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CHEMOSPHERE · 2024 · IF 8.1

Iron-based materials functionalized with carbon and phosphorus recovered from sludge enhanced the formation of stable minerals to passivate lead and chromium in wastewater and soil

Liyan Wang,Bojie Jia,Zedong Teng,Hao Cao,Yanli Miao,Huiyuan Guo,Tinggang Li

The bioaccumulation and toxicity of heavy metals are serious threats to human activities and ecological health. The exploitation of environmentally friendly passivated materials is major importance for the remediation of heavy metal contaminated soil. This research developed a new type of environmental functional material with a core-shell structure, which is an iron-based material functionalized with phosphorus and carbon from sludge for heavy metal pollution remediation. The results indicated that the C/P@Fe exhibits excellent heavy metal removal ability, and the maximum removal rates of the two heavy metals in simulated wastewater could reach 100% under optimum reaction conditions. It also effectively converts the labile Cr/Pb into the stable fraction after 28 days of incubation, which increased the maximum residual fraction percentage of Cr and Pb by 32.43% and 160% in soil. Further analysis found that the carbon layer wrapped around the iron base could improve the electron transport efficiency of reducing iron, phosphorus and ferrum could react with heavy metal ions to form stable minerals, such as FeCr 2 O 4 , FeO·Cr 2 O 3 , Pb 5 (PO 4 ) 3 OH, PbCO 3 , 2PbCO 3 ·Pb(OH) 2 and PbS, after reacting with C/P@Fe. The study demonstrated that the Iron-based materials functionalized with carbon and phosphorus from sludge provided a more efficient way to remove heavy metals.

CAS / MDL: 7705-08-0 10099-74-8
研究领域: 环境科学 · 材料科学
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Catalysts · 2023 ·Vol. 13 ·期 7 ·1057 · IF 3.9

Oxygen-Vacancy-Rich Fe@Fe3O4 Boosting Fenton Chemistry

Rongwei Zheng,Ruifan Tan,Yali Lv,Xiaoling Mou,Junqiao Qian,Ronghe Lin,Ping Fang,Weidong Kan

Iron-based materials are widely applied in Fenton chemistry, and they have promising prospects in the processing of wastewater. The composition complexity and rich chemistry of iron and/or oxides, however, hamper the precise understanding of the active sites and the working mechanism, which still remain highly controversial. Herein, iron oxides of four different model systems are designed through a conventional precipitation method plus H2reduction treatment. These systems feature Fe@Fe3O4with abundant oxygen vacancy, Fe0and Fe3O4particles with interface structures, and Fe3O4-dominated nanoparticles of different sizes. These materials are applied in the decomposition of methyl orange as a model reaction to assess the Fenton chemistry. The Fe@Fe3O4with core–shell structures exhibits significantly higher decomposition activity than the other Fe3O4-rich nanoparticles. A thin Fe3O4layer formed by auto-oxidation of iron particles when exposed to air can boost the activity as compared with the Fe0and Fe3O4particles with interface structures but poor oxygen vacancy. The unique hetero-structure with the co-existence of both metallic iron and oxygen vacancy displays excellent redox propensity, which might account for the superior Fenton activity. This finding provides a new perspective to understand and design highly efficient iron-based Fenton catalysts.

研究领域: 环境科学 · 材料科学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Robust Activity and Stability of P-Doped Fe–Carbon Composites Derived from MOF for Bromate Reduction

Li Long,Xuechun Wang,Heyun Fu,Xiaolei Qu,Shourong Zheng,Zhaoyi Xu

Iron-based materials are effective for the reductive removal of the disinfection byproduct bromate in water, while the construction of highly stable and active Fe-based materials with wide pH adaptability remains greatly challenging. In this study, highly dispersed iron phosphide-decorated porous carbon (Fe2P(x)@P(z)NC-y) was prepared via the thermal hydrolysis of Fe@ZIF-8, followed by phosphorus doping (P-doping) and pyrolysis. The reduction performances of Fe2P(x)@P(z)NC-y for bromate reduction were evaluated. Characterization results showed that the Fe, P, and N elements were homogeneously distributed in the carbonaceous matrix. P-doping regulated the coordination environment of Fe atoms and enhanced the conductivity, porosity, and wettability of the carbonaceous matrix. As a result, Fe2P(x)@P(1.0)NC-950 exhibited enhanced reactivity and stability with an intrinsic reduction kinetic constant (kint) 1.53–1.85 times higher than Fe(x)@NC-950 without P-doping. Furthermore, Fe2P(0.125)@P(1.0)NC-950 displayed superior reduction efficiency and prominent stability with very low Fe leaching (4.53–22.98 μg L–1) in a wide pH range of 4.0–10.0. The used Fe2P(0.125)@P(1.0)NC-950 could be regenerated by phosphating, and the regenerated Fe2P(0.125)@P(1.0)NC-950 maintained 85% of its primary reduction activity after five reuse cycles. The study clearly demonstrates that Fe2P-decorated porous carbon can be applied as a robust and stable Fe-based material in aqueous bromate reduction.

