JOURNAL OF SOILS AND SEDIMENTS
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2022
·Vol. 22
·期 7
·2009-2021
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IF 3.536
Liu Quanfeng,Yu Jiang,Jiang Yinying,Zhong Chengwei,Ding Senxu,Zhou Peng,Jin Yuanxiao
Purpose Soil organic matter pollution is a serious threat to the human living environment. The purpose of this paper is to investigate the effect of MIL-101(Fe)/g-C 3 N 4 catalyzed peroxynitrite degradation of 2-chlorophenol in soil and to analyze the reaction mechanism and further to explore the optimal parameters of this reaction system with utilizing the mathematical model. Methods MIL-101(Fe)/g-C 3 N 4 was successfully obtained by hydrothermal synthesis method by growing MIL-101(Fe) on the surface of g-C 3 N 4 to catalyze the degradation of 2-CP (2-chlorophenol) in soil by sodium persulfate. The influence factors on the removal rate of 2-CP were analyzed by the response surface methodology (RSM) and combined with theoretical calculations. RSM can be used to model continuous variable surfaces with less data and determine the optimal level range. Results MIL-101(Fe)/g-C 3 N 4 had a good catalytic performance due to its good catalytic properties and the adsorption of g-C 3 N 4 on 2-CP in the system and made the best removal rate of 2-CP increase to 91.2%. The correlation of model fitting results was significant, and the verification of its optimal parameters yielded results with an error of only 4.1%. Conclusion Further studies revealed that SO 4 •− and • OH were the reactive radicals, and SO 4 •− was the dominant, which impelled Fe 2+ and Fe 3+ to interconvert in the complex system. Possible degradation pathways were derived by analyzing the intermediates. Generally, this experiment provides some ideas for future research of MOFs in soil organic pollutant removal systems. Graphical abstract
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Weixuan Wu,Weiqi Feng,Jingyu Bao,Xin Yang,Zhongfeng Shi,Jianmin Chen,Liqin Zhou,Zhenxia Zhao,Zhongxing Zhao
High detection stability makes sarcosine oxidase (SOx) nanozyme as natural enzyme substitute, a promising sensor for prostate cancer biomarker Sarcosine (Sar). However, its limited catalytic capacity towards product (H 2 O 2 ) and the following weak signal response significantly restrict the detection sensitivity of Sar. Herein, a novel NH 2 -MIL88B(Fe)-porphyrin/riboflavin (NM88B-POR/Rf) electrochemical sensor with a hyperoxia microenvironment and cascade reaction functions is proposed to promote catalytic H 2 O 2 production and cascade signal amplification (from H 2 O 2 to •OH). Fe-porphyrin implantation in NM88B-POR/Rf as bionic heme enhanced the O 2 -carrying capacity, thus effectively improving the sensor's utilization rate of dissolved oxygen and the catalytic H 2 O 2 production ability of Rf. Based on enzymatic cascade strategy, NM88B in NM88B-POR/Rf as peroxidase nanozyme further catalyzed H 2 O 2 to generate •OH. Methyl blue was used to capture •OH and enhance Sar detection sensitivity. Detection results revealed that NM88B-POR/Rf presented as low limit of detection (LOD) as 3.31 pM with detection range of 10 pM∼1 mM. The synergistic effect of the hyperoxia microenvironment and enzyme cascade make LOD about 4 orders of magnitude lower than reported state-of-the-art biosensors. Moreover, NM88B-POR/Rf has good selectivity and stability and hence also be applied to the detection of Sar in real urine.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2016
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IF 2.196
Pan Liang,Jie Wang,Zhi-Hong Liu
