JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Heng Zhang,Mengfan Luo,Peng Zhou,Yang Liu,Ye Du,Chuanshu He,Gang Yao,Bo Lai
Recently, the enhancing role of hydrogen peroxide (H 2 O 2 ), a self-decay product of ferrate (Fe(VI)), on Fe(VI) reactivity has received increasing attention. In this study, we found that calcium peroxide (CaO 2 ) as a slow-releasing reagent of H 2 O 2 could also enhance the Fe(VI) performance for removing sulfamethoxazole (SMX). Compared with sole Fe(VI), sole CaO 2 and Fe(VI)-H 2 O 2 systems, the Fe(VI)-CaO 2 system showed higher reactivity to remove SMX. The radical scavenger and chemical probe test results indicated that the better oxidation performance of Fe(VI)-CaO 2 system than Fe(VI) alone was ascribed to the generation of Fe(Ⅳ) and Fe(Ⅴ) rather than • OH. In addition, the performance of Fe(VI)-CaO 2 system for degradation of contaminants was also superior to Fe(VI)-Na 2 SO 3 , Fe(VI)-NaHSO 3 and Fe(VI)-Na 2 S 2 O 3 systems under the same experimental conditions. Moreover, the effects of critical operating parameters, inorganic anions, inorganic cations, and humic acid on the degradation of SMX by Fe(VI)-CaO 2 system were revealed. The Fe(VI)-CaO 2 system exhibited good applicability in authentic water. Finally, the underlying degradation intermediates of SMX by Fe(VI)-CaO 2 system and their toxicity were confirmed. In conclusion, this study provides a new strategy for enhancing the oxidation capacity of Fe(VI) and comprehensively reveals the oxidation mechanism.
研究领域:
环境科学
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水处理技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Ji Shu,Xiping Xu,Yichong Zhang,Kanming Wang,Yuanxin Zhu,Xiran Lian,Hongyu Wang
This paper describes the ferrate(VI) (Fe(VI)) activation by mineral zincite for efficient micropollutants removal such as carbamazepine (CBZ). In the Fe(VI)-zincite activation system, the zincite stimulated the Fe(V) production and impelled the Fenton reaction by preventing the transformation of Fe(II), generated from the Fe(VI), to Fe(III). Furthermore, adducts formation between Lewis sites derived from zincite and Fe(VI) induced the generation of organic radical. The mechanism was unveiled via kinetic study, reactive species identification, Fe(VI)-zincite deposit characterization and CBZ degradation products detection. Results indicated that hydroxyl radical (•OH), Fe(V) and carboxyl radical (R-COO ) contribute to the CBZ degradation in Fe(VI)-zincite system and play different roles with pH change. The optimum application condition of [Fe(VI)]:[CBZ] = 5:1, [zincite] = 5 mg/L, the zincite particle size of 500–750 mesh and pH of 7.0 was further determined. Under this condition, 91% CBZ removal and 61% mineralization were achieved by the Fe(VI)-zincite system. The feasibility of Fe(VI)-zincite system for real condition was also evaluated. The CBZ removal and mineralization were decreased 6% and 8%, respectively, suggesting that Fe(VI)-zincite system was still highly effective for CBZ degradation in real natural water. Furthermore, amphoteric property of zincite contributed to the stability of pH in deficient buffering solution, ensuring the stability of reaction activity. Importantly, this study provided new insight into the Fe(VI) activation which was not achieved by the traditional introduced reducing substance, and has potential applications for micropollutant remediation in aquatic environment.
