Materials Chemistry Frontiers
·
2022
·Vol. 6
·期 21
·3213-3224
·
IF 8.683
Wenfang Miao,Feirong Huang,Xiaochen Shen,Shaopeng Li,Xingru Cao,Xuefeng Zhang,Jieyi Yu,Xinglong Dong
The development of high-efficiency, stable, and low-cost Fe–N–C electrocatalysts for the oxygen reduction reaction (ORR) has attracted considerable attention. Herein, a stable atomically dispersed Fe–Nx-based catalyst was synthesized from a hierarchical structure involving carbon nanofiber (CNF)-supported zeolitic-imidazolate-framework-8 (ZIF-8) encapsulated Fe–Phen complex ((Fe,N)-ZIF-8/CNFs). The Fe–Nx–CNFs obtained from the pyrolysis of (Fe,N)-ZIF-8/CNFs showed a good hierarchical multi-layer structure. The natural network structure of the carbon nanofibers serves as a matrix to uniformly distribute the ZIF-8 particles, and the Fe–Nx sites derived from the Fe–Phen complex were uniformly distributed in ZIF-8 particles. It exhibits excellent ORR performance with a high half-wave potential of 0.875 V (vs. RHE), which was 55 mV higher than that of the commercial Pt/C catalyst. In addition, density functional theory (DFT) calculations on the catalyst further revealed the origin of the ORR activity via a 4e− pathway from the precise local coordination of FeN4 sites.
研究领域:
材料科学
·
电化学
·
催化化学
·
纳米技术
·
能源化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Rui Ming,Jingjing Du,Lijian Xu,Yong Xu,Zhao Liang,Qiao Liu,Dongjiang Yang,Qiliang Wei,Weiyou Yang,Qing Shi
Fe doping reduces the Volmer barrier of MoNi 4 to enhance HER activity. • Mo leaching induces reconstruction into active NiMoFeOOH@MoO 4 2- for OER. • The AEMWE using this catalyst as dual electrodes reaches low voltages at 500 and 1000 mA cm -2 . • The electrolyzer operates stably for over 200 h, revealing great application potential in water electrolysis. The hydrogen evolution reaction (HER) is fundamentally limited by the sluggish water dissociation step, while the oxygen evolution reaction (OER) is constrained by the reconstruction behavior of the catalyst under operating conditions. Herein, we report a Fe-doped NiMoO x nanoflower decorated with Fe-doped MoNi 4 nanoparticles (Fe-MoNi 4 @NiMoO x ). Density functional theory (DFT) calculations reveal that the incorporation of Fe lowers the Volmer step energy barrier for MoNi 4 , thereby boosting its HER performance. For the OER, Mo leaching drives the reconstruction of MoNi 4 into catalytically active NiMoFeOOH@MoO 4 2− . Furthermore, theoretical calculations confirm that Fe/Mo doping and adsorbed MoO 4 2− facilitate rapid electron transfer within NiMoFeOOH and reduce the energy barrier of the rate-determining step for the OER. As a result, the Fe-MoNi 4 @NiMoO x catalyst delivers exceptional HER and OER activities, with overpotentials as low as 102 and 212 mV for HER, and 278 and 343 mV for OER at current densities of 100 and 500 mA cm −2 , respectively, alongside excellent stability exceeding 100 h at 500 mA cm −2 . When employed as both the cathode and anode in an anion exchange membrane water electrolyzer (AEMWE), this catalyst achieves current densities of 500 and 1000 mA cm −2 at low cell voltages of 2.22 and 2.56 V, respectively, while maintaining stable operation for over 200 h at 500 mA cm −2 . Fe-MoNi 4 @NiMoO x nanoflower electrode was developed for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). For HER, Fe incorporation lowers the Volmer step energy barrier of MoNi 4 , thereby boosting its HER performance. For OER, Mo leaching induces reconstruction into NiMoFeOOH@MoO 4 2− , where Fe/Mo doping and MoO 4 2− adsorption synergistically enhance electron transfer and reduce the rate-determining step barrier. Download: Download high-res image (241KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Haoyang Wu,Zhilong Tan,Bin Miao,Hailong Hu,Sanying Hou
