JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Xingyun Hu,Xianjia Peng,Linghao Kong,Feng Zhu
The most toxic and mobile form of vanadium (V) is V(V). Thus, the oxidation of V is a subject of considerable importance since the process may increase environmental risks of V. V(IV) is known to be stable when pH < 4.5. However, in this study, stable V(IV) was oxidized almost completely in goethite suspension within 60 min at pH 2.0 and pH 4.0, correspondingly, only 25%–30% and 15%–20% of V(IV) were oxidized in equimolar Fe 3+ solution and the blank solution, respectively. The promoted oxidation of V(IV) by FeOOH is attributed to the formation of the complex, VO(OFe<) + or VO(OFe<) 2 . On the one hand, the formation of the complex caused higher pH in the interface of solid FeOOH and corresponding lower conditional potential of V(V)/V(IV) than those in bulk solutions, which facilitates the oxidation of V(IV). On the other hand, the surface group OFe < may serve as a medium that facilitating the electron transfer from V(IV) ions to dissolved oxygen molecules, also favoring the oxidation of V(IV). This study not only deepens our understanding of the transfer, transformation, and risk of V in environments, but also provides a reference to speculate the fate of similar elements in environments.
研究领域:
环境化学
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地球化学
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水污染控制
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金属形态转化
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界面过程
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124740
·
IF 7.5
Jinyu Chen,Wen Yu,Jixing Liu,Xiaoxia Chen,Yulun Gu,Jingwen Cui,Jiayi Wei,Haibo Chen,Hui Li
Natural iron (oxyhydr)oxides are increasingly recognized as important regulators of microplastics (MPs) transformation, yet their mechanistic influence on polymer photodegradation remains poorly understood. Here, we investigated how goethite (α-FeOOH) alters the photodegradation of polystyrene microplastics derived from disposable plastic spoons (Spoon-MPs) under simulated sunlight. Goethite increased Spoon-MP mass loss from 14.41% under light-only conditions to 21.78% after 12 d and increased the apparent degradation rate constant. Photodegradation induced pronounced physicochemical changes, including surface erosion, loss of structural order, molecular-weight reduction, and enhanced surface oxidation. Time-resolved FTIR and 2D-COS revealed distinct transformation sequences: aromatic-associated bands responded earlier under light-only conditions, whereas backbone C–H-associated bands responded earlier in the presence of goethite. EPR and scavenger experiments further showed enhanced generation of multiple reactive species, particularly •OH, supporting a greater contribution of hydrogen-abstraction-driven oxidation in the goethite system. GC–MS revealed increased relative abundances of low-molecular-weight oxygenated products, including ketone- and ester-containing compounds. DFT calculations identified aromatic and benzylic regions as intrinsically reactive sites, complementing the experimentally observed transformation patterns. Collectively, these findings demonstrate that goethite not only accelerates PS photodegradation but also alters the temporal sequence and relative importance of oxidative pathways, providing mechanistic insight into mineral-mediated transformation of microplastics in aquatic environments.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
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IF 11.3
Shaofu Huang,Man Chen,Youming Diao,Zihan Xie,Hao Lin,Lingyan Huang,Jiahuan Tang,Raymond Jianxiong Zeng,Shungui Zhou
Streaming potential generation through water flow in porous media represents an ancient and ubiquitous geophysical phenomenon. For centuries, this process has been regarded as merely a process of charge redistribution without involving any redox reactions. By using NO3– reduction as a model reaction, this study demonstrated for the first time that water flow drives abiotic denitrification associated with streaming potential generation. The nitrate (NO3–) reduction rate reached 10.6 μmol·L–1·d–1, which is comparable to that of FeS-driven chemical NO3– reduction (75.0–380 μmol·L–1·d–1) and significantly higher than that of photochemistry-driven NO3– reduction (0.1–1 μmol·L–1·d–1). Through monitoring of nitrogenous products and 15NO3– isotopic experiments, we showed that NO3– was selectively reduced to nitrogen (99%) via nitrite and nitrous oxide, confirming a denitrification process. Electron paramagnetic resonance (ESR) spectroscopy using DMPO as the probe detected the generation of hydrogen radicals (H•), which served as the reducing force for NO3– reduction. Using TEMPO as the electron probe, linear electron production was observed with an electron efficiency of 6.3% for NO3– denitrification. Moreover, H218O isotope experiments demonstrated that water oxidation is the ultimate electron source for NO3– reduction, indicating a chemical-free NO3– reduction process. An electric field strength of approximately 106 V/cm was detected using surface-enhanced Raman scattering, providing evidence of a strong interfacial electric field (IEF)-induced electron transfer process during water flow. This work reveals ubiquitous but long-overlooked redox reactions associated with streaming potentials. Water-flow-driven denitrification also highlights a newly identified abiotic NO3– elimination pathway, suggesting potent chemical-free NO3– remediation strategies.