研究领域: 环境科学 · 材料科学
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Energy Technology · 2020 ·Vol. 8 ·期 10 ·2000544 · IF 3.404

Hierarchical Fe3O4@FeS2 Nanocomposite as High-Specific-Capacitance Electrode Material for Supercapacitors

Xuexia Liu,Limin Liu,Weiwei Yan,Yinfeng Wang,Chunfang Huang,Zhijun Wang

Iron-based materials are ideal faradaic electrodes for supercapacitors. However, boosting the specific capacitance and preparation with the simple method of iron-based materials remains a great challenge. Herein, hierarchical Fe 3 O 4 @FeS 2 nanocomposites are constructed through an annealing strategy with monohydrate ferrous sulfate as the precursor. X-ray diffractometry, high-resolution transition electron, and X-ray photoelectron spectroscopy results reveal that the hierarchical Fe 3 O 4 @FeS 2 nanocomposite is successively fabricated. The as-prepared materials exhibit a remarkable specific capacitance of 597.1 F g −1 at a current density of 3 A g −1 as electrode materials of supercapacitors. Inspiringly, specific capacitance is superior to most iron-based electrodes in previous reports. This may be ascribed to the junction at the interface of the different components and the efficient electron transfer of FeS 2 . This work is meaningful for the design and preparation of electrode materials with specific capacitance.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Highly efficient removal of hexavalent chromium from electroplating wastewater by ferrous/ferric hydroxide complex: From lab-scale to pilot-scale study

Xiaoqing Lin,Longqian Xu,Zhenyu Zhao,Shanshan Liu,Jiaming Zhang,Deli Wu

Low electron-transfer efficiency and cumbersome processes are widely known to negatively affect the application of Fe-based materials for treating electroplating wastewater. In this study, ferrous/ferric hydroxide complex (FHC) was successfully synthesized to greatly improve the electron-transfer efficiency for Cr(VI) removal; meanwhile, the effect of the interlayer type on Cr(VI) removal and the possible removal mechanisms were well investigated. The sulfate interlayer of FHC was shown to strongly promote Cr(VI) removal, with 10.4 % and 29.0 % improvements over those achieved by chloride and carbonate interlayers, respectively, in close association with the amounts of surface structural Fe(II), surface –OH, and adsorbed water. The initial pH value was demonstrated to exert almost no effect on Cr(VI) removal by FHC(SO 4 2− ) owing to the buffering effect of the surface –OH. These results were different from some previously reported Cr(VI) removal of Fe-based materials. Moreover, the results of characterization and lab-scale experiments indicated that most of Cr(VI) binds rapidly with the surface –OH owing to electrostatic attraction. The peak at 618 cm −1 in the FT-IR spectra shifted to 549 cm −1 and new peaks at 576.79 and 586.39 eV in the XPS spectra were observed after the reaction, which was attributed to the formation of CrOOH and FeCr 2 O 4 owing to reduction and coprecipitation. Pilot-scale experiments revealed that the chemical cost and sludge yield during the FHC process decreased by 71.3 % and 54.1 %, respectively, compared with those in the NaHSO 3 process. These findings provide new insight for utilizing different interlayers to improve the reactivity of FHCs in remediating electroplating wastewater containing Cr(VI).

研究领域: 环境科学 · 化学工程
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Small · 2021 ·Vol. 17 ·期 7 ·2007334 · IF 13.281

Engineering Bimetallic NiFe-Based Hydroxides/Selenides Heterostructure Nanosheet Arrays for Highly-Efficient Oxygen Evolution Reaction

Caichi Liu,Yu Han,Libing Yao,Limin Liang,Jiayin He,Qiuyan Hao,Jun Zhang,Ying Li,Hui Liu

Developing cost-effective and high-efficiency electrocatalysts toward alkaline oxygen evolution reaction (OER) is crucial for water splitting. Amorphous bimetallic NiFe-based (oxy)hydroxides have excellent OER activity under alkaline media, but their poorly electrical conductivity impedes the further improvement of their catalytic performance. Herein, a bimetallic NiFe-based heterostructure electrocatalyst that is composed of amorphous NiFe(OH) x and crystalline pyrite (Ni, Fe)Se 2 nanosheet arrays is designed and constructed. The catalyst exhibits an outstanding OER performance, only requiring low overpotentials of 180, 220, and 230 mV at the current density of 10, 100, and 300 mA cm −2 and a low Tafel slope of 42 mV dec −1 in 1 m KOH, which is among the state-of-the-art OER catalysts. Based on the experimental and theoretical results, the electronic coupling at the interface that leads to the increased electrical conductivity and the optimized adsorption free energies of the oxygen-contained intermediates plays a crucial role in enhancing the OER activities. This work focusing on improving the OER performance via engineering amorphous-crystalline bimetallic heterostructure may provide some inspiration for reasonably designing advanced electrocatalysts.

