APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Yingying Guo,Chenhui Wang,Yuhang Xiao,Xiaohong Tan,Weidong He,Jianpo Chen,Yan Li,Hao Cui,Chengxin Wang
Fe single-atom catalysts (SACs) have emerged as a promising alternative to platinum for catalyzing oxygen reduction reactions (ORR). Nevertheless, their practical applicability is hindered by insufficient stability caused by structural corrosion during ORR. Here, we developed an effective strategy to optimize and stabilize the Fe SAs (single-atoms) sites by implanting chromium (Cr) atomic clusters (ACs) to address the formidable deactivation issue of the best-performing yet unstable Fe-N-C catalysts. Cr AC -Fe 1 /N-S-C demonstrates an amazing stability with a negligible decline in activity after 100,000 CV cycles, and can maintain 81% of initial current after a continuous 50-hour operation period. Theoretical calculations and experimental evidence substantiate that the integration of Cr ACs not only weakens the binding of OH* to the Fe site, thereby facilitating the ORR process, but also eliminates in situ-generated reactive oxygen species (ROS) and retards Fe ion leaching from active sites, thus stabilizing of the Fe SA sites.
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高影响因子
FUEL
·
2023
·
IF 7.4
Zhihan Wu,Kuan Ding,Guiying Lin,Hongqi Sun,Shu Zhang
Ketonization of oxygenated compounds in pyrolytic products of biomass is an effective means for deoxygenation and upgrading of bio-oils. However, the ketonization potential of biomass-derived sugars and the mechanism underneath remain unclear. On this basis, a series of Fe doped CeO 2 catalysts were synthesized and employed for catalytic ketonization of xylan. Characterization of the catalysts proved the successful formation of the Fe-CeO x solid solution. Doping an appropriate amount of Fe (20–33%) ions on CeO 2 could obviously increase the number of oxygen vacancy and basic sites by up to 56.31% and 29.6%, respectively. During the catalytic reaction of xylan, pure CeO 2 exhibited a good ketonization ability during xylan pyrolysis, and the introduction of a certain amount of Fe further enhanced the ability. The highest yield of ketones was obtained by 33%Fe-CeO 2 , which was 38% higher than pure CeO 2 . The selectivity to linear ketones (acetone and 2-butanone) reached a maximum of 85% for 57%Fe-CeO x . Thus, oxygen-rich compounds had been converted to low oxygen containing and high-quality ketone components. Introducing Fe into CeO 2 favored the production of ethylene glycol rather than 2,3-dihydroxy propanal, and thus promoted the yield of acetone. This investigation provides fundamentals for the deoxygenation of biomass through catalytic ketonization, aiming at the production of value-added ketone products.
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Li Gong,Leben Qiu,Xiaoqian Xing,Jieyun Zhu,Mengzhi Lu,Feier Dong,Yan Yu,Weiting Yu
Selectively reducing nitroaromatics into aromatic amines will not only remove nitroaromatic pollutants in waste effluents to reduce environmental risks, but also yield important feedstocks for chemical industrial manufactures. In this study, a FeCo-co-embedded N-doped Carbon (FeCo-N-C) catalyst with Fe-Co atomic pair has been identified with favorable activity, superior selectivity , excellent reusability, as well as outstanding performance in the treatment of real water. The combined results from theoretical study and experimental tests indicate that the improved catalytic performance of FeCo-N-C is owing to the narrowed band gap and electron delocalization caused by the Fe-Co atomic pair which can improve electron transport in its catalytic reaction. The results of isotope experiments and H* quenching experiments confirm that H 2 O is the source of hydrogen in catalytic reduction of PNP. FeCo-N-C is identified as a superior catalyst to replace multitudinous currently used noble-metal catalysts for the selective catalytic reduction of nitroaromatics in wastewater treatment .
