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ACS Omega · 2024 · IF 3.7

Effects of Nanocomposite Derivatives of Ni–Fe, Ni–Co, Ni–Co–Fe Prussian Blue Analogues on the Thermal Decomposition Performance of Nitrocellulose

Junhong Liu,Zhitao Liu,Jing Yang,Bin Xu,Feiyun Chen,Xin Liao

The incorporation of nanomaterials generated from Prussian blue (PB) derivatives has emerged as a promising strategy to significantly improve the properties of energetic materials. In this study, we comprehensively investigated the influence of nanomaterials derived from PB on the thermal decomposition characteristics of energetic materials. To achieve this goal, we prepared nanomaterials using coprecipitation and heat treatment methods with PB derivatives as catalysts. Advanced techniques such as X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Brunauer–Emmett–Teller (BET) analysis for specific surface area and pore size, and X-ray photoelectron spectroscopy were employed to thoroughly characterize these nanomaterials. Differential scanning calorimetry was used to assess the thermal behavior of nitrocellulose (NC), and the relevant kinetic parameters were determined through thermal decomposition kinetics calculations and analysis. This work revealed the influence of catalysts on the NC decomposition process and provided comprehensive insights into the effect of integrating nanomaterials derived from PB derivatives on the thermal decomposition performance of NC. The results of this work demonstrated the possibility of using nanomaterials generated from PB derivatives as effective catalysts to enhance the thermal decomposition characteristics of NC, offering interesting opportunities for their application in the field of high-energy materials.

CAS / MDL: 68-04-2
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ELECTROCHIMICA ACTA · 2024 · IF 5.5

Carbon nanotubes cross-linked Fe/Fe3C nanoparticles and Fe single atoms as high-efficiency bifunctional oxygen electrocatalyst for rechargeable zinc-air batteries

Zhiwen Xu,Lanlu Lu,Weiwei Chen,Fei Yang,Guimei Liu,Yan Sun,Xiaoyi Qiu,M. Danny Gu,Ping Gao,Dong Su,Minhua Shao

Although zinc-air batteries (ZABs) have made great progress in recent years, there still a great challenge to develop low-cost bifunctional electrocatalysts with high catalytic activity and stability. Herein, we report a bifunctional oxygen electrocatalyst consisting of ZIF-derived carbon-anchored Fe/Fe 3 C nanoparticles and Fe single atoms, which are crosslinked by carbon nanotubes (denoted as CNT@Fe/Fe 3 C||FeNC). Benefiting from the synergetic effect of Fe/Fe 3 C nanoparticles, Fe-N 4 active sites, and the 3D interpenetrating network structure, CNT@Fe/Fe 3 C||FeNC shows excellent bifunctional catalytic activities with a low ΔE of 0.671 V. Furthermore, the assembled rechargeable ZAB demonstrates a high peak power density of 187 mW cm –2 and shows excellent cycling stability up to 600 h This work provides new ideas for constructing non-precious metal bifunctional catalysts for practical applications in ZABs.

CAS / MDL: 693-98-1 10196-18-6
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JOURNAL OF CATALYSIS · 2024 · IF 6.5

Enhanced hydrogen production of Fe-based spinel by relay catalysis of Fe0 and Fe-Ov-Cr species in chemical looping H2O splitting

Yujia Han,Teng Zong,Yuehan Wang,Ming Tian,Chaojie Wang,Nanxin Wang,Xiaodong Wang

Chemical looping H 2 O splitting is considered as a promising approach to produce hydrogen thanks to its lower energy consumption and carbon footprint compared with traditional steam reforming. Fe-based oxides have been paid much attention but suffer from inferior H 2 production rate and stability due to insufficient activation for H 2 O. Herein, it was found that the introduction of Cr into MgFe spinel oxides (MgFe x Cr 2-x O 4 , MFCO) could greatly increase the performance of H 2 O splitting driven by CH 4 reduction with the highest peak H 2 production rate of about 4.65 mmol min −1 g −1 , H 2 productivity of about 2.88 mmol g −1 and good stability during multiple redox cycles for MFCO-46 (the atomic ratio of Fe and Cr of 2:3), which exceeded most of the state-of-the-art Fe-based oxides. This originated from the Cr doping promoting Fe 0 nanoparticles exsolution by activating CH 4 and Fe-O v -Cr species formation which relay catalyzed H 2 O splitting and was favorable for the fast recovery of lattice oxygen converted.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Enhancing the Fenton catalytic activity of Fe-MOFs by incorporation of carbon nanotubes: The crucial role of C-O-Fe coordination structure