研究领域:
环境科学
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化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Yonglong Li,Wenming Liu,Ran Yan,Jian Liang,Tao Dong,Yangyang Mi,Peng Wu,Zheng Wang,Honggen Peng,Taicheng An
A series of hierarchical three-dimensionally ordered macroporous Fe 10-x V x binary metal oxides (3DOM-Fe 10-x V x ) catalysts were designed and synthesized for selective catalytic reduction of NO x from marine diesel engine exhaust. The physical-chemical performance of the 3DOM-Fe 10-x V x catalysts were subjected by various techniques and found that the 3DOM-Fe 10-x V x with the Fe to V atomic ratio of 9.0/1.0 exhibited a wider active temperature window, better soot resistance performance compared with the conventional Fe 9.0 V 1.0 catalyst due to its special 3DOM structure. Even when simultaneously exposed to the soot and high concentration of sulfur dioxide reaction feeds, the 3DOM-Fe 9.0 V 1.0 catalyst also displayed superior catalytic activity. Interestingly, we found that the soot had a reduction activity for NO x at high reaction temperature, which can effectively extend its active temperature window. The 3DOM-Fe 10-x V x catalysts prepared in this work could be potentially a good candidate for the cargo ships de NO x catalysts to satisfy the more stringent exhaust emission rules.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yin Li,Jiahui Hu,Yubin Zou,Lin Lin,Hebin Liang,Huaxin Lei,Bing Li,Xiao-yan Li
High-valent iron–oxo species (Fe V =O) generated through peroxide activation by Fe-based catalysts can realize the selective and efficient degradation of organic pollutants in water treatment. However, the rapid and efficient generation of Fe V =O for the selective degradation of pollutants over a wide pH range with high stability is challenging. In this study, a N, P, and S co-doped Fe-single atom (SA) catalyst (Fe SA -NPS@C) with FeN 4 active center was synthesized as a highly efficient catalyst for the peroxymonosulfate (PMS)-based oxidation. The Fe SA -NPS@C catalyst exhibited an excellent catalytic performance at low dosages of both the catalyst and PMS for the degradation of pollutants over a wide pH range with high stability. For the degradation of ofloxacin (OFX), the rate constant pertaining to PMS with Fe SA -NPS@C was 1.68 min −1 , considerably higher than those obtained using the N -doped and N and P co-doped Fe-SA catalysts. The degradation pathway of OFX revealed that the electrostatic effect was of significance in its degradation by Fe V N 4 =O with Fe V N 4 =O being the dominant reactive species. Density functional theory calculations revealed that the heteroatom doping effectively altered the electronic structure of the FeN 4 site of Fe SA -NPS@C, which strengthen its coordination with PMS, promote the electron transfer to PMS, and facilitate the interaction between Fe V N 4 = O and OFX, and thus significantly enhanced its catalytic activity. These findings provide new insights into the oxidation mechanism of Fe V =O in heterogeneous systems and the catalytic ability enhancement through heteroatom doping.
研究领域:
环境科学
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催化化学
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材料科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Zi-Ang Lu,Shan Jin,Tingting Qu,Ranran Liang,Yunchen Du,Mengxin Chen,Ping Xu
Conductive oxides with chemically distinct local environments are attractive for bifunctional water splitting because hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) impose different requirements on adsorption and charge transfer. Here, a descriptor-informed Fe/V co-doping strategy is proposed to regulate MoO 2 for photo-assisted electrocatalysis. Density functional theory (DFT) screening based on incorporation thermodynamics, local M–O bond mismatch, and near-Fermi-level electronic states identifies V as the most favorable dopant for lattice incorporation and Fe as the dopant that minimizes local bond-length mismatch while strongly perturbing the electronic structure. Guided by this complementarity, Mo 0.9 Fe 0.05 V 0.05 O 2 was synthesized and compared with pristine MoO 2 and single-doped controls. The co-doped catalyst preserves the MoO 2 framework and delivers the best overall performance, requiring 166 and 243 mV for HER and 253 and 281 mV for OER to reach 10 and 50 mA cm −2 under illumination. Electrochemical measurements reveal improved charge-transfer behavior and enhanced light-induced current response. Optical characterization and Finite-difference time-domain (FDTD) simulations indicate that the hollow architecture promotes optical-field localization, while DFT reaction energetics suggest site-dependent catalytic preferences, with V-associated environments favoring hydrogen adsorption and Fe-associated environments facilitating OER intermediate conversion. This study demonstrates that pairing dopants according to lattice compatibility and electronic perturbation is an effective route to activate MoO 2 for photo-assisted bifunctional water splitting. A descriptor-guided Fe/V co-doping strategy activates hollow MoO 2 for photo-assisted water splitting. Fe/V co-doping enables complementary HER/OER active sites, while the hollow architecture promotes optical-field localization and enhances interfacial charge-transfer kinetics under illumination. Download: Download high-res image (143KB) Download: Download full-size image