In this work, Fe, N co-doped hierarchical porous graphite-like carbon with carbon-encapsulated Fe/Fe 3 C@ Fe-N-C was synthesized by a facile solid-phase synthesis strategy, and was employed as an efficient catalyst to activate peroxymonosulfate (PMS) for oxidation of tetracycline (TC). The optimal Fe-N/C 800 outlined a highly catalytic performance in activating peroxymonosulfate (PMS) with TC decomposition rate reaching 89.2 % in 20 min at ultra-low catalyst dosage. Meanwhile, the effect of operating parameters was also investigated in order to evaluate the potential of using Fe-N/C 800 in practical applications. In addition, the characterization analysis and experiments results elucidated that graphitic N, pyridinic N, C O, Fe 3 C, Fe 0 and FeN 4 were considered as the main reactive species promoting the PMS activation to generate reactive oxygen species (ROS) (including singlet oxygen ( 1 O 2 ), sulfate radical (SO 4 •- ) and hydroxyl radical (•OH)). The electron paramagnetic resonance (EPR) experiments and radicals quenching analyses further demonstrated that the non-radical species singlet oxygen ( 1 O 2 ) was the dominant reactive oxygen species. Moreover, the TC degradation pathways were presented by LC-MS. Ultimately, the toxicity of the intermediate products were also investigated by ECOSAR system.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Junyuan Zhang,Ziwei Deng,Shuli Bai,Changyu Liu,Mengchen Zhang,Chao Peng,Xiaolong Xu,Jianbo Jia,Tiangang Luan
In this work, potassium acetate (KAc) was added during the synthesis of a Zn-Fe based metal-organic framework (Fe-ZIF-8) to increase the fixed amount of Fe while simultaneously enhancing the number of pores. Electrospinning was utilized to embed KAc-modified Fe-ZIF-8 (Fe-ZIF-8-Ac) into the polyacrylonitrile nanofiber mesh, to obtain a network composite (Fe@NC-Ac) with hierarchical porous structure. Fe@NC-Ac was co-pyrolyzed with thiourea , resulting in Fe, N, S co-doped carbon electrocatalyst . The electrochemical tests indicated that the prepared catalyst displayed relatively remarkable oxygen reduction reaction (ORR) catalytic activity, with an onset potential (E onset ) of 1.08 V (vs. reversible hydrogen electrode, RHE) and a half-wave potential (E 1/2 ) of 0.94 V, both higher than those of the commercial Pt/C (E onset = 0.95 V and E 1/2 = 0.84 V), respectively. Assembled into Zn-air batteries, the optimized catalyst exhibited higher open circuit voltage (1.698 V) and peak power density (90 mW cm −2 ) than those of the commercial 20 wt% Pt/C (1.402 V and 80 mW cm −2 ), respectively. This work provided a straightforward manufacturing strategy for the design of hierarchical porous carbon-based ORR catalysts with desirable performance.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Yujing Chen,Jipeng Meng,Di Bai,Chuang Li,Xiao Chen,Changhai Liang
Pt/xFe/ZSM-23 catalysts with various Fe contents were prepared to explore the influence of extra-framework Fe (EF-Fe) on the n-hexadecane (n-C16) hydroisomerization performance. UV–vis and 57Fe Mössbauer spectroscopic results suggest that the Fe species composition was significantly different under various Fe contents, with (HO–Fe(III)–O–Fe(III)–OH) and [Fe(OH)2]+ as the main Fe species at low Fe content (<1.98 wt %), whereas the Fe2O3 clusters/particles as the dominant ones at high Fe content (>1.98 wt %). Moreover, the concentration of Brønsted acid sites and Pt dispersion could be controlled by tailoring the Fe content. Correspondingly, the hydroisomerization performance of n-C16 over Pt/xFe/ZSM-23 catalysts was dramatically changed with various Fe contents. The Pt/1.98Fe/ZSM-23 catalyst with 1.98 wt % EF-Fe content exhibited considerably excellent hydroisomerization performance, and both n-C16 conversion and selectivity to iso-hexadecane (i-C16) could reach over 80 wt % when the reaction temperature was 310 °C.