Jingjing Tang,Hongchao Li,Xuan Zhang,Jieshu Qian,Bingcai Pan

Fe-based metal–organic frameworks (MOFs) have garnered significant attention as catalysts for heterogeneous Fenton reactions, while the limited efficiency of the Fe(III)/Fe(II) redox cycle hinders their widespread use in wastewater treatment. Herein, we successfully incorporated carbon nanotubes (CNTs) into MIL-101(Fe) to modulate the coordination environment of Fe for achieving better catalytic activity. The MIL-101(Fe)/CNTs/H 2 O 2 system shows outstanding performance in degrading various pollutants, with the catalytic activity of the MIL-101(Fe)/CNTs composites (98.8%) significantly surpassing that of MIL-101(Fe) alone (26.4%) or CNTs alone (3.5%). Multiple experimental findings suggest that this synergistic effect is primarily attributed to the C-O-Fe bridge bonds resulting from the interaction of surface carboxyl groups on CNTs with Fe in MIL-101(Fe). This unique coordination structure accelerates the redox cycle of Fe(III)/Fe(II), thereby promoting the generation of hydroxyl radicals (HO • ). Furthermore, the MIL-101(Fe)/CNTs composites demonstrate excellent reusability and stability, maintaining effectiveness over a wide pH range from 3.0 to 6.5. This study provides new insights into regulating the microstructure of Fe-based MOFs to enhance their Fenton catalytic activity.

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BIOMASS & BIOENERGY · 2017 · IF 3.219

Catalytic conversion of glucose to 5-hydroxymethyfural over Fe/β zeolites with extra-framework isolated Fe species in a biphasic reaction system

Haian Xia,Hong Hu,Siquan Xu,Kehao Xiao,Songlin Zuo

A series of Fe/β zeolite catalysts with various Fe/Al ratios were prepared by liquid ion-exchanged method and were characterized by N 2 adsorption, XRD , UV–Vis DRS, EPR , NH 3 -TPD, and FTIR of pyridine adsorption techniques. The catalysts were used to catalyze the transformation of glucose into 5-hydorxymethyfural (HMF) in a biphasic reaction system under mild reaction conditions. The Fe/β catalysts with Lewis acidic Fe sites is able to effectively improve the HMF yield compared to H-β zeolite under identical reaction conditions, which is ascribed to the enhanced isomerization activity of glucose-to-fructose by Lewis acidic Fe species. Moreover, the Fe/Al ratio had a remarkable impact on the conversion of glucose and the yield of HMF, indicating that the synergetic effect of Lewis and Brønsted acid sites is critical to achieving high HMF yield. Under optimal reaction conditions, Fe/β-0.06 catalyst afforded 61% HMF yield at glucose conversion of 95% after the reaction of 90 min at 120 °C, which is one of the most effective catalysts for the conversion of glucose into HMF in a biphasic medium up to now. Furthermore, extra-framework isolated Fe species bound to the framework Al sites, are most likely the active sites for the isomerization of glucose-to-fructose in the conversion of glucose. The catalysts were very stable and could be reused at least five runs without significant loss in the catalytic activity .