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PubMed
高影响因子
Environmental Science-Processes & Impacts
·
2025
·
IF 3.9
Dan Luo,Sipei Yang,Haoyang Wang,Zhibin Wu,Xiaomin Gong,Yuan Yang,Yunshan Liang,Yaoyu Zhou
The fractionation of extracellular polymeric substances (EPS) on mineral surfaces alters their composition and reactivity, thereby influencing heavy metal behavior in the environment. However, the molecular-level mechanisms governing how this process affects metal-binding properties remain unclear. Hence, this study combined multispectral techniques and chemometrics to investigate the adsorptive fractionation of EPS on mineral and its impact on heavy metal binding. Excitation–emission matrix coupled with parallel factor analysis (EEM-PARAFAC) demonstrated that aromatic and protein-like components were preferentially adsorbed on hematite (Hema) and goethite (Goet). Two-dimensional correlation spectroscopy (2D-COS) further indicated that protein-like substances were adsorbed prior to fulvic-like substances, following the sequence: tyrosine-like > tryptophan-like > fulvic-like substances. Notably, the fractionation process altered the binding affinity and order of Cu2+ to EPS components. Adsorption onto Hema reduced the copper-binding affinity of EPS, whereas adsorption onto Goet enhanced it. This difference was maybe attributed to changes in carboxyl and polysaccharide groups within the EPS. This study elucidates the influence of EPS fractionation on mineral surfaces regarding heavy metal binding at the molecular level. These findings enhance our understanding of the biogeochemical behavior of heavy metals in the presence of mineral-organic composites across aquatic and terrestrial ecosystems, providing a theoretics foundation for environmental remediation.
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PubMed
高影响因子
RSC Advances
·
2026
·Vol. 16
·期 18
·16505-16511
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IF 6.1
Cong Gao,Houfen Li,Jize Liu,Wenchao Yang,Hong Chen,Jianbo Han
The heterogeneous Fenton-like reaction is a promissing technology for removing organic pollutants in water. The reduction of Fe(III) to Fe(II), as the rate-limiting step for generating ˙OH, is crucial in heterogeneous Fenton-like reactions and may be improved using organic pollutants with lower redox potential than that of Fe(III)/Fe(II). In this work, the rapid reduction of Fe(III) to Fe(II) on the MIL-100-Fe catalyst was achieved by degrading methylene blue (MB, E0 = 0.01 V), which has the desired lower redox potential than that of MIL-100-Fe(III)/Fe(II) (E0 = 0.76 V). By contrast, organic pollutants with higher redox potentials than that of MIL-100-Fe, such as phenol (E0 = 0.97 V) and p-nitrophenol (E0 = 1.23 V), were incapable of reducing Fe(III) to Fe(II). As a result, the degradation rate constant of MB was one order of magnitude higher than those of phenol and p-nitrophenol. Notably, MB could also promote the reduction of Fe(III) to Fe(II) in the presence of phenol or p-nitrophenol; thus, the degradation rate constants of phenol and p-nitrophenol were significantly enhanced by 50 and 30 times, respectively. The results revealed that organic pollutants with lower redox potential than that of Fe(III)/Fe(II) could facilitate the reduction of Fe(III) to Fe(II), which is beneficial for producing more ˙OH, thus improving the heterogeneous Fenton-like catalytic performance.
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高影响因子
CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Baisheng Ma,Jincheng Li,Yan Zhu,Kewei Wang,Boyan Sun,Ke Ren
In this paper, the reactive flash sintering method was adopted to synthesize a series of Li x (CoCrFeMnNi)O y oxides with x in the range of 0–1. The phase compositions and electrical conductivities of the oxides at different Li incorporation level were characterized. A single phase of spinel structure ( Fd-3m ) was obtained for the sample (CoCrFeMnNi) 3 O 4 . With incorporation of Li, the phase transformed into Rock-salt structure ( Fm-3m ) and then layered structure ( R-3m ). The ionic and electronic conductivities of the samples were characterized by impedance spectrometry. The ionic and electronic conductivities of the samples decreased with increasing Li incorporation level at first along with the spinel to Rock-salt structure transformation, and then increased with further increasing Li incorporation level along with the Rock-salt to layered structure transformation.
