area, and multiple active sites of single components. Herein, we report novel hybrid UiO-66-NH2@HDU-25 heterojunctions based on a condensation reaction. The optimal ratio of UiO-66-NH2@HDU-25 presented significantly superior photocatalytic activity to most reported MOFs and COFs due to heterojunction formation, which promoted charge separation. Under identical conditions, the optimally formulated UiO-66-NH2@HDU-25 could remove over 99% of Cr(VI), approximately 1.8 and 2.6 times the original UiO-66-NH2 and HDU-25 levels. Furthermore, the UiO-66-NH2@HDU-25 (8 : 1) heterojunction demonstrated favorable reusability and stability over five reaction cycles. Various experiments and density functional theory (DFT) calculations investigated the charge carrier transport pathways and possible photocatalytic mechanisms. The Z-scheme mechanism for the photocatalytic Cr(VI) reduction by UiO-66-NH2@HDU-25 was proposed and validated. This work aims to open new horizons for preparing novel photocatalyst heterojunctions with excellent visible light responsiveness for environmental water remediation.
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高影响因子
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