CAS / MDL: 78-92-2 71-36-3 123-86-4
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CHEMICAL GEOLOGY · 2024 · IF 3.6

Reduction of c-type cytochromes by Fe(II)-ligand under oxic conditions: Roles of Fe(II)-heme complexation and reactive oxygen species

Kuan Cheng,Yunlu Yin,Ying Wang,Guoyong Huang,Dandan Pan,Milan Wang,Xuxin Song,Tongxu Liu,Xiaomin Li

Microbial Fe(II) oxidation is mainly mediated by the outer-membrane proteins that contain c -type cytochromes ( c- Cyts), and the widespread Fe(II)-oxidizing bacteria are usually subjected to fluctuations between oxic and anoxic conditions. However, it remains unclear how oxygen affects the redox dynamics of c- Cyts by Fe(II), particularly in the presence of organic ligands that are widely distributed in the environment. Here, the reduction of a model heme-containing c- Cyts by Fe(II) was investigated in the absence and presence of organic ligands (i.e., citrate and acetate) at pH 5.5 under anoxic and oxic conditions . The kinetic results showed that c- Cyts reduction was enhanced by citrate and acetate under anoxic conditions, and the enhancement by citrate was more pronounced than that by acetate. The speciation calculation and cyclic voltammetry results suggested that the proportions of Fe(II)-Citrate complexes were much higher than those of Fe(II)-Acetate complex, but the addition of acetate and citrate caused minor changes in redox potential of Fe(II)/Fe(III) species. Further analysis using quantum chemical computation demonstrated that the formation of Fe(II)-Heme complexes via lateral binding to the carboxyl group of c- Cyts was more stable than those via replacing the S-linked axial ligand of heme, with the recombination energy with Heme ranking as Fe(II)-Citrate < Fe(II)-Acetate < Fe(II). Therefore, the stronger complexation of Fe(II)-Citrate and its lower recombination energy with c- Cyts drive the enhanced c- Cyts reduction under anoxic conditions. By contrast, the c- Cyts reduction by Fe(II) and Fe(II)-ligand was inhibited under oxic conditions. The electron spin resonance characterization indicated that both O 2 − • and OH• radicals were produced in the system of c- Cyts with Fe(II) or Fe(II)-ligand under oxic conditions and the signals were higher with Fe(II)-ligand than those with Fe(II). These reactive oxygen species were proposed to enable a re-oxidation of the c- Cyts that was reduced by Fe(II) or Fe(II)-ligand, causing an inhibitory effect on the observed c- Cyts reduction and forming more reactive oxygen species . Our findings shed light on the important roles of Fe(II)-ligand-heme complexation and reactive oxygen species in the interaction between Fe(II) and c- Cyts, which deepen the understanding of microbial/enzymatic Fe(II) oxidation under oxic conditions at the molecular level.

CAS / MDL: 68-04-2 7775-14-6
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Phosphor-doping modulates the d-band center of Fe atoms in Fe-N4 catalytic sites to boost the activity of oxygen reduction

Yuan Qin,Zihao Ou,Chaozhong Guo,Yao Liu,Rong Jin,Chuanlan Xu,Haifeng Chen,Yujun Si,Honglin Li

Regulating the electronic structure by phosphor-doping is a preferred strategy to boost the performance of carbon-based catalysts for oxygen reduction reaction (ORR). Here, a porous Fe, P, N-codoped carbon catalyst (PCF-FeTz-900) is designed by a phytic acid-assisted thermal etching strategy, in which P atoms are first doped into the carbon matrix to form a stable P C bond, and then FeN 4 sites are produced from Fe-2,4,6-Tris(2-pyridyl)-s-triazine complex (Fe-TPTz). Theoretical calculations suggest that the electrons are transferred from the doped P atom to the neighboring FeN 4 sites, which facilitates the ORR at the Fe sites by reducing the energy barrier and the adsorption energy of intermediates. Additionally, the P-doped FeN 4 (FeN 4 P) structure manifests a lower free energy difference than that of FeN 4 and the d -band center of Fe is also lowered, which further ensures its higher ORR catalytic ability. As a result, the PCF-FeTz-900 catalyst exhibits superior ORR activity and stability in alkaline electrolyte, and the assembled primary zinc-air battery shows greater performances compared to the commercial Pt/C catalyst. This work can provide an effective pathway for modulating the performance of doped-carbon materials in energy conversion devices.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Understanding the high performance of an iron-antimony binary metal oxide catalyst in selective catalytic reduction of nitric oxide with ammonia and its tolerance of water/sulfur dioxide