✓ 已验证
产品关联
DOI
高影响因子
CLAY MINERALS
·
2023
·
IF 1.5
Qinkai Lei,Yahui Lv,Chengshuai Liu,Wenpo Xu,Shujie Hu,Manjia Chen,Hongling Bu,Junhui Li
Mineral–organic matter (OM) associations play an important role in determining the long-term retention of OM in soils. However, the retention mechanisms of OM in cation–mineral–OM systems remain unclear. Taking into account the dominance of montmorillonite (Mnt) in the soil of the temperate zone, we investigated the stability of humic substances (HSs) in the Fe(III)–Mnt–HS system using thermal analysis. The HS degradation started at ~387°C in the Fe(III)–Mnt–HS system, which was higher than that of the Fe(III)–HS system (290°C). The formed ferrihydrite (Fhy) mainly contributed to the enhanced labile OM retention through adsorption and/or co-precipitation, whereas Mnt inhibited the initial formation and subsequent transformation of Fhy, thus improving the stability of OM. These results suggest that the HS stability in Fe(III)–clay–HS systems depends on the Fe speciation affected by clay minerals, and this finding provides insights into OM–mineral interactions in temperate-zone soils.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Qi Yang,Dan Chen,Libing Chu,Jianlong Wang
In present work, we studied a novel Fe/C nanomaterial fabricated using Fe-based metal organic frameworks (MOFs) as precursors through thermal pyrolysis to catalyze gamma irradiation-induced degradation of antibiotics, cephalosporin C (CEP-C) and sulfamethazine (SMT) in aqueous solution. The MOFs-derived Fe/C nanomaterials (DMOFs) had the regular octahedrons structure of MOFs and contained element C, Fe and O, while Fe° with a fraction of Fe 3 O 4 and Fe 2 O 3 were identified. Results showed that DMOFs addition could accelerate the generation of OH during gamma irradiation, while the intermediates of bonds cleavages of antibiotic molecules and OH addition were identified. DMOFs were more effective to improve the decomposition of antibiotic having the higher adsorption capacity like SMT. The degradation rate of CEP-C and SMT increased by 1.3 times and 1.8 times, and TOC reduction at 1.0 kGy reached 42 % and 51 %, respectively by gamma/DMOFs treatment, while only 20.2 % (CEP-C) and 4.5 % (SMT) of TOC reduction were obtained by γ-irradiation alone. The crystal structure, functional groups and magnetism of DMOFs changed slightly after gamma irradiation, which made it possible to be reused. DMOFs were promising to enhance the degradation of antibiotics during gamma irradiation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Guang Li,Yiqiao Zhang,Xue Zhang,Jian Zhang,Bo Sun
This study delves into the formation of ferryl ions (Fe(IV)) within the Fe(II)/peroxydisulfate (PDS) process, a pivotal reaction in advanced oxidation processes (AOPs) aimed at organic pollutant removal. Our findings challenge the conventional view that Fe(IV) predominantly forms through oxygen transfer from PDS to Fe(II), revealing that sulfate radicals (SO4•–) play a crucial role in Fe(IV) generation. By employing competitive kinetics, the second-order rate constant for Fe(III) oxidation by SO4•– was quantified as 4.58 × 108 M–1 s–1. Factors such as the probe compound concentration, chloride presence, and iron species influence Fe(IV) generation, all of which were systematically evaluated. Additionally, the study explores Fe(IV) formation in various Fe(II)-activated AOPs, demonstrating that precursors like peroxymonosulfate and H2O2 can also directly oxidize Fe(II) to Fe(IV). Through experimental data, kinetic modeling, and oxygen-18 labeling experiments, this research offers a comprehensive understanding of the Fe(II)/PDS system, facilitating the optimization of AOPs for pollutant degradation. Finally, introducing HSO3– was proposed to shift the Fe(II)/PDS process from Fe(IV)-dominated to SO4•–-dominated mechanisms, thereby enhancing pollutant removal efficiencies.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chemical Science
·
2024
·
IF 7.6
Wei-Xing Chen,Zi-Sheng Li,Harry W. T. Morgan,Cong-Cong Shu,Zhong-Ming Sun,John E. McGrady
We report here the synthesis and characterization of two endohedral Zintl-ion clusters, [Fe4Sn18]4− and [Fe4Pb18]4−, which contain rhombic Fe4 cores. The Fe–Fe bond lengths are all below 2.5 Å, distinctly shorter than in the corresponding Cu clusters, indicating the presence of Fe–Fe bonding. Subtle differences in the structure of the Fe4 core between the two clusters suggest that the change in tetrel element causes a change in electronic ground state, with a very short Fe–Fe bond length of 2.328 Å present across the diagonal of the rhombus in the lead case.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Zewen Fan,Wannan Wang,Jing Ren,Shaofei Zhang,Ruipeng Ren,Yong-Kang Lv
