CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Siyuan Sun,Fan Yang,Xiaoyun Zhang,Jinxiu Qian,Kexin Wei,Junpu An,Yang Sun,Shuyang Wang,Xi Li,Yongfeng Li
Transition metal single-atom catalysts (SACs) have been widely used in oxygen reduction reactions (ORR) and oxygen evolution reaction (OER) due to its greatest atomic utilization and low costs, which catalytic performance can be further enhanced by electron distribution adjustment. Herein, we synthesized a carbon-encapsulated FeS/Fe 3 C nanoparticles doped carbon-based Fe single atom catalyst from fluid catalytic cracking (FCC) slurry though a one-pot pyrolysis. The synergistic effect between FeS/Fe 3 C nanoparticles and Fe single atom structure (FeN x ) promotes the ORR/OER processes, which may due to the reduction of the adsorption free energy of intermediates. Meanwhile, the polyaromatic hydrocarbon in FCC slurry enhances the graphitization of catalyst to facilitate charge transfer in electrocatalysis process, and the carbon-encapsulated nanoparticles sites possess higher stability and dispersion. As a result, the optimized catalyst (FeS/Fe 3 C@Fe-N-C) presents a high nanoparticles dispersion and graphitization level, which has a higher ORR catalytic ability (E 1/2 = 0.91 V vs RHE) compared with commercial Pt/C (20 wt%, E 1/2 = 0.879 V vs RHE) and a similar OER catalytic ability (E 10 = 0.1.506 V vs RHE) compared with RuO 2 (E 10 = 1.518 V vs RHE). A liquid Zn-air battery assembled with FeS/Fe 3 C@Fe-N-C show a peak power density of 113 mW cm −2 and an open potential of 1.432 V. This work sheds light on a new method to design transition metal active sites carbon based single-atom catalyst for enhanced ORR and OER processes.
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高影响因子
ELECTROCHIMICA ACTA
·
2025
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IF 5.6
Fei Qian,Liuyi Hu,Yonggen Jin,Linhe Li,Ruyi Fang,Jun Zhang,Xinping He,Yongping Gan,Yang Xia,Xinhui Xia,Wenkui Zhang,Hui Huang
All