Xuanxuan Jia,Hao Liu,Yu Zhang,Wei Chen,Qing Tong,Guangxia Piao,Chuanzhi Sun,Lin Dong

In recent years, Fe-based catalysts for the selective catalytic reduction of NO with NH 3 (NH 3 -SCR) have been attracting more attention. In this work, a novel Fe-Sb binary metal oxide catalyst was synthesized using the ethylene glycol assisted co-precipitation method and was characterized using a series of techniques. It was found that the catalyst with a molar ratio of 7:3 (Fe:Sb) displayed the best NH 3 -SCR activity with 100% conversion of NO x (nitrogen oxides) over a wide temperature window and with good resistance to H 2 O + SO 2 at 250 °C. The X-ray photoelectron spectroscopy (XPS) and in situ diffused reflectance infrared Fourier transform spectroscopy ( in situ DRIFTS) of NO x adsorption results suggested that strong electron interactions between Fe and Sb in Fe-O-Sb species existed and electrons of Sb could be transferred to Fe through the 2Fe 3+ + Sb 3+ ↔ 2Fe 2+ + Sb 5+ redox cycle. The introduction of Sb significantly improved the adsorption behaviour of NO x species on the Fe 0.7 Sb 0.3 O x surface, which benefitted the adsorption/transformation of NO x , thereby facilitating the NH 3 -SCR reaction. In addition, the Fe 0.7 Sb 0.3 O x catalyst demonstrated a good tolerance of H 2 O and SO 2 , since the decomposition of NH 4 HSO 4 on the catalyst surface was promoted by the introduction of Sb.

研究领域: 催化 · 环境科学 · 材料科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2018 · IF 5.667

An electrochemical biosensor for sensitive detection of microRNAs based on target-recycled non-enzymatic amplification

Fang Hu,Wancun Zhang,Jiaqi Zhang,Qi Zhang,Tao Sheng,Yueqing Gu

In this study, a simple, economic, and label-free electrochemical biosensor was developed for highly sensitive and selective miR-21 detection based on Fe(CN) 6 3− /Fe(CN) 6 4− electrochemical signal, which relies on DNA structures conjugating with carboxyl multi-wall carbon nanotubes (MWCNTs-COOH)-modified glassy carbon electrode (GCE). High sensitivity and specificity of the biosensor were achieved by taking advantage of the target-recycled non-enzymatic amplification strategy (TRNEAS), which relies on sequence-specific hairpin strand displacement and does not require the addition of environment-susceptible enzymes. Besides, the SP-DNA strictly binds to the cMWCNTs/GCE via amide bonds, which ensure good electrochemical results and excellent stability for target miRNA detection. The developed miR-21 electrochemical biosensor exhibited a broad linear dynamic range of 0.1 fmol to 5 pmol and a detection limit of 56.7 amol for miR-21 detection in vitro . The relative miR-21 expression levels were particularly detected by our developed miR-21 biosensor and were highly consistent with the stem-loop RT-PCR results. In summary, our developed electrochemical biosensor exhibits great potential for further application in biomedical research and early clinical diagnosis.

研究领域: 生物传感器 · 电化学 · 纳米技术 · 分子生物学 · 临床诊断
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POLYMER DEGRADATION AND STABILITY · 2021 · IF 5.03

Synthesis of a bio-based flame retardant via a facile strategy and its synergistic effect with ammonium polyphosphate on the flame retardancy of polylactic acid

Yuanyuan Zhan,Xujuan Wu,Shasha Wang,Bihe Yuan,Quan Fang,Sheng Shang,Chengran Cao,Gongqing Chen

