Environmental Science-Nano
·
2020
·Vol. 7
·期 12
·3814-3823
·
IF 7.683
Hanfeng Zhou,Zhibo Deng,Tianbao Liu,Tao Liu,Lijuan Zhang,Xintai Su,Zhang Lin
The science linking thermochemical conversion of large-scale industry oily sludge with applied materials has been improved in the last ten years. However, with the traditional converting methods it is hard to precisely control the composition and structure of oily sludge-based products during pyrolysis due to the complexity of the composition of the oily sludge. Here, a chlorinating calcination method using sodium chloride (NaCl) as a chlorinating salt and template was first developed to prepare porous Fe–N–C materials (FCN-500) through pyrolysis of oily sludge containing iron-bearing minerals and pyridine. The formation mechanism of FCN-500 was proposed, where iron ions (Fe3+) from the inorganic component (anorthite) in the sludge were rapidly dissociated with the assistance of NaCl, followed by coordination with the organic component (pyridine nitrogen) in the oily sludge to form the pyridine nitrogen–iron ((C5H6N)n–Fe) complex, and then carbonization. As-obtained FCN-500 exhibited higher specific capacitance (286.3 F g−1 at a current density of 0.5 A g−1), enhanced energy density (33.5 W h kg−1 at a power density of 606.1 W kg−1) and more excellent stability and durability (more than 80.1% capacitance retention after 10 000 cycles) compared with two other electrodes. The reasonably better performance of the obtained FCN-500 in supercapacitors (SCs) is attributed to its large surface area, hierarchically porous channels, high conductivity, and unique Fe–N–C structure. Therefore, this work not only provides a feasible way to solve the bottleneck problem in sludge pyrolysis, but also provides a method to design large scale porous Fe–N–C materials for practical applications.
研究领域:
环境科学
·
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Ying Liu,Yi Liu,Yingying Xu,Qingshen He,Rongyang Yin,Pengfei Sun,Xiaoping Dong
Nitrophenols (NPs) are widely used in industries and highly toxic to ecological environment and human health. Because aminophenols (APs) are important chemicals, catalytic reduction of NPs via efficient and environment-friendly strategies is of great importance. Herein, we developed a green photocatalysis route to efficiently convert NPs to APs using a Fe (II) modified graphitic carbon nitride (g-C 3 N 4 ) photocatalyst, where phenanthroline units were employed to bridge Fe (II) and carbon nitride framework. The optimized sample P-CN-8-Fe presented significantly improved absorption of visible light, separation of photogenerated charges and carrier transportation in comparison with the pristine g-C 3 N 4 and the modified samples of CN-Fe and P-CN-8. Accordingly, the P-CN-8-Fe showed a high conversion (97%) of p -nitrophenol ( p -NP) to p -aminophenol ( p -AP) under 2 h visible light irradiation, and meanwhile possessed high photocatalytic durability. Its high activity was also demonstrated through photocatalytic reduction of other NPs and nitrobenzene compounds. Finally, a possible mechanism was proposed for the photocatalytic reduction of p -NP by P-CN-8-Fe. This work provides an effective approach to prepare Fe (II) modified g-C 3 N 4 through the bridging effect of phenanthroline group, which is a potential visible light driven photocatalyst for reduction of nitrobenzene derivatives.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Shuting Huang,Yanxian Geng,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jianmei Lu
Microbial fuel cells (MFCs) have become new energy approach for sustainable development. The exploitation of economic and efficient electrocatalysts for the oxygen reduction reaction (ORR) is essential for obtaining remarkable MFCs performance. Herein, metal–organic framework (MOF)-derived Fe/Fe 3 C embedded in nitrogen-doped carbon hybrids, prepared through a simple solvothermal and pyrolysis approach, are highly efficient ORR catalysts. The unique mixed dimension (1D/2D) and mesoporous structure provide abundant active sites and build transfer channels for improvement. Additionally, the presence of nitrogen doping played an important role to accelerate electron diffusion and transport. A maximum power density of 1974.75 ± 26.16 mW m −2 is earned by Fe/Fe 3 C/NC-800, and is 1.45 times of 20% Pt/C (1366.45 ± 28.65 mW m −2 ). Therefore, the Fe/Fe 3 C/NC catalyst is a prospective ORR catalyst in MFCs and in future renewable energy storage and conversion technologies.