Fe[Fe(CN)6] (FeHCF) is considered a promising material for capacitive deionization–desalination of saline wastewater due to its excellent structure. However, additives are usually introduced during the synthesis of FeHCF in order to avoid [Fe(CN)6]3– vacancy defects filled by ligand water, which can result in the appearance of harmful byproducts and additional water treatment costs. In this study, an additive-free in situ vacancy repair strategy is proposed for the rapid synthesis of high-quality FeHCF in a saturated K3Fe(CN)6 solution. During the process of synthesizing FeHCF in solution, a high concentration of [Fe(CN)6]3– is found to facilitate the binding of Fe3+ to [Fe(CN)6]3– and hinder the hydrolysis and coordination reaction of Fe3+. After undergoing repair, FeHCF4 demonstrates an increased capacity and highly reversible electrochemical performance due to the robust structure. When utilized as Faraday cathodes in hybrid capacitive deionization (HCDI) systems, FeHCF4 exhibits a higher salt removal capacity (65.67 mg g–1) and lower energy consumption (0.68 kWh kg–1-NaCl) compared to unrepaired FeHCF1, while still maintaining excellent cycling performance. This environmentally friendly approach of repairing vacancies serves as a source of inspiration for the advancement of high-performance Prussian Blue analogues as capacitive sodium-removing materials.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yunpeng Zha,Xiaoxiao Sun,Zhengjun Xiong,Dandan Dong,Shili Li,Qinqin Wang,Minmin Liu
The porous carbon materials co-coordinated with Fe and N (Fe-N-C) were successfully synthesized through one-step pyrolysis with the zeolitic imidazolate framework (ZIF-8) as the precursor. Through systematic optimization of iron ion concentration during synthesis, the Fe-N-C-20 specimen exhibited optimal adsorption performance toward dibenzothiophene (DBT), demonstrating a maximum sulfur adsorption capacity of 22.14 mg S/g with a corresponding removal efficiency of 92 %. This superior performance can be primarily ascribed to the formation of Fe-S bonds anchored on Fe-N active sites, N-S interactions mediated by graphitic nitrogen species and appropriate pore size that allows access to thiophenic compounds. Furthermore, the experimental adsorption isotherms for DBT exhibited strong correlation with the Density Functional Theory (DFT) calculation. Additionally, the material's adsorption process followed pseudo-second-order kinetics and Langmuir isotherms of Fe-N-C, and the pseudo-second-order model shows the smallest RMSE (0.66), extremely low SSE (3.03) and AIC (-1.86), which further proves its excellent fitting ability. And the best balance between parameter efficiency and fitting performance. The high stability and recyclability of ZIF-derived Fe-N-C porous adsorbents contribute to sustainable industrial practices.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Hong Zhang,Xin Zhang,Bo Wang,Bo Ren,Xiaodong Yang
Food spoilage leads to plenty of food being wasted every year. Safe and multifunctional food preservation packaging is urgently required to prevent food from contamination. Chitosan/gallic acid/Fe 3+ (CSGA-Fe 3+ ) composite films were synthesized by incorporating gallic acid (GA) and Fe 3+ into a chitosan solution. The integration of GA forms covalent and hydrogen bonds with chitosan, whereas Fe 3+ addition establishes metal-ligand interactions with both chitosan and GA, resulting in a film characterized by a multi-crosslinked network structure. This multi-crosslinked system substantially enhanced the material's mechanical properties and increased resistance to oxidation and ultraviolet degradation. The data indicate that the mechanical strength of chitosan/gallic acid (CSGA) films, with an inclusion of 0.3 mmol of GA, improved by 37.5 % over pure chitosan (CS) films. Moreover, the mechanical strength of the CSGA-Fe 3+ films saw a significant increase of 124.2 %, escalating from 1.32 MPa to 17.72 MPa. Additionally, the free radical scavenging capacities of the CSGA and CSGA-Fe 3+ films rose by 279.4 % and 255.0 %, respectively, compared to the pure CS film. The UV-blocking efficacy of the CSGA-Fe 3+ films, evaluated at 365 nm, reached 84.9 %. The water contact angle of the CSGA-1.5Fe 3+ film increased by 18.08 % compared to the CS film. This study provides innovative ideas to promote the broader application of safe and multifunctional chitosan-based composite films in food preservation packaging.
研究领域:
食品科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）