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Journal of Materiomics
·
2023
·
IF 9.4
Fangze Chen,Dacheng Zhou,Xueqing Xiong,Juntao Pan,Donglin Cai,Ze Wei,Xiyong Chen,Yihui Liu,Nengneng Luo,Jialin Yan,Toyohisa Fujita
A series of single-phase double perovskite Pr 1- x Gd x BaCo 2- y Fe y O 5+ δ ( x = 0, 0.5 and 1, 0 ≤ y ≤ 1) materials were engineered through A/B site co-doping strategy to improve the mechanical, electrical and electrochemical properties as potential cathode materials for the application of intermediate solid oxide fuel cells (IT-SOFCs). The corresponding thermochemical stability, thermal expansion behavior, electrical conductivity and cathodic polarization resistance of the materials were systematically investigated. It was found that the A-site dual lanthanide doped Pr 0.5 Gd 0.5 BaCo 2 O 5+ δ (PGBCO) exhibits improved electrical conductivity, reduced thermal expansion, and comparatively low electrochemical polarization resistance versus single lanthanide double perovskite, PrBaCo 2 O 5+ δ (PBCO) and GdBaCo 2 O 5+ δ (GBCO) materials. Further investigation on the effect of B-site Fe-doping on Pr 0.5 Gd 0.5 BaCo 2- y Fe y O 5+ δ (PGBCF- y , 0 ≤ y ≤ 1) reveals that all the PGBCF- y compositions exhibit excellent chemical stability with Gd-doped ceria (GDC) at operating temperatures not higher than 1 100 °C. Besides, doping of Fe in B-site can effectively reduce the thermal expansion coefficients (TECs) of the Pr 0.5 Gd 0.5 BaCo 2 O 5+ δ ceramics at 30–1 000 °C. And the electrochemical impedance spectra (EIS) results show that the PGBCF- y |GDC| PGBCF- y symmetric cells have acceptable low area specific polarization resistances. Further examination of the cathodic polarization and characteristic capacitance from the AC impedance spectra by employing the relaxation time distribution (DRT) method demonstrated that charge transfer is the dominating sub-process for the oxygen transport through the materials.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiaoyang Li,Jiahang Liu,Ruolin Lv,Yingying Chu,Lu Lv,Junhe Lu,Weiming Zhang
Self-quenching of radicals and their non-selective attack on co-existing substrates result in the low oxidant utilization efficiency in Fenton and Fenton-like systems. Herein, we developed a novel octahedral carbon-encapsulated zirconium oxide catalyst (ZrO 2 -C) featured by large specific surface area (219.5 m 2 /g), highly-dispersed sub-5 nm active sites, and strong metal-support interactions. The catalyst shows outstanding performance for peroxymonosulfate (PMS) activation, and a two-step catalytic mechanism is proposed. First, it interacts with PMS via inner-sphere coordination to form a metastable surface complex (Stage I); then, the reactive complex reacts with selected molecules via oxygen-atom-transfer route (Stage II). Surprisingly, only 1.21 PMS molecules was consumed for each molecule of carbamazepine (CBZ), almost close to the stoichiometric ratio. Based on a quantitative structure–activity relationship between the reaction rates and the molecular structures of fourteen substituted phenols, we demonstrated that this catalytic process was highly selective towards electron-rich compounds, that is, only those organics with E HOMO values higher than ca. −6.52 eV could be oxidized. Overall, this study provides mechanistic insights into the catalytic selectivity of Zr-based catalysts and advances their further application in Fenton-like systems.