研究领域:
材料科学
·
能源技术
·
环境科学
✓ 已验证
DOI
高影响因子
Industrial Chemistry & Materials
·
2024
·
IF 0
Jiayao Cui,Junyong Min,Hao Wang,Jianglan Shui,Lishan Peng,Zhenye Kang,Jieyuan Liu,Qingjun Chen,Shuo Bai,Yanrong Liu
Developing single-atom Fe–N4/C catalysts is crucial for the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). While Fe–N4/C catalysts are inherently active in accelerating the slow ORR process, their performance is still inferior to that of Pt/C. Herein, a trace Co-doped Fe single-atom catalyst (Fe(tCo)–N–C) containing more active Fe2N8 sites has been synthesized. Interestingly, compared with typical FeN4 sites in an Fe–N–C electrocatalyst, the Fe2N8 sites generate a larger Fe–N bond length due to Co-doping. The elongated Fe–N bond in Fe2N8 lowers the d-band center and charge density of iron sites, enhancing the ORR process by facilitating the formation of *OOH and generation and desorption of *OH. Fe(tCo)–N–C manifested excellent acidic and alkaline ORR activity, with a half-wave potential (E1/2) of 0.80 V in HClO4 solution and 0.89 V in KOH medium. More importantly, high peak power densities (Pmax) were realized by applying Fe(tCo)–N–C in PEMFCs, with the Pmax reaching 890 mW cm−2 in H2–O2 and 380 mW cm−2 in H2–air. Additionally, trace Co dopants in the catalyst improved carbon graphitization and provided high ORR catalytic stability. This research introduces an innovative approach to engineering highly active Fe2N8 sites, providing valuable insights for the sustainable progress of PEMFC technology.
研究领域:
电化学
·
催化
·
能源材料
·
燃料电池
·
纳米技术
✓ 已验证
DOI
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 18
·8566-8577
·
IF 3.3
Tingting Tang,Bo Jin,Ping Zhao
Aromatic nitro compounds are the main components of explosives. They are not only explosive and dangerous but also have high toxicity and high stability in the human body, soil, and water resources, destroying the ecological environment. Herein, a simple hydrothermal method is used to successfully prepare layered MIL-100 (Fe). A series of aromatic nitro compounds including p-nitrophenol (PNP), nitrobenzene (NB), dinitrotoluene (2,4-DNT), dinitrophenol (2,4-DNP), and 2,4,6-trinitrophenol (2,4,6-TNP) were degraded by the photo-Fenton method. The MIL-100 (Fe) photo-Fenton agent can almost completely degrade PNP within 2 min. Similarly, it has a good degradation effect on other pollutants. Finally, the mechanism of the photo-Fenton reaction was discussed by product analysis and free radical capture experiments after the photochemical reaction. This study demonstrates the potential application value of MIL-100 (Fe) as a photo-Fenton reagent to degrade nitroaromatic explosives.
研究领域:
环境化学
·
材料科学
·
催化化学
·
环境污染与控制
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应用化学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2022
·Vol. 49
·期 7
·10265-10272
·
IF 5.532
Wenchao Xi,Boxue Song,Zhengyu Sun,Tianbiao Yu,Jun Wang,Qi Sun
To improve the wear resistance of Fe-based cladding, NbC particles with different morphology are generated in situ by adding Nb, Cr 3 C 2 and C with different content. The composition of samples and the morphology of NbC particles generated in situ are revealed by XRD , SEM and EDS. The wear resistance is studied by a reciprocating friction and wear testing machine. The wear mode and the wear mechanism of each sample are investigated. The results show that although NbC particles are generated in situ in samples with different Nb, Cr 3 C 2 and C content, the morphology of NbC particles is varied. The wear resistance of samples containing cross-shaped NbC particles is more outstanding than that of samples containing only rectangular NbC particles. In addition, changing Nb, Cr 3 C 2 and C content does not result in a change in wear mode, but leads to the formation of continuous lattice structure of Cr 0.19 Fe 0.7 Ni 0.11 and Cr 23 C 6 compounds at grain boundaries and a change in the wear resistance. When the additions of Nb, Cr 3 C 2 and C are 11.2 wt%, 8.6 wt% and 0.2 wt% respectively, the coefficient of friction of the sample is the lowest, and the wear resistance is the most outstanding.