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DOI
PubMed
高影响因子
Journal of Materials Research and Technology-JMR&T
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2026
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IF 7.3
Jian-fa Jing,Shuai Wang,Yu-feng Guo,Feng Chen,Jinlai Zhang,Ling-zhi Yang,Guan-zhou Qiu
This study elucidates the influence of the CaO/MgO mass ratio and quaternary basicity (R 4 (CaO + MgO)/(SiO 2 /Al 2 O 3 )) on slag-phase evolution and element partitioning during electric-furnace smelting of pre-reduced vanadium titanomagnetite pellets. Thermodynamic calculations were employed to delineate a Ti-rich pseudobrookite-type slag domain that is amenable to subsequent acid-leaching processing for TiO 2 extraction. Smelting experiments under optimized conditions revealed that a balanced slag composition can simultaneously achieve high Ti enrichment in the slag and efficient Fe/V recovery in the metal phase, while suppressing the formation of CaTiO 3 . At 1600 °C with a holding time of 30 min and a carbon addition of 2 wt%, the combination of CaO/MgO = 0.5 and R 4 = 0.9 was identified as an optimal operating condition, yielding recovery rates of 99.82% for Fe, 93.12% for V, and 94.64% for TiO 2 . XRD and EPMA results show that the resulting slag is predominantly composed of anosovite, with subordinate diopside and magnesium titanium spinel, confirming the effective retention of Ti in the slag and the preferential partitioning of Fe and V into the metal phase. Collectively, these findings define a viable composition window for the design of acid-soluble titanium-bearing slags within the direct-reduction/electric-furnace processing route for vanadium titanomagnetite.
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DOI
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Kaijin Guo,Mingliang Li,Yahao Liu,Zhihui Zhu,Mengfei Wang,Xuewen Tang,Guangming Zhu
In the oxygen evolution reaction (OER), the lattice oxygen mechanism (LOM) has the potential to exceed the theoretical overpotential limit of approximately 370 mV associated with the traditional adsorbate evolution mechanism (AEM). Therefore, it is crucial to promote lattice oxygen involvement in the OER through careful design. We prepared a self-supported NiFeV hydroxide pre-catalyst electrode using a one-step electrochemical deposition method. Most of the V in the pre-catalyst dissolved during electrochemical activation, as confirmed by various ex situ and in situ characterization studies. The actual catalyst comprised V-doped FeOOH and NiOOH. Notably, significant oxygen vacancies were generated due to V element dissolution and leaching. The reconstructed catalyst can facilitate oxygen production via both the AEM and LOM, supported by theoretical calculations and experimental validation. It operates steadily for 750 hours at a current density of 50 mA cm−2, requiring only 200 mV and 253 mV overpotentials to achieve current densities of 10 mA cm−2 and 100 mA cm−2, respectively. This work elucidates the electrochemical reconstruction of V-containing hydroxides in alkaline media under anodic conditions while providing valuable insights into developing high-performance catalysts that involve the LOM.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Shuya Zhang,Qiming Chen,Qianqiao Wang,Xinyu Luo,Mingjun Cen,Wenchao Peng,Yang Li,Qicheng Zhang,Xiaobin Fan
The electrochemical oxygen reduction reaction (ORR) plays a crucial role in air-breathing energy conversion systems. However, its kinetics are constrained by a multistep proton-coupled electron transfer process, wherein the adsorption of the OOH* introduces high energy barriers. Herein, we present N-doped carbon-supported ultrafine V-incorporated Fe 3 C nanoparticles (V-Fe 3 C@NC) featuring abundant Fe coupling with V, serving as reaction sites for efficient ORR. Experimental characterizations confirm the incorporation of V species leads to a significant enhancement in ORR kinetics. The prepared V-Fe 3 C@NC electrocatalyst demonstrates exceptional ORR activity with a half-wave potential of 0.91 V. Density functional theory calculations elucidate that the synergy between Fe and V sites facilitates direct O–O bond breakage, circumventing the formation of the OOH* and resulting in lower ORR energy barriers. Moreover, the aluminum-air (Al-air) batteries derived from ultrafine V-Fe 3 C@NC nanoparticles display outstanding performance with a high open-circuit voltage of 1.92 V and a large specific capacity of 2309 mAh g −1 under the air environment. The elucidation and understanding of synergy in dual reaction sites present a novel approach for the rational design of supported metal nanoparticle electrocatalysts for energy-related applications.