The high flammability and severe melt-dripping during the combustion are the most marked fire hazards for polyesters, such as polylactic acid (PLA). In this work, a bio-based flame retardant (ATMP-NA-Fe) was successfully synthesized by a simple aqueous ionic reaction by using amino trimethylene phosphonic acid (ATMP), nicotinamide (NA) and FeCl 3 •6H 2 O as raw materials. The ATMP-NA-Fe and ammonium polyphosphate (APP) have good synergistic effects on improving the flame-retardant performance and retarding the combustion melt-dripping of PLA. With a 10 wt% total loading of ATMP-NA-Fe and APP (1:1), the limiting oxygen index value of corresponding PLA composite (PLA3) increases from 20.1% to 32.8%, and it passes UL-94 V-0 rating without melt dripping. The cone calorimetry results show that compared with pure PLA, the peak heat release rate, total heat release and average mass loss rate of PLA3 are reduced by 66.4%, 14.9% and 76.7%, respectively. Via the analysis on the condensed and gas phase products, the flame-retardant mechanism of PLA/APP/ATMP-NA-Fe composites is proposed. This work provides a new approach for improving flame-retardant performance of PLA and promoting the utilization of renewable resource.

研究领域: 材料科学 · 化学工程 · 可再生资源利用
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APPLIED CATALYSIS A-GENERAL · 2025 · IF 4.8

FeOx clusters confined in ZSM-5 as a high-performance catalyst for Fischer-Tropsch synthesis of lower hydrocarbons

Qichao Lu,Jie Li,Chen Liang,Lei Liu,Jinxiang Dong

Under the dual pressures of oil depletion and low-carbon transition, Fischer-Tropsch synthesis (FTS) technology offers a viable option for producing high value-added lower (C 2 -C 4 ) hydrocarbons from non-oil sources. However, conventional Fe-based catalysts often suffer from deactivation due to carbon deposition and sintering. Here, we report a unique Fe-ZSM-5 catalyst synthesized by doping Fe into ZSM-5, which demonstrates excellent FTS catalytic performance. During high-temperature template removal, Fe species migrated from the zeolite framework to form highly dispersed FeO x clusters (∼2 nm). Upon treatment by syngas, these FeO x clusters aggregate to form uniformly small-sized Fe 5 C 2 @C core-shell particles distributed on ZSM-5 support. The confinement effect of the inter-crystalline structure effectively prevents the sintering of Fe 5 C 2 . The smaller Fe 5 C 2 particles exhibit controlled CO dissociation, reducing the concentration of activated carbon species (C*), and the carbon shells (∼6.5 nm) limit the departure of C*, effectively suppressing carbon deposition. This unique structure enables stable catalytic activity for over 100 hours with maintained product selectivity. The Fe-ZSM-5 catalyst achieved a C 2 -C 4 hydrocarbons selectivity of 54.52 %, nearing the 56 % theoretical limit of the Anderson-Schulz-Flory (ASF) distribution. Additionally, the hydrophobic carbon shell prevents excessive oxidation of Fe 5 C 2 , reducing CO 2 selectivity by ∼56 % compared to conventional Fe/ZSM-5 catalysts, significantly enhancing atomic utilization efficiency and aligning with the principles of green development.

研究领域: 化学工程 · 材料科学 · 能源催化
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JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY · 2023 ·Vol. 28 ·期 4 ·379-391 · IF 3

Biomimetic synthesis of hydroxytyrosol from conversion of tyrosol by mimicking tyrosine hydroxylase

Chen Chan,Tang Weikang,Chen Qinfei,Han Mengqi,Shang Qi,Liu Wenbin

Hydroxytyrosol, one of the most powerful natural antioxidants, exhibits certificated benefits for human health. In this study, a biomimetic approach to synthesize hydroxytyrosol from the hydroxylation of tyrosol was established. EDTA-Fe 2+ coordination complex served as an active center to simulate tyrosine hydroxylase. H 2 O 2 and ascorbic acid were used as oxygen donor and hydrogen donor, respectively. Hydroxy radical and singlet oxygen contributed to active species. The biomimetic system displayed analogous component, structure, and activity with TyrH. Hydroxytyrosol titer of 21.59 mM, and productivity of 9985.92 mg·L −1 ·h −1 was achieved with 100 mM tyrosol as substrate. The proposed approach provided efficient and convenient route to quickly produce high amount of hydroxytyrosol. Graphical abstract

研究领域: 生物化学 · 合成生物学 · 抗氧化研究
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