A pure zinc borate, Zn[B 12 O 14 (OH) 10 ], has been synthesized and characterized by XRD, FT-IR, simultaneous TG-DTA techniques, and chemical analysis. The molar enthalpy of solution of Zn[B 12 O 14 (OH) 10 ] (s) in 1 mol·dm −3 HCl(aq) was measured by microcalorimeter at T = 298.15 K. The molar enthalpy of solution of ZnO(s) in the mixture solvent of 2.00 cm 3 of 1 mol·dm −3 HCl(aq) and calculated amount of H 3 BO 3 was also measured. With the incorporation of the previously determined enthalpy of solution of H 3 BO 3 (s) in 1 mol·dm −3 HCl(aq), together with the use of the standard molar enthalpies of formation for ZnO(s), H 3 BO 3 (s), and H 2 O(l), the standard molar enthalpy of formation of −(9646.6 ± 9.6) kJ·mol −1 at T = 298.15 K was obtained on the basis of an appropriate thermochemical cycle. In addition, the molar enthalpy of formation of −9492.7 kJ·mol −1 for [B 12 O 14 (OH) 10 ] 2− has also been estimated by a group contribution method, which has been used to predict the Δ f H m θ of a series of transition metal borates of M[B 12 O 14 (OH) 10 ] (M II = Mn, Zn, Fe, Co, Ni). These estimated data have been used to further compare the stability of this series of transition metal borates.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Shuai Li,Yimei Zhang
Enhancing the energy efficiency of hydrogen evolution reaction (HER) represents a significant yet challenging goal. One promising approach to achieve this is developing catalysts with high activity and robust stability to couple HER with Fenton reaction. Herein, mesoporous nanosheet arrays (MNA) with featuring a mean pore size of 25 nm, was fabricated via a hydroxide precursor annealing strategy. The produced Co-P MNA 25 and Fe-Co-P MNA 25 are applied in HER and Fenton reaction, respectively. Compared to the MNA 12 synthesized by traditional method of self-growth and solid-phase phosphorization, the MNA 25 exhibited remarkable enhancement in performance, including a 49 % reduction in HER overpotential at 10 mA cm −2 , a 41 % increase in pseudo-first-order degradation kinetics of methylene blue in Fenton reaction, along with superior stability. In addition, the MNA 25 based flow reactor, which couples the two reaction and features a fastener-free design, demands just a minimal voltage of 1.61 V to drive, demonstrating impressive energy efficiency (81.56 % for HER and 2.77 g kWh −1 for Fenton) and application potential. More importantly, numerical simulations reveals that the larger pore size in MNA not only facilitated faster electrolyte diffusion, but also enhanced its impact buffer performance, thereby improving its catalytic activity and stability. Our work unveils the mechanism of mesopore size on the electrochemical performance of catalysts at the theoretical level, which offers a promising avenue for enhancing the energy efficiency of HER.
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Catalysts
·
2024
·Vol. 14
·期 6
·356
·
IF 3.8
Jing Xu,Songlin Zhu,Huizhi Zhou,Minghao Hou,Kangle Wan,Xueqi Zhang,Wei Yan,Yingcong Wei,Yuanping Chen
Metal–organic frameworks (MOFs) have recently gained attention as a highly promising category of photocatalytic materials, showing great potential in the degradation of organic dyes such as Rhodamine B (RhB). Nonetheless, the mono-metal MOF materials in this application are often constrained by their limited light absorption capabilities and their propensity for recombination with carriers. The combination of different metal-based MOFs to form heterogeneous reactors could present a promising approach for the removal of dyes from water. In this work, a new CAU-17/MIL-100(Fe) Z-scheme heterojunction photocatalyst composed of two MOFs with the same ligands is reported to realize the efficient degradation of dyes in water. The combination of the two MOFs results in a significant enhancement of the surface open sites, optical responsivity range, and charge-separating efficiency through synergistic effects. In addition, the capture experiments conducted on the photocatalytic process have verified that ∙O2−and h+are the primary active species. Consequently, CAU-17/MIL-100(Fe) exhibited excellent photocatalytic activity and stability. The degradation rate of the optimal CAU-17/MIL-100(Fe) photocatalyst was 34.55 times that of CAU-17 and 3.60 times that of MIL-100(Fe). Our work provides a new strategy for exploring the visible-light degradation of RhB in bimetallic MOF composites.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Rongbin Lin,Xiaoliang Zhang,Hai Li,Jinchun Tu,Cong Li,Zaowen Zhao,Weiwei Li,Lei Ding