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PubMed
高影响因子
CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Li Guo,Jialing Chen,Shaokang He,Tingyu Liang,Lijun Lu,Shenke Zheng,Xinyue Hu,Lan Yi,Xiaoqin Wu
The [Fe, Al]-FER zeolites, which are prepared from the interzeolite conversion method (from MWW to FER topology) with high Al and Fe content (Si/Al of 8–18 and Si/Fe of 11–13), exhibit excellent catalytic performances and hydrothermal tolerance for NH 3 -SCR reaction. The interzeolite conversion process can be tuned by optimizing the zeolite synthesis conditions such as synthesis gel composition, crystallization time, crystallization temperature, and adding MWW seeds. The work can provide a new strategy to synthesize high Al and Fe content zeolite with high hydrothermal stability for NO x removal.
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DYES AND PIGMENTS
·
2023
·
IF 4.5
Bing Cong,Yuqi Wu,Hongwei Zhou,Chunhai Chen,Xiaogang Zhao
Near-infrared electrochromic materials have garnered great attention due to their potential applications in optical data storage and military camouflage. Herein, a networked metal-organic coordination polymer bearing multi-redox centra ( Fe-MCP ) was successfully prepared by coordination interaction of Fe ions with D-A-D-structure ligands through the liquid-liquid interface self-assembly strategy. The resultant uniform film exhibits improved NIR electrochromic attributed to the construction of mixed-valence system. Furthermore, a sandwich-structured electrochromic device was fabricated by combining Fe-MCP electrochromic layer, a gel composed of LiClO 4 , PMMA , and PC as the electrolyte layer, and anodically coloring PB as an ion storage layer. The resultant device illustrated an optical contrast of 31.4 % at 800 nm and 34.2 % at 1000 nm, a response speed of 4.0 s/8.3 s at 800 nm and 7.6 s/2.7 s at 1000 nm, and good cycling durability. The design principles proposed in this study provide a new insight for the preparation of high-performance NIR electrochromic materials .
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Results in Physics
·
2023
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IF 5.3
Jin Qiu,Wen-Juan Huang,Young Jin Lee,Seung Kim,Xiang-Bai Chen,In-Sang Yang
Magnetism in van der Waals (vdW) materials has recently garnered significant attention due to their potential for advanced applications. In this study, we investigate the magnetic transition in layered MPSe 3 (M = Fe, Mn) bulk flakes utilizing temperature-dependent Raman spectroscopy. Our findings reveal unique features in the Raman spectrum that are strongly correlated with the antiferromagnetic ordering in MPSe 3 . We analyze the spin-dependent Raman scattering modes in MPSe 3 by applying the Suzuki–Kamimura formalism. Consequently, our comparative analyses of the spin correlation function and the reduced magnetization provide compelling evidence of the 2D Ising characteristic especially in FePSe 3 . Our results clearly show the potential of MPSe 3 as a prominent platform for exploring fundamental aspects of low-dimensional magnetism.
