Fe Se @C superlattice nanocrystals for peroxymonosulfate activation: Intrinsic nature of Fe spin state

Zhong, Qiang; Sun, Yue; Xu, Chenmin; Li, Yanfang; Sun, Dunyu; Wu, Leliang; Yang, Shaogui; Liu, Yazi; Qi, Chengdu; Xu, Zhe; He, Huan; Li, Shiyin; Wang, Zunyao; Wang, Shaobin

doi:10.1016/j.apcatb.2023.123113

Cited by 27 publications

(4 citation statements)

References 53 publications

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“…[ 24,30 ] The value of Fe 2+ /Fe 3+ increased from 1.01 to 1.15, which confirmed that Fe 2+ /Fe 3+ cycle participated in the degradation process, and speculated that Fe 3+ might continue to bind to HSO 5 − to form the precursor of Fe IV =O (Equations and ; Figure 6f). [ 7,41 ] XPS results further demonstrated that PMS could be effectively activated by electron transfer between variable metals to generate reactive species for pollutant degradation.

{normalO}_{normalv} + {HSO}_{5}^{-} \to {HSO}_{4}^{-} + {normalO}_{2}^{\cdot -}

Co (II) / Fe (II) + {HSO}_{5}^{-} \to + {SO}_{4}^{\cdot -} + {OH}^{-} + Co (III) / Fe (III)

Co (III) / Fe (III) + {HSO}_{5}^{-} \to {SO}_{5}^{\cdot -} + {normalH}^{+} + Co (II) / Fe (II)

Co (III) + Fe (II) \to Co (II) + Fe (III)

Fe (III) + {normalO}_{2}^{\cdot -} \to Fe (II) + {normalO}_{2}

Fe (III) + {HSO}_{5}^{-} \to

…”

Section: Resultsmentioning

confidence: 91%

“…[ 3,4 ] Compared to hydroxyl radicals (•OH, E 0 = 2.8 V, 10 −3 μs),

{SO}_{4}^{\cdot -}

possess higher redox potential ( E 0 = 2.5–3.1 V), superior rate constant (106–109 μ m −1 s −1 ), a longer half‐lifetime (30–40 μs) and a wide functioning pH range. [ 5–7 ] Peroxymonosulfate (PMS) is a kind of convenient carrying, storage and transportation of oxidant, there are a variety of materials that can be used to activate it. It is understood that the presence of multiple transition metals in the system may enhance the activation of PMS through intermetallic synergy.…”

Section: Introductionmentioning

confidence: 99%

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Boosting Peroxymonosulfate Activation via Co‐Based LDH‐Derived Magnetic Catalysts: A Dynamic and Static State Assessment of Efficient Radical‐Assisted Electron Transfer Processes

Yang,

Xia,

Shang

et al. 2024

Energy & Environ Materials

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Heterogeneous catalysts promoting efficient production of reactive species and dynamically stabilized electron transfer mechanisms for peroxomonosulfates (PMS) still lack systematic investigation. Herein, a more stable magnetic layered double oxides (CFLDO/N‐C), was designed using self‐polymerization and high temperature carbonization of dopamine. The CFLDO/N‐C/PMS system effectively activated PMS to remove 99% (k = 0.737 min−1) of tetracycline (TC) within 10 min. The CFLDO/N‐C/PMS system exhibited favorable resistance to inorganic anions and natural organics, as well as satisfactory suitability for multiple pollutants. The magnetic properties of the catalyst facilitated the separation of catalysts from the liquid phase, resulting in excellent reproducibility and effectively reducing the leaching of metal ions. An electronic bridge was constructed between cobalt (the active platform of the catalyst) and PMS, inducing PMS to break the O–O bond to generate the active species. The combination of static analysis and dynamic evolution confirmed the effective adsorption of PMS on the catalyst surface as well as the strong radical‐assisted electron transfer process. Eventually, we further identified the sites where the reactive species attacked the TC and evaluated the toxicity of the intermediates. These findings offer innovative insights into the rapid degradation of pollutants achieved by transition metals in SR‐AOPs and its mechanistic elaboration.

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{normalO}_{normalv} + {HSO}_{5}^{-} \to {HSO}_{4}^{-} + {normalO}_{2}^{\cdot -}

Co (II) / Fe (II) + {HSO}_{5}^{-} \to + {SO}_{4}^{\cdot -} + {OH}^{-} + Co (III) / Fe (III)

Co (III) / Fe (III) + {HSO}_{5}^{-} \to {SO}_{5}^{\cdot -} + {normalH}^{+} + Co (II) / Fe (II)

Co (III) + Fe (II) \to Co (II) + Fe (III)

Fe (III) + {normalO}_{2}^{\cdot -} \to Fe (II) + {normalO}_{2}

Fe (III) + {HSO}_{5}^{-} \to

…”

Section: Resultsmentioning

confidence: 91%

“…[ 3,4 ] Compared to hydroxyl radicals (•OH, E 0 = 2.8 V, 10 −3 μs),

{SO}_{4}^{\cdot -}

Section: Introductionmentioning

confidence: 99%

Boosting Peroxymonosulfate Activation via Co‐Based LDH‐Derived Magnetic Catalysts: A Dynamic and Static State Assessment of Efficient Radical‐Assisted Electron Transfer Processes

Yang,

Xia,

Shang

et al. 2024

Energy & Environ Materials

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“…It was previously reported that Fe x Se y phases can be tuned by the treating temperature when the annealing process is applied to synthesize iron selenides. − Accordingly, we designed a straightforward procedure to synthesize a series of multielement-doped Fe x Se y /CNT composites containing different iron selenide phases from a single priceless stainless-steel powder, and the synthesis scheme is shown in Figure A. A mixture of stainless-steel powder and CNT was ball-milled together and underwent a subsequent annealing process at specific temperatures, providing targeted Fe x Se y /CNT composites.…”

Section: Resultsmentioning

confidence: 99%

Multielement-Doped Fe_xSe_y/Carbon Nanotube Composites for High Performance Sodium-Ion Storage

Chen,

Shi,

et al. 2024

ACS Appl. Nano Mater.

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Fe x Se y -based composites have become very attractive anode materials for sodium-ion batteries due to their excellent electrochemical reversibility and the low price of iron resources. However, the unsatisfactory rate capacities and cycling stabilities continue to stimulate modification studies on synthetic strategies, crystal structure, morphologies, and composition structures. Here, we presented a straightforward synthetic route to a series of multielement-doped Fe x Se y /carbon nanotube (Fe x Se y /CNT) composites containing different ion selenide phases (Fe 3 Se 4 , FeSe 2 , and FeSe) from a single priceless stainless-steel powder. Among them, Fe 3 Se 4 /CNT exhibits the best rate capability and cycling stability with micron-scale sizing (250.0 mAh g −1 at 50 A g −1 and 338.6 mAh g −1 after 1600 cycles at 10 A g −1 ). The excellent sodium-ion storage properties of the Fe 3 Se 4 /CNT electrode could be attributed to the small subgrain size, abundant crystal boundaries, and amorphous regions in the composite structures caused by high-content multielement doping. The performance differences among the as-prepared composites containing various iron selenides lie in their intrinsic crystal structure characteristics. The practical application prospects of the Fe 3 Se 4 /CNT electrodes are also proved. The full cell assembled with Fe 3 Se 4 /CNT and Na 3 V 2 (PO 4 ) 2 F 3 /C displayed a high-rate capability of 368 mAh g −1 at 5 A g −1 and good capacity retention (about 100%) after 150 cycles.

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“…8–12 Various transition-metal oxide composites have been reported in PMS activation. 13–17 Among them, transition-metal oxides (Co 2+ , Fe 2+ , and so on) have garnered significant attention as their diverse chemical states and unoccupied orbitals facilitate electron transfer and generate reactive species within the M 3+ /M 2+ redox cycle. 13,15,18–20 Previous research has indicated that oxygen vacancies with abundant electrons facilitate the generation of ˙O 2 − , promoting the activation process.…”

Section: Introductionmentioning

confidence: 99%

Crystallinity regulation-induced organic degradation on ultra-thin 2D Co₃O₄/SiO₂ nanosheets: the critical trigger of oxygen vacancies

Bai,

Lu,

Liu

et al. 2024

Environ. Sci.: Nano

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Fe Se @C superlattice nanocrystals for peroxymonosulfate activation: Intrinsic nature of Fe spin state

Cited by 27 publications

References 53 publications

Boosting Peroxymonosulfate Activation via Co‐Based LDH‐Derived Magnetic Catalysts: A Dynamic and Static State Assessment of Efficient Radical‐Assisted Electron Transfer Processes

Boosting Peroxymonosulfate Activation via Co‐Based LDH‐Derived Magnetic Catalysts: A Dynamic and Static State Assessment of Efficient Radical‐Assisted Electron Transfer Processes

Multielement-Doped Fe_xSe_y/Carbon Nanotube Composites for High Performance Sodium-Ion Storage

Crystallinity regulation-induced organic degradation on ultra-thin 2D Co₃O₄/SiO₂ nanosheets: the critical trigger of oxygen vacancies

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Fe Se @C superlattice nanocrystals for peroxymonosulfate activation: Intrinsic nature of Fe spin state

Cited by 27 publications

References 53 publications

Boosting Peroxymonosulfate Activation via Co‐Based LDH‐Derived Magnetic Catalysts: A Dynamic and Static State Assessment of Efficient Radical‐Assisted Electron Transfer Processes

Boosting Peroxymonosulfate Activation via Co‐Based LDH‐Derived Magnetic Catalysts: A Dynamic and Static State Assessment of Efficient Radical‐Assisted Electron Transfer Processes

Multielement-Doped FexSey/Carbon Nanotube Composites for High Performance Sodium-Ion Storage

Crystallinity regulation-induced organic degradation on ultra-thin 2D Co3O4/SiO2 nanosheets: the critical trigger of oxygen vacancies

Contact Info

Product

Resources

About

Multielement-Doped Fe_xSe_y/Carbon Nanotube Composites for High Performance Sodium-Ion Storage

Crystallinity regulation-induced organic degradation on ultra-thin 2D Co₃O₄/SiO₂ nanosheets: the critical trigger of oxygen vacancies