Seawater electrolysis offers a viable strategy for the large-scale production of clean hydrogen. However, the oxygen evolution reaction (OER) catalysts is often compromised by the competitive chloride evolution reaction and the associated corrosion in seawater environments. Herein, we present a novel NiFe-S aerogel (AG) electrocatalyst featuring a porous 3D-network structure and a core–shell architecture. This catalyst demonstrates outstanding OER performance, achieving a low overpotential of 260 mV at 100 mA cm −2 , a Tafel slope of 55 mV dec -1 , and remarkable stability exceeding 500 h at 500 mA cm −2 in alkaline natural seawater. Through combined experimental and computational analyses, we discovered that the self-reconstructed crystalline-amorphous (Ni,Fe)OOH/NiFeS 2 heterojunction is pivotal to the outstanding performance of the NiFe-S AG electrocatalyst. The unique heterostructure facilitates electron transfer and down shifts the d-band center of the active sites, optimizing the adsorption strength of oxygen-containing intermediate species. Moreover, the stability is augmented by increased Fe and Ni vacancy formation energies, and higher affinity for OH – over Cl - , hence attenuating the corrosion from Cl - and suppressing the leaching of active sties. This work highlights the significance of the crystalline-amorphous heterojunction in aerogel catalyst and offers new insights into the design of efficient electrocatalysts for seawater oxidation.
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WATER RESEARCH
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2024
·
IF 11.4
Fangyuan Meng,Hui Tong,Chunhua Feng,Ziyuan Huang,Pan Wu,Jimei Zhou,Jian Hua,Fei Wu,Chengshuai Liu
Magnetite is a reductive Fe(II)-bearing mineral, and its reduction property is considered important for degradation of contaminants in groundwater and anaerobic subsurface environments. However, the redox condition of subsurface environments frequently changes from anaerobic to aerobic owing to natural and anthropogenic disturbances, generating reactive oxygen species (ROS) from the interaction between Fe(II)-bearing minerals and O 2 . Despite this, the mechanism of ROS generation induced by magnetite under aerobic conditions is poorly understood, which may play a crucial role in As(III) oxidation. Herein, we found that magnetite could activate O 2 and induce the oxidative transformation of As(III) under aerobic conditions. As(III) oxidation was attributed to the ROS generated via structural Fe(II) within the magnetite octahedra oxygenation. The electron paramagnetic resonance and quenching tests confirmed that O 2 •− , H 2 O 2 , and •OH were produced by magnetite. Moreover, density function theory calculations combined with experiments demonstrated that O 2 •− was initially formed via single electron transfer from the structural Fe(II) to the adsorbed O 2 ; O 2 •− was then converted to •OH and H 2 O 2 via a series of free radical reactions. Among them, O 2 •− and H 2 O 2 were the primary ROS responsible for As(III) oxidation, accounting for approximately 52 % and 19 % of As(III) oxidation. Notably, As(III) oxidation mainly occurred on the magnetite surface, and As was immobilized further within the magnetite structure. This study provides solid evidence regarding the role of magnetite in determining the fate and transformation of As in redox-fluctuating subsurface environments.