研究领域:
材料科学
·
金属学与热处理
·
表面工程
·
摩擦学
·
复合材料
✓ 已验证
DOI
高影响因子
ACS Applied Engineering Materials
·
2023
·
IF 0
Demin Jiang,Kai Cheng,Liang Li,Kun Xie,Haijun Tao,Yuqiao Wang
Anodes are considered an important component of microbial fuel cells (MFCs) to recover electric energy from organic wastewater. Herein, Fe/N codoped paper carbon fiber foam was developed as an anode for MFCs to enhance electricity generation and wastewater treatment. The interconnected microporous network was beneficial for bacteria colonization and biofilm formation. The N doping enhanced the hydrophilicity to facilitate bacterial proximity. The Fe doping modulation adhered to the microorganisms due to the positive charge of iron ions. The codoped anode promoted the organic matter degradation efficiency and intrinsic electricity generation property based on the optimized thick biofilm. The high electricity output of MFCs was increased by the decreased internal resistance. The assembled MFCs possessed a short start-up time of 29.1 h, high maximum power density of 2270 ± 118 mW·m–2, desirable chemical oxygen demand removal efficiency of 71.7 ± 1.9%, and high decolorization efficiency of 90.3 ± 2.5% at 44 h. Fe/N codoped strategy is proposed to construct anodes for improving the electricity generation property and wastewater treatment efficiency of MFCs.
研究领域:
环境科学
·
生物电化学
·
材料科学
·
微生物学
✓ 已验证
DOI
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yi Yang,Minyi Liu,Xintong You,Ying Li,Haowen Lin,J. Paul Chen
Treatment of organic wastewater is of great importance and can be carried out by catalysis technologies such as catalytic wet peroxide oxidation (CWPO). A novel bimetallic Fe-Cu-CNT catalyst was first developed by a facile hydrothermal method; Fe species (Fe (Ⅱ) and Fe (Ⅲ)) and Cu species (Cu (Ⅰ) and Cu (Ⅱ)) were used to fabricate the catalyst with the CNTs, which was stable during testing. Methylene blue (MB) was chosen as model compound for the study; the optimization for treatment by the Box-Behnken design indicated that a combination of low pH, high MB concentration and intermediate temperature led to better treatment performance. The CWPO reaction obeyed the 2 nd -order kinetic equation and the catalyst activity increased with an increase in the Cu content. The reaction induction period was shortened with decreasing Fe:Cu ratio. The cycling reaction between Fe 3+ /Fe 2+ and Cu 2+ /Cu + pairs generated a large number of oxidative radicals and improved the pollutant degradation efficiency. Finally, the reaction rate equation of CWPO over Fe-Cu-CNT was derived, and it was experimentally illustrated that hydroxyl radicals played a crucial role in the treatment. This study demonstrates that the optimized Fe-Cu-CNT has great potentials for treatment of organic wastewater with higher efficiency and lower cost.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Jiajie Xu,Shengye Wang,Changyu Yan,Hafiz Mohammad Adeel Sharif,Bo Yang
Advanced oxidation processes based on sulfate radicals are considered as a promising approach for environmental remediation. In this study, TiO 2 @MIL-101(Fe) is successfully fabricated by a facile impregnation method and is used for sodium persulfate (SPS) activation. TiO 2 @MIL-101@SPS combines the advantages of photocatalysis and SPS activation, which shows high removal efficiency for nitrobenzene and methyl orange. In addition, the effect of multiple factors, including light source, SPS amount and catalyst amount, on nitrobenzene degradation have been investigated. Results show that the nitrobenzene degradation efficiency is up to 66.53 % while that of TOC removal is 32.21 % under 4-h visible light irradiation with 30 mg catalyst and 1.6 mM SPS. Moreover, LC-MS have been carried out to study the route of nitrobenzene degradation. Besides, ESR analysis reveals that both ● SO 4 − and ● OH radicals are generated sustainably under visible light irradiation, and more ● OH radicals can be detected owing to the synergic effect of photocatalysis and SPS activation. Interfacial charge transfer effect provides photoinduced electrons for the Fe 3+ /Fe 2+ cycle in MIL-101(Fe), which boosts the SPS activation process, resulting in high photocatalytic activity.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chen Qiao,Zahid Usman,Tai Cao,Souleymen Rafai,Zhitao Wang,Youqi Zhu,Chuanbao Cao,Jiatao Zhang