研究领域:
材料科学
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电化学
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能源技术
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Lu-Lu Wang,Shun-Feng Jiang,Jing Huang,Hong Jiang
Oxygen-containing functional groups in functionalized biochar (BC) play an important role in its environmental applications. Herein, we introduced oxygen atoms into BC by copyrolysis of sawdust and magnesium carbonate basic pentahydrate (MgCO 3 ) 4 ·Mg(OH) 2 ·5 H 2 O for the preparation of O-enriched porous BC (OPBC). OPBC800 (OPBC pyrolyzed at 800 °C) exhibited ultrahigh activity to activate ferrate (K 2 FeO 4 ) for the oxidation of sulfadiazine (SDZ, 100% removal of SDZ in 2 min at pH = 5). We found that SDZ molecules can be rapidly adsorbed by the hierarchical porous structure of OPBC and were expediently oxidized by in situ generated Fe(IV) and Fe(V) active species on the surface of OPBC. The degradation mechanism of SDZ involved is quite different from the well-confirmed mechanism in which only active species in the solution play a role. Electrochemical impedance spectroscopy showed that O-doping in OPBC improved the electron-donating ability and expedited the electron transfer to ferrate, thus enhancing the catalytic activity of OPBC. This provides a new functionalization method for BC and provides more information about the activation of ferrate.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
高影响因子
WATER RESEARCH
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2026
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IF 12.8
Peijie Li,Jinchuan Lian,Xiaoxiang Cheng,Xinsheng Luo,Kunyu Chen,Congwei Luo,Ruimin Mu,Daoji Wu,Tao Yang
Although light-assisted ferrate (Fe(VI)) activation offers an activator-free strategy for micropollutant abatement, how visible light generates Fe(V)/Fe(IV) remains unclear at the molecular level. Here, five narrow-band LEDs (440–525 nm) were used to link Fe(VI) photochemistry with pollutant oxidation kinetics and iron-species contributions. At 440 nm, Vis-LED/Fe(VI) degraded 79.6–99.3% of six electron-rich micropollutants within 3 min, increasing rate constants by up to 4.3-fold relative to Fe(VI). Scavenging experiments and kinetic modeling identified Fe(V) and Fe(IV) as the dominant reactive species, together accounting for over 96% of diclofenac sodium (DCF) degradation. Time-dependent density functional theory calculations showed that visible excitation induced ligand-to-metal charge transfer (LMCT), which elongated a Fe-O bond from 1.654 to 2.025 Å and generated an Fe(V)-oxyl excited state that abstracted a hydrogen atom from water to give Fe(V). The apparent quantum yield of Fe(VI) decomposition decreased from 0.140 to 0.104 mol einstein −1 as wavelength increased from 440 to 525 nm, consistent with the charge-transfer component being photochemically productive. The system performance improved with light intensities and Fe(VI) concentrations, but declined under alkaline conditions and in humic-acid-rich water. These results establish visible-light activation of Fe(VI) via LMCT and identify Fe(V)/Fe(IV) as the oxidants responsible for micropollutant abatement.
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
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IF 9.028
Shuchang Wang,Yang Deng,Binbin Shao,Jiahui Zhu,Zixin Hu,Xiaohong Guan
For the first time, this study showed that the apparent second-order rate constants (kapp) of six selected emerging organic contaminants (EOCs) oxidation by Fe(VI) increased, remained constant, or declined with time, depending on [EOC]0/[Fe(VI)]0, pH, and EOCs species. Employing excess caffeine as the quenching reagent for Fe(V) and Fe(IV), it was found that Fe(V)/Fe(IV) contributed to 20–30% of phenol and bisphenol F degradation by Fe(VI), and the contributions of Fe(V)/Fe(IV) remained nearly constant with time under all the tested conditions. However, the contributions of Fe(V)/Fe(IV) accounted for over 50% during the oxidation of sulfamethoxazole, bisphenol S, and iohexol by Fe(VI), and the variation trends of kapp of their degradation by Fe(VI) with time displayed three different patterns, which coincided with those of the contributions of Fe(V)/Fe(IV) to their decomposition with time. Results of the quenching experiments were validated by simulating the oxidation kinetic data of methyl phenyl sulfoxide by Fe(VI), which revealed that the variation trends of kapp with time were significantly determined by the change in the molar ratio of Fe(V) to Fe(VI) with time, highlighting the key role of Fe(V) in the oxidative process. This study provides comprehensive and insightful information on the roles of Fe(V)/Fe(IV) during EOC oxidation by Fe(VI).
研究领域:
环境科学
·
化学动力学
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产品关联
DOI
PubMed
高影响因子
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