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
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IF 4.6
Hangxi Liu,Haorong Sun,Ming Fang,Yifeng Zhang,Mingguang Kong,Zhimin Lv,Xiaoli Tan
The evaluation of the concentration of Pb(II) in solution has great significance in avoiding harm to ecology health. In this work, NH 2 -MIL-53(Fe) modified ITO glass (NH 2 -MIL-53(Fe)@ITO) was utilized as an electrochemical sensor for the detection of Pb(II) in solutions. FTIR and XPS investigation disclosed that the plentiful surface –NH group on the NH 2 -MIL-53(Fe) should be responsible for the highly efficient and selective detection abilities of Pb(II) due to the capture and conductivity abilities. The NH 2 -MIL-53(Fe) was prepared by a solvothermal technique and electrophoresed on the surface of ITO glass . A square wave voltammetry (SWV) method is employed for the sensitive determination of Pb(II). The factors of the detection condition such as the pH and ion interference are also studied. The sensitivity of 16.072 μA μM −1 cm −2 in the linear range of 2–4 μM and 54.143 μA μM −1 cm −2 in the linear range of 5–17 μM, and the limit of detection (LOD) of 0.1 μM are acquired. The repeatability and reproducibility are also studied. EIS and Tafel curves are utilized to investigate the effect of temperatures on the properties of the NH 2 -MIL-53. This work presents a facile strategy for the preparation of NH 2 -MIL-53(Fe)@ITO electrochemical sensor via electrolysis, which enhances the sensitivity toward Pb(II) and shows great application potential.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yiqing Liu,Lin Tian,Zhenran Wang,Yongsheng Fu,Dandan Zhao
Citric acid (CA) can effectively complex with Fe(Ⅲ) to improve the solubility of Fe(Ⅲ) and accelerate the reduction of Fe(Ⅲ) to Fe(II), while its use in Fe(Ⅲ)-activated peracetic acid (PAA) system has not been reported so far. Therefore, CA was introduced into Fe(Ⅲ)/PAA system in this study to degrade oxytetracycline (OTC), and the degradation efficiency and mechanism of OTC in this system were systematically investigated. The results showed that the removal efficiency of OTC in Fe(Ⅲ)-CA/PAA system at pH 7.0 could reach 81.5% after 20 min, and the degradation of OTC followed pseudo-first-order kinetic. The addition of CA into Fe(Ⅲ)/PAA system could effectively reduce Fe(Ⅲ) to Fe(Ⅱ) driving the cycle of Fe(Ⅲ)/Fe(Ⅱ) and accordingly enhance the OTC removal in this system. According to the results of electron paramagnetic resonance (EPR) and scavenging experiments, hydroxyl radical (HO • ) and organic radicals (CH 3 C(O)O • and CH 3 C(O)OO • ) played major roles for the degradation of OTC in Fe(Ⅲ)-CA/PAA system. Four possible transformation paths of OTC in this system were proposed, including demethylation, hydroxylation, dehydrogenation and dehydration, based on five detected degradation products . This study provides an idea to improve PAA activation by Fe(Ⅲ) and broadens the practical application of Fe(Ⅲ) in advanced oxidation processes .
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ACS Catalysis
·
2023
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IF 12.9
Xiaoxue Han,Qiao Zhao,Huiyong Gong,Chongyang Wei,Jing Lv,Yue Wang,Mei-yan Wang,Shouying Huang,Xinbin Ma
Fe-based catalysts undergo complex reduction, carburization, and phase interconversion as well as oxidation during Fischer–Tropsch synthesis (FTS). Unraveling the evolution of carbides and establishing the dominant factors are essential for rational design and modulation of Fe-based catalysts. In this work, Fe–oxide interfaces were constructed to investigate the effect on phase transformation and FTS performance. By correlating performance to the composition of iron species, the crucial role of Fe2.2C in high CO conversion and C5+ productivity has been confirmed. More importantly, a heterogeneous spatial distribution of iron carbides and oxides induced by Fe–oxide interfaces was observed. Fe3O4 preferentially forms at interfaces with the coexistence of carbon-rich Fe2.2C at subadjacent interfaces, while Fe5C2 locates at the region away from oxides or in the bare Fe catalyst. Further ex/in situ characterizations, including XPS, TPO, in situ XRD, and in situ IR, were conducted for revealing the mechanism. This study provides insights for iron carbides formation and stability by modulating interfaces, which guides the further development of Fe-based FTS catalysts.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Shaoqi Zhang,Haiyang Yu,Yi Wang,Yuxiang Yan,Jun Dai,Dajun Shu,Xinglong Wu
CO2 possesses extraordinary thermodynamic stability, and its reduction reaction involves multiple electron-transfer processes. Thus, high-density electron occupation on a catalyst surface is an effective driving force for improving the photocatalytic activity. Here, we report on the fabrication of Fe-doped Bi2O3 catalysts (denoted as FexBi2-xO3) with different Fe contents using the solvothermal method. The self-assembled catalyst has a nanoflower-like morphology, and its performance of CO2 reduction to CO is improved largely dependent on the Fe content. In the sample with a 7.0% Fe content (Fe0.07Bi1.93O3), the CO evolution rate reaches 30.06 μmol g–1 h–1, which is about 6 times higher than the 4.95 μmol g–1 h–1 of pristine Bi2O3, and shows excellent photostability after three cycles, with each cycle lasting for 7 h. Theoretical calculation and spectral characterization reveal that such a good CO2 reduction reaction performance arises from effective surface occupation of Fe, which not only enhances sunlight absorption but also significantly increases the surface electron density on the double metal active sites. This work provides a new strategy for improving the photocatalytic performance by surface metal doping in some metal oxide photocatalysts.