High-valence Ni and Fe metal sites have demonstrated a crucial role in enhancing the catalytic performances of NiFe-LDH electrocatalysts in oxygen evolution reaction (OER). Although considerable OER catalytic performances achieved under high overpotential, the catalytic talent of NiFe-LDH electrocatalysts at low overpotential is rarely realized due to the absence of high-valence Ni and Fe sites. We herein report a surface engineering route to fabricate sulfated NiFe-LDH nanosheets via ion exchange strategy in sulfate-rich media. XPS results reveal a modified surface electronic structure with high-valence Ni and Fe after ion exchange reaction. Computational PDOS results suggest that computed d-band centers (ε d ) of Fe and Ni for sulfated NiFe-LDH show a significant downward shift resulting an increased valence of metal cation with orbital volume shrinkage. The high-valence Fe can facilitate a optimized multi-electron process of Ni center from [Ni II -OH] − /[Ni III -OH] − to Ni IV -OOH rather than Ni II /Ni III to Ni IV at low overpotential. The high-valence Ni can serve as the highly active center for O-O coupling during OER process. Combined with the synergetic action of high-valence Fe and Ni, the sulfated NiFe-LDH nanosheets exhibit much larger reaction kinetics and outstanding electrocatalytic activity on glassy carbon electrode (η 10 = 219 mV, η 50 = 288 mV) with a remarkable long-term stability.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
ANALYST
·
2020
·Vol. 145
·期 19
·6349-6356
·
IF 3.978
Ye Hu,Chaochao Yue,Jing Wang,Yuhua Zhang,Wenhui Fang,Jiaqi Dang,Ying Wu,Hong Zhao,Zengxi Li
Fe–Ni-MOFs with different amounts of Fe are synthesized through a two-step template etching method. Kinetic analysis indicates that Fe–Ni-MOF exhibits prominent intrinsic peroxidase-like activity, which could catalytically oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to produce oxidized TMB (oxTMB) with a blue color. As a peroxidase-mimicking MOF, Fe–Ni-MOF with its efficient stable catalysis properties is demonstrated to allow a sensitive colorimetric assay for Sn2+ ions. The mechanism is explored, whereby Sn2+ ions could reduce the peroxidase-like activity of Fe–Ni-MOF based on a redox interaction, making the oxTMB color lighter and decreasing the absorbance intensity at 652 nm. The linear determination of the Sn2+ ion concentration using a UV-vis spectrometer ranges from 0.01 mM to 1.0 mM and from 1.0 mM to 4.0 mM. The presented Fe–Ni-MOF-based assay of Sn2+ ions was successfully applied to real water samples.
研究领域:
材料科学
·
分析化学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2021
·Vol. 23
·期 8
·4690-4699
·
IF 3.676
Zhengyan Zhao,Wei Liu,Yantao Shi,Heming Zhang,Xuedan Song,Wenzhe Shang,Ce Hao
We report a combination of experimental and computational mechanistic studies for the photoreduction of CO2 to CO with water, catalyzed by single-atom Fe supported on graphitic carbon nitride (g-C3N4). Density functional theory (DFT) and time-dependent DFT (TDDFT) methods were utilized to explore the behavior of single-atom Fe in g-C3N4, which is of vital importance to the understanding of the CO2 reduction reaction (CO2RR) mechanism. The calculation results reveal that the rate-limiting step of the hydrogen-bonded complex in the absence of Fe atoms is the cleavage of C–O bonds in COOH radicals during the whole CO2RR, which includes the photophysical and photochemical processes. The presence of Fe atoms not only activated CO2 in the ground state and increased the rate constant of the limiting step in the photophysical process, but also functioned as the catalytic active center, lowering the reaction barrier of the C–O bond cleavage in COOH˙ in the photochemical process and resulting in improved photocatalytic activity. In addition, DFT calculations further demonstrated that the electron and proton transfer involved in the photophysical and photochemical processes is closely related to and induced by the hydrogen bonds in the excited state.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）