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PubMed
高影响因子
ANALYTICA CHIMICA ACTA
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2025
·
IF 6
Lei Hu,Junkai Hao,Ruhui Shang,Huitian Zhi,Xujie Wang,Yingchao Yang,Hanning Song,Chenxi Li,Juan Yu,Zhengquan Yan
Background Environmental safety and protection is accordingly one of the hottest issues to be concerned nowadays. Among all the chemicals to be monitored urgently, aminophenol and luminol are both quite hazardous but widely utilized in the fields of chemical industry, medicine, scientific research, chemical sensing, and so on. Although some reported ways could detect them satisfactorily, few reports could be found for portable visual monitoring and degradation of aminophenol and luminol, using only one sensor to judge the degradation degree as well. Results Fe-doped-Ce oxide modified chitosan fiber (Fe–Ce ox@CF) was developed by microwave-assisted hydrothermal method. By virtue of the excellent physical and chemical performance of carboxylated chitosan and its synergistic effect, Fe–Ce ox@CF possessed prominent oxidase-mimic activity to catalyze over 94 % luminescent luminol into dicarboxylic acid at room temperature. When utilized to accelerate the oxidization of ABTS, K m / V max were 0.0403 mM/2.327 × 10 −8 M s −1 . Especially, ultra-trace m -aminophenol ( m -AP) could exclusively alter the color of Fe–Ce ox@CF-ABTS from green to purple-red with remarkable visibility. Under the optimized conditions, there exhibited an excellent ratiometric colorimetric linear relationship between lg( A 515 / A 730 )/lg( A 515 / A 415 ) and c m -AP , and a fluorescent one between ΔF 427 and c luminol with detection limits (LOD) of 2.0 × 10 −9 M and 5.6 × 10 −9 M respectively. Especially, the red-green-blue (RGB) values got by a common smartphone also possessed good linear relationships with LODs of 1.7 × 10 −8 M and 1.34 × 10 −8 M. Significance This work represents the first oxidase-mimic based sensing system for potable and quantitative degradation of luminol and visual detection of m -aminophenol as well with the help of smartphones. It will also shed promising light on modified natural carbohydrate polymer-based sensors by non-destructive self-assembly and further application in practices.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Ying Jiang,Hao Lu,Lingli Lei,Daniel Scherman,Yingshuai Liu
The design of nanomedicines targeting specific tumor microenvironment (TME) characteristics, such as low pH, hypoxia, and elevated glutathione (GSH) concentration, holds significant potential for selectively killing cancer cells. In this study, we have developed a TME-responsive nanoparticle, i.e. , MIL-53(Fe)@MnO 2 stabilized with polyethylene glycol (FMP), which is capable of depleting GSH and sustainably generating hydroxyl radical (•OH) for enhanced chemodynamic therapy of cancer. After endocytosis, the FMP nanoparticles undergo gradual decomposition, resulting in GSH depletion while releasing Fenton-active Fe 2+ and Mn 2+ ions. These ions then subsequently catalyze a Fenton-like reaction to generate highly toxic •OH, ultimately inducing oxidative cell death. As a synergistic effect, the depletion of GSH further enhances therapeutic efficacy by inhibiting intracellular •OH scavenging. In vivo experiments demonstrated that this synergistically chemotherapeutic approach efficiently suppressed tumor growth without inducing significant systemic toxicity. This work presents a promising nanotherapeutic strategy that simultaneously depletes intracellular GSH and sustains cytotoxic •OH generation for enhanced tumor treatment.
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Journal of Energy Storage
·
2024
·
IF 8.9
Kai Lin,Zuming He,Long Shen,Jiangbin Su,Zhengyi Huang,Yongmei Xia,Yong Wang
Prussian blue analogues (PBAs) have attracted wide attention as cathode materials for sodium-ion batteries. Nevertheless, the poor cycle performance caused by the [Fe(CN) 6 ] 4− defects and Jahn-Teller (J-T) effect hinders its practical application. Here, Zn-substituted PBAs were synthesized through co-precipitation method and studied as cathodes for Na-ion batteries. The synthesized Na 1.14 Zn 0.39 Fe 0.61 [Fe(CN)₆]·4.14H 2 O (NZFC) and Na 1.18 Zn 0.42 Fe 0.58 [Fe(CN)₆]·4.96H 2 O (NZFE) showed outstanding exceptional electrochemical properties , including high capacity (first capacity of 114.56 and 97.76 mAh·g −1 at 10 mA·g −1 , respectively), excellent rate property (71.81 and 68.69 mAh·g −1 at 500 mA·g −1 , respectively), and cycling stability (64.72 % and 80.27 %, respectively) after 350 cycles at 200 mA g −1 , which is attribute to introduction of Zn element induced a weak Jahn-Teller effect and a low-spins and a high-spins Fe II /Fe III redox sites coordinated by C and N atoms prompt reversible diffusion of sodium ions and without structural transformation in the Na-ion storage. Using combined experiment and theory via ex situ X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations, it is confirmed that the weak J-T distortion contributes significantly to fast-overall kinetics, structural stability , and high electronic conductivity of the electrode. These findings provide new insights into comprehending for the future development of high-performance and stable sodium ion batteries .
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Jingyu Cai,Junjie Shi,Jian Zhang,Xiaoyu Miao,Sen Wang,Longqiang Xiao,Dan Liu,Linxi Hou
Electronic-grade isopropyl alcohol is widely utilized in the cleaning of semiconductors and microelectronic components. Removing ions like Pb2+ is crucial since the presence of impurities may cause degradation of electronics, increased failure rates, and short circuits. Membrane materials offer a number of advantages in the field of adsorption separation; however, the lack of adsorption sites results in limited adsorption capacity. In the current work, guanidino-grafted NH2-MIL-101(Fe) was incorporated into polyvinylidene fluoride (PVDF) to prepare MOF/PVDF mixed matrix membranes (NM/PVDF) for the removal of Pb2+ from isopropanol. Benefiting from the larger specific surface area and more lone electron pairs in the guanidine group, the Pb2+ adsorption capacity of the as-prepared NM/PVDF membrane was 29.4458 mg/g, which was higher than that of the NH2-MIL-101(Fe)/PVDF membrane (20.9306 mg/g) and the pure PVDF membrane (6.7324 mg/g). The NM/PVDF membrane was able to reduce the concentration of Pb2+ from 500 to 86.73 ppb. This work highlights the potential of guanidine-grafted Fe-based MOFs/PVDF membranes as adsorbents for acquisition of electronic-grade solvents.
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Journal of Energy Storage
·
2025
·
IF 9.8
Huan-Huan Liu,Rui-Yue Qi,Dong Xiang,Guo-Xian Yu,Hai-Feng Li,Jing Xiang
A stable 6-coordinate Fe III compound K[Fe III (THEED)] (H 4 THEED = N,N,N′,N′ -tetrakis(2-hydroxyethyl)ethylenediamine) was used as the anodic active material for all‑iron alkaline redox flow battery (ARFB), which shows a redox potential of E 1/2 = −0.93 V ( vs. Ag/AgCl). When it was paired with K 4 [Fe(CN) 6 ] as the cathodic counterpart, it gives a cell voltage of ∼1.3 V. Fe(THEED) exhibits the enhanced resistance to metallic iron deposition as compared with the 5-coordinate Fe-triethanolamine complex Fe(TEOA), mainly attributed to its saturated 6-coordinate structure with a large stabilization constant that effectively inhibits various side reactions. The cell performance of ARFB can be significantly improved by using Fe(THEED) as the negative active material. The ARFB containing 0.5 M Fe(THEED) and Fe(CN) 6 electrolytes demonstrated a discharge capacity of 14.59 Ah L −1 at a current density of 80 mA cm −2 , with a coulombic efficiency (CE) of 99.8 %, and an energy efficiency (EE) of 79.9 %. The peak power density can reach 194 mW cm −2 at a current density of 240 mA cm −2 . The system can exhibit exceptional cycling stability with 99.9 % capacity retention over 100 cycles (∼36 h). The low cost of Fe-THEED and Fe(CN) 6 components increases the economic viability, as compared to conventional V-based and previously reported Fe-based systems.
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