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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Chengcheng Qi,Yuhua Luo,Yongping Dong
The study of single atoms in the field of electrochemical sensing is at the early stage. How to boost the catalytic performance of single atoms is still a big challenge. Herein, we prepare Fe-Se dual single-atom sites on N-doped ultrathin carbon carrier (Fe 1 Se 1 /NC) for realizing highly sensitive nonenzymatic detection of H 2 O 2 . Fe 1 Se 1 /NC was synthesized through the pyrolysis strategy, and then was characterized by transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS) mapping, high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray diffraction (XRD), X-ray photoelectron spectrometer (XPS), and electrochemical techniques, respectively. The results displayed that Fe and Se both existed in an atomically dispersed status. Compared to the single-atom Se or Fe catalyst (Se 1 /NC or Fe 1 /NC), the Fe 1 Se 1 /NC significantly boosted the electrocatalytic activity for H 2 O 2 reduction. The Fe 1 Se 1 /NC modified electrode could be used to detect H 2 O 2 in a wide linear range of 0.02 mM to 13 mM with a high sensitivity of 1508.6 µA·mM −1 ·cm −2 and a low detection limit of 11.5 µM. Moreover, the sensor was successfully employed for detecting H 2 O 2 in disinfectant and urine samples. This work provides a novel design of dual-atom catalysts for excellent electrochemical sensing applications.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 23
·9446-9458
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IF 4.5
Cheng Zhipeng,Yin Jingzhou,Chu Xiaozhong,Yang Tingting,Gao Yuan,Zhong Hui,Zhang Lili
Transition metals (TMs) have an excellent catalytic effect on the thermal decomposition of ammonium perchlorate (AP). However, nanosized TM catalysts tend to agglomerate due to their high surface energy and magnetism. In this work, a new Fe/Al composite catalyst was synthesized by loading Fe nanoparticles onto Al powder through a facile replacement route, and its effect on the thermal decomposition stability of AP and AP-based propellants was investigated. Morphological and structural characterization showed that Fe nanoparticles were successfully decorated on the Al surface without noticeable aggregation or shedding. The diameter of Fe nanoparticles was approximately 10 nm. The constructed Fe/Al composite catalyst presented a strawberry-like structure. Elemental mapping analysis revealed that the dispersion state of the Fe/Al composite catalyst was better than that of commercial Fe nanoparticles with AP. Thermal analysis indicated that the Fe/Al composite catalyst presented excellent catalytic stability in the high-temperature decomposition (HTD) of AP, reducing the HTD temperature by approximately 100 °C. Burning tests showed that the relative standard deviations of the burning rate with the Fe/Al composite catalyst were 2.5 and 2.2% at 5 and 10 MPa, respectively, whereas those with Fe reached 17.1 and 13.9% at 5 and 10 MPa, respectively. The Fe/Al composite catalyst inherited the good dispersion of Al, effectively resolving the problems of Fe nanocatalyst agglomeration. Therefore, the as-obtained Fe/Al composite catalyst can significantly improve the thermal decomposition stability of AP and AP-based propellants and will have wide application prospects in the field of AP-based propellants.
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