研究领域: 材料科学 · 电化学 · 能源转换与储存
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CARBON · 2020 · IF 8.821

Fe-based material@N-doped carbon composites as environment-friendly microwave absorbers

Qingwei Liu,Min Zeng,Jue Liu,Baiyu Guo,Xiaozhu Hao,Qian Cao,Yuchen Shang,Xin Sun,Jinzhang Liu,Xuexu Gao,jiheng Li,Jie Zhu,Xixiang Zhang,Ronghai Yu

Environment-friendly Fe-based material@N-doped carbon nanoparticles imbedded in polylactic acid (PLA) matrix are prepared and applied in microwave absorption field. In the synthesis process, polydopamine (PDA) in the precursor could rationally regulate the phases of the iron-based particles and carbon contents. It turns out that optimizing the chemical composition plays a vital role in modulating microwave absorption performance . For instance, the maximum reflection loss ( R Lmax ) for Fe@N-doped carbon particles (S-120) reaches −61.6 dB (12.56 GHz, 2.1 mm), and the effective bandwidth is 4.48 GHz (from 13.52 GHz to 18 GHz) with a thickness of only 1.7 mm. The excellent microwave absorption performance could be attributed to perfect impedance matching brought by the synergies of multiple components. Moreover, the microwave absorbers display not only high microwave absorption performance but also environment-friendly characteristics that can avoid leaving stubborn waste after failure. The preparation process of the composite is pollution-free and the PLA in the composite can almost be naturally degraded within one month under simulated marine environment. This work may provide a new perspective on preparing high-efficient functional materials which are also harmless to the environment.

CAS / MDL: 77-86-1
研究领域: 材料科学 · 环境科学
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CERAMICS INTERNATIONAL · 2018 · IF 3.057

Facile synthesis of hierarchical polycystic iron-nitride/phosphide hybrids microsphere constructed by CNTs for stable and enhanced lithium storage

Peng Jing,Qiong Wang,Boya Wang,Mingwu Xiang,Hongjun Jiang,Yin Zhang,Yunhong Wei,Yun Zhang,Hao Wu,Heng Liu

Diverse Fe-based nitrides and phosphides have drawn considerable attention owing to their abundant source, high theoretical capacities, and environment benignity. However, it still remains a crucial challenge to develop a facile preparation approach of robust Fe-based anode materials for the next-generation durable lithium-ion batteries. Herein, we constructed two type polycystic microsphere anode materials (Fe 2 N@C/CNTs and FeP@C/CNTs) through a scalable industrial spray-drying technology combined with following chemical nitridation/phosphorization conversion strategy. Both the resultant Fe 2 N@C/CNTs and FeP@C/CNTs materials exhibit unique hierarchical polycystic microsphere structure and improved conductive network caused by the incorporation of amorphous carbon and dense CNTs coating layers. The unique structure merits endow these capabilities of facilitating electrons/ions transport and accommodating notorious volume change during charge-discharge cycling. Consequently, the Fe 2 N@C/CNTs and FeP@C/CNTs anode materials deliver enhanced rate capability (216 and 232 mA h g −1 , respectively, at a high current density of 5 A g −1 ) and durable cycling stability with reversible capacities of 489 and 571 mA h g −1 at 0.5 A g −1 after 500 cycles, respectively. In addition, this work also provides a transplantable preparation strategy for other conversion-type anode materials with poor electrical conductivity and large volume effect.

CAS / MDL: 1309-37-1 20344-49-4
研究领域: 材料科学 · 能源存储
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

Porous carbon polyhedrons with exclusive Metal-NX moieties for efficient oxygen reduction reaction

Wei-Chang Chen,Gang Yang,Yue Zhao,Gao-Qing Yuan,Jian-Shan Ye,Hai-Yang Liu,Xin-Yan Xiao

This work has manufactured a series of M-N X /C (M = Fe, Cu, Ni) ORR catalysts by the pyrolysis of metal tetraphenylporphyrin (MTPP) adsorbed onto N-doped porous carbon polyhedrons (NPCP) derived from ZIF-8. The comprehensive characterization data shows that the prepared M-N X /C catalysts have hierarchical porous structure with high specific surface area and abundant M-N X moieties. All prepared M-N X /C catalysts exhibit good ORR performance. The ORR half-wave potentials E 1/2 of Fe-N X /C, Cu-N X /C and Ni-N X /C catalyst are 0.885, 0.801 and 0.755 V respectively. The rotating ring-disk electrode (RRDE) test reveals that the ORR of Fe-N X /C is a four electron process. While a two and four electron mixing ORR process are observed for Cu-N X /C and Ni-N X /C. In an alkaline medium , E 1/2 of Fe-N X /C is observed 44 mV higher than that of commercial Pt/C. Also, Fe-N X /C catalyst has outstanding long-term durability and good methanol resistance.