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Advanced Electronic Materials
·
2023
·Vol. 9
·期 5
·2201243
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IF 6.2
Fangzhe Li,Hongjun Zhang,Huijiadai Luo,Miao Xing,Lu Cao,Chunlong Wu,Yongchun Zou,Dechang Jia,Yu Zhou,Yong Huang,Hua Ke
Dielectric tunability is widely used in numerous electronic devices, including wavelet filters, lens antennae, and varactors. However, a dielectric device often has only one tunable dielectric constant range, confining the integration of a multi-frequency electronic circuit. Herein, a new kind of dielectric tunable textured BaTi 0.99 Fe 0.01 O 3− δ ceramics with micro-twin boundaries is proposed for the dual-channel controllable dielectric constants. The relative tunability with the acceptable figure of merit is as large as 76% in the crossover channel, which is superior to that of the most state-of-the-art Ba x Sr 1 − x TiO 3 counterparts. This new design strategy offers the possibility of dual-channel filters in one dielectric device controlled by external electric fields. The required external electric field is moderate with the help of reversible micro twins, which is confirmed by first-principles studies. The static magnetic field interference on the dielectric constant is also evaluated, showing the frequency stability of dielectric tunability in a range between 5k and 1 m Hz.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Meiqi Zhang,Yijie Yang,Luo Feng,Xiaoqi Sun
Near infrared reflective inorganic pigment YIn 1-x-y Mn y Fe x O 3 (x/y = 0.1–0.5) was prepared by solid state reaction. The X-ray diffraction analysis and CIE1976 L*a*b* colorimetric analysis reveal that the main phase of the sample is changed from YInO 3 phase to YFeO 3 phase and the color of the sample is changed from blue to black (x ≥ 0.4) with the increase of iron content. The brightness value of black pigment ranges from 23.27 to 32.12. When In 3+ is replaced by Fe 3+ and Mn 3+ , the band gap of the black sample is decreased from 1.73eV to 1.39eV. The near-infrared reflectance (R) and near-infrared solar reflectance (R*) of the sample reach the maximum when x = 0.4 and y = 0.1, which are 77.82% and 53.44%, respectively. YIn 1-x-y Mn y Fe x O 3 (x = 0.4–0.5, y = 0.1–0.5) black samples have higher near infrared reflectivity than common commercial black pigments. In the thermal insulation study, under the condition of infrared irradiation for 90 min, the internal air temperature difference between the iron car model coated with YIn 0.5 Mn 0.1 Fe 0.4 O 3 pigment and the iron car model coated with commercial iron black pigment can reach 7 °C. YIn 0.5 Mn 0.1 Fe 0.4 O 3 black pigment was soaked in 5% acid-alkali solution for 24 h, the chromaticity was almost unchanged before and after immersion, indicating that the sample has good chemical stability. The above properties show the potential of synthetic black pigments in the field of energy conservation.
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高影响因子
FUEL
·
2023
·
IF 7.4
Qihuang Huo,Yahui Wang,Huijun Chen,Yu Feng,Lina Han,Weiren Bao,Liping Chang,Jiancheng Wang,Kechang Xie
It is a win–win strategy to prepare mercury sorbents from low-cost high-sulfur raw materials. In part 1, mercury sorbents with excellent performance were prepared from high inorganic sulfur coal through KOH activation. However, this method does not work for high organic sulfur coal. In this work, a two-step preparation method is developed to prepare mercury sorbents from high organic sulfur coal. The first step is the co-pyrolysis/carbonization of Fe 2 O 3 and coal, during which organic sulfur in coal is converted into FeS x . XPS shows that the percentage of S x 2– /S on the surface of the carbonized samples gradually increases from 5.4% to 22.2% with the m(Fe):m(S o ) ratio from 0:4 to 5:4. The second step is KOH activation, and it converts FeS x into various S species, including C-S, S 0 , S 2 2− and S 2− . Among the prepared mercury sorbents, LF+3Fe/4S-A (m(Fe):m(S o ) = 3:4) shows the best mercury removal performance, and its mercury removal efficiency remains above 84% for 120 min under N 2 +O 2 at 120 °C. The Hg-TPDD and XPS results indicate that S*, including C-S, S 0 and S 2 2− , are the major active sites for mercury removal rather than Fe element, and HgS is the main existing form of mercury on the used sorbents. Besides LF coal, this two-step process is also applicable to other high organic sulfur coals (such as LL coal, WJZ coal, and SY coal) and high-sulfur petroleum coke.
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高影响因子
Journal of Energy Storage
·
2023
·
IF 9.4
Fei Cheng,Yang Xu,Jinheng Zhang,Lin Wang,Huanhuan Zhang,Qi Wan,Shuai Xu,Wanpeng Li,Lei Wang,Zhaohui Huang
Aiming at solid waste resources reuse and energy saving issue, a novel flexible paraffin/carbon fiber@carbon nanotubes (Paraffin/CF@CNTs) composite PCM was prepared in this study. In the flexible composite PCM, CNTs grew in-situ surrounding by recycled CF trunk via chemical vapor deposition to construct the fiber net-structure utilized as the supporting material, and paraffin as a thermal energy storage material was absorbed into spongy CF@CNTs by vacuum impregnation methods. The prepared Paraffin/CF@CNTs composite has a best solid-liquid phase change latent heat of 81.94 Jg −1 after solid-solid phase transition with 15.28 Jg −1 , and still keep the high latent heat retention of 99.4 % even after being subjected to 300 melting/freezing cycles. The thermal conductivity of Paraffin/CF@CNTs composite (1.551 Wm −1 K −1 ) is enhanced by up to 573 % than that of pure paraffin, while this composite exhibits the good thermal stability that it decomposes over 215.6 °C with totally 51.9 % mass loss. Overall, the novel flexible Paraffin/CF@CNTs composite PCM behaves very stable performances in structure, chemical component, thermal storage and thermal stability, looking promising for applications in electronic device temperature control, near-infrared stealth, smart wear and textile industries.
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