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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Pre-oxidized zerovalent iron creates reactive Fe(II) species for continuous self-driven depassivation: Implications for contaminant removal

Zimo Lou,Ludi Song,Xuanlong Zhang,Xiaofei Wen,Dong Cheng,Jianming Yu,Xinhua Xu

Exogenous ferrous ion dosing allows depassivation of aged zerovalent iron (ZVI) for industrial wastewater treatment, while sustaining the persistent existence of Fe(II) species for continuous depassivation throughout decontamination remains challenging. To tackle this dilemma, pre-oxidized microscale ZVI (poZVI bm ) is proposed via ball milling with peroxydisulfate (PDS) solids, for tailoring an “continuous self-driven depassivation” scenario with Fe 0 /Fe(II) symbiosis. The poZVI bm exhibits a 4.4 ∼ 19.0 times higher equilibrated adsorption capacity for hexavalent chromium (Cr(VI)) than the referenced ball milled ZVI (ZVI bm ) and other benchmarked mZVI composites (e.g. oxalated ZVI bm , sulfidized ZVI bm , and nanoscale ZVI), following a chemisorption-reduction process. It also demonstrates a 4.5 ∼ 18.7 folds faster surface area-normalized removal rate for nitrobenzene (NB) than all these counterparts, mediated by reductive transformation. Cr(VI) removal and NB reduction depend on the dissolved and surface-sorbed Fe(II), respectively, which can be optimized by regulating pre-oxidation degree of poZVI bm . The “continuous self-driven depassivation” of poZVI bm starts with the local microenvironment acidification due to the adsorption of abundant dissolvable Fe(II) over surface-located Fe(III), which drives continuous dissolution of Fe 0 core to create more reactive Fe(II), and therefore repeats the above procedure. Owing to wide pH adaptability (pH 3 ∼ 9) and impressive corrosion behavior of poZVI bm , these findings inspire the intimate integration of Fe 0 /Fe(II) component for high-efficient remediation of multicomponent industrial wastewater.

CAS / MDL: 7439-89-6 7775-27-1
研究领域: 环境科学 · 材料科学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-12 · IF 14.7

Iodine-induced self-depassivation strategy to improve reversible kinetics in Na-Cl2 battery

Feng Wenting,Wei Xinru,Yang Jianhang,Ma Chenyu,Sun Yiming,Han Junwei,Kong Debin,Zhi Linjie

Rechargeable sodium-chlorine (Na-Cl 2 ) batteries show high theoretical specific energy density and excellent adaptability for extreme environmental applications. However, the reported cycle life is mostly less than 500 cycles, and the understanding of battery failure mechanisms is quite limited. In this work, we demonstrate that the substantially increased voltage polarization plays a critical role in the battery failure. Typically, the passivation on the porous cathode caused by the deposition of insulated sodium chloride (NaCl) is a crucial factor, significantly influencing the three-phase chlorine (NaCl/Na + , Cl - /Cl 2 ) conversion kinetics. Here, a self-depassivation strategy enabled by iodine anion (I - )-tuned NaCl deposition was implemented to enhance the chlorine reversibility. The nucleation and growth of NaCl crystals are well balanced through strong coordination of the NaI deposition-dissolution process, achieving depassivation on the cathode and improving the reoxidation efficiency of solid NaCl. Consequently, the resultant Na-Cl 2 battery delivers a super-long cycle life up to 2000 cycles.

研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 29 ·14634-14643 · IF 11.301

Coexistence of humic acid enhances the reductive removal of diatrizoate via depassivating zero-valent iron under aerobic conditions

Chuan-Shu He,Rong-Rong Ding,Guan-Nan Zhou,Di He,Peng Fan,Xiao-Hong Guan,Yang Mu

Surface passivation is one of the most challenging aspects in the successful application of zero-valent iron (ZVI) for water decontamination, especially when oxygen is inevitably present. This study found that the coexistence of HA ranging from 0 to 40.0 mg-C/L appreciably improved the pseudo-first-order kinetic rate constant of pollutant diatrizoate (DTA) reduction by ZVI from 0.0454 to 0.1365 h−1 under aerobic conditions. For the first time, it revealed that the coexistence of HA could accelerate the reductive removal of organic contaminants via ZVI surface depassivation rather than the previously proposed electron-shuttle mechanism under aerobic conditions. Interestingly, both DTA removal and Fe0 consumption were found to undergo two stages in the presence of HA, with an initial slight enhancement attributed to the Fe(III)–HA complex formation partially suppressing iron precipitation, followed by a remarkable promotion arising from the HA-associated iron oxide detachment from the Fe0 surface. These findings not only provide a good strategy to enhance ZVI reactivity with minimal extra cost and complexity under aerobic conditions, but also help understand the ZVI behavior in practical applications.

研究领域: 环境科学 · 污染治理
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LANGMUIR · 2018 · IF 3.789

Reversible “Off–On” Fluorescence of Zn2+-Passivated Carbon Dots: Mechanism and Potential for the Detection of EDTA and Zn2+

Mingxi Yang,Qiuling Tang,Yang Meng,Junjun Liu,Tanglue Feng,Xiaohuan Zhao,Shoujun Zhu,Weixian Yu,Bai Yang

Zn2+-passivated carbon dots (named Z-CDs) were synthesized from zinc gluconate for the first time through a one-step pyrolysis treatment. The mechanism of Zn2+-enhanced fluorescence was carefully investigated, and a new strategy to passivate the surfaces of CDs by Zn2+ was proposed. Inspired by the complexation reaction between Zn2+ and ethylenediaminetetraacetic acid (EDTA), a reversible “off–on” fluorescent nanosensor for the detection of EDTA and Zn2+ was constructed based on the depassivation and repassivation of Z-CDs, with a limit of detection as low as 3.2 × 10–7 M and 5.1 × 10–7 M, respectively. The proposed Z-CD-based nanosensor had been further utilized for EDTA and Zn2+ monitoring in tap water with excellent recovery. To the best of our knowledge, this was the first report of a fluorescence-based sensor of EDTA and a turn-on sensor of Zn2+ based on CDs with reversible detection capability. Also, benefiting from the low toxicity of zinc, Z-CDs were applied for multicolor bioimaging and in vitro detection in cells.

研究领域: 材料科学 · 分析化学 · 纳米技术 · 环境科学 · 生物医学工程
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