研究领域: 材料科学 · 电化学 · 催化化学
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FOOD CHEMISTRY · 2023 · IF 8.8

A fluorescent dual-emitting platform for fluorescent “turn-on” ratiometric detection of ascorbic acid in beverages utilizing luminol-embedded iron-based metal–organic frameworks

Kanglin Pei,Jianyang Xu,Di Wu,Lin Qi,Lingyan Ma,Renwen Zhang,Wenjing Qi

A fluorescent dual-emitting platform for fluorescent “turn-on” ratiometric detection of ascorbic acid in beverages was developed utilizing luminol-embedded iron-based metal–organic frameworks (luminol@Fe-DOBDC MOFs). Luminol@Fe-DOBDC MOFs with fluorescent emissions at 430 nm and 540 nm under excitation wavelength of 365 nm were applied to detect ascorbic acid on the basis of ascorbic acid triggering the reduction of Fe 3+ into Fe 2+ . In the presence of ascorbic acid, fluorescent intensity at 540 nm was increased significantly while fluorescent intensity at 430 nm was changed slightly. Two emission peaks separated by 110 nm can eliminate environmental interferences by built-in self-calibration of ratiometric signal, enhancing the sensitivity and accuracy. The increasing ratiometric fluorescent intensity ( I 540 nm / I 430 nm ) has linear relationship with the concentration of ascorbic acid from 0.2 to 30 μM with limit of detection of 70 nM. It is an efficient, sensitive and accurate platform to detect ascorbic acid in commercial beverages using transition-metal-based MOFs.

研究领域: 分析化学 · 食品科学 · 材料科学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2020 · IF 3.807

Mesoporous cobalt‑iron based materials as highly efficient electrocatalysts for oxygen evolution reaction

Donggang Guo,Hongzhi Kang,Zewei Hao,Yang Yang,Pengkun Wei,Quanxi Zhang,Lu Liu

The cost-effective and high-performance electrocatalysts toward oxygen evolution reaction (OER) have been a research hotspot for the electrochemical water splitting. In view of the unique surface effect and good electrical conductivity, mesoporous nanomaterials have been a promising alternative to the precious RuO 2 for OER. Herein, two mesoporous CoFe-based nanomaterials were designed and synthesized through a facile solvothermal process as efficient OER electrocatalysts in 1.0 M KOH solution. The catalysts with a larger pore size show more excellent catalytic performance, which possess a lower overpotential of 248 mV at 10 mA·cm −2 and a Tafel slope of 58.7 mV·dec −1 , illustrating an increase of catalytic activities toward OER with the enhancement of mesoporous pore diameters. This work also contributes to the development of OER nanomaterials and the understanding of the effects of mesoporous on catalytic activity.

研究领域: 材料科学 · 电化学
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

A nitrogen-enriched strategy to accelerate the remediation of Cr(VI)-contaminated soil by iron-based materials in microwave fields

Yuxin Liu,Qintie Lin,Jieyi Pan,Yirong Deng,Junli Zheng,Mingchao Lyu,Hao Luo,Yang Luo

The existing remediation technologies for Cr(VI) contamination soil suffer from long processing times. Microwave catalysis is an efficient environmental remediation technology, and the reasonable design of microwave catalysts can enable a microwave catalytic system to rapidly complete the remediation of Cr(VI). In this study, a microwave catalyst, NRFC-3, with high microwave absorption performance and electron density was designed via a nitrogen enrichment strategy. Density functional theory (DFT) calculations verified that the electron density of the material was increased by nitrogen-enriched strategy. Under the experimental conditions, the electrons (e − ) of NRFC-3 originate from “hot spots” and the current density is not lower than 3.78 × 10 9 e·g −1 ·s −1 . In addition, the reduction of Cr(VI) in the MW/NRFC-3 system is feasible through DFT predictions, and this conclusion was experimentally verified. The MW/NRFC-3 system has a remediation efficiency of 100 % for Cr(VI)-contaminated soil within 25 min, significantly reduced the toxicity of Cr(VI) to the environment and humans, and had long-term stability. The potential application of the MW/NRFC-3 system was verified by remediation experiments on Cr(VI)-contaminated soils of different degrees. This study provides a new technology for the rapid and harmless treatment of Cr(VI)-contaminated soil.

研究领域: 环境科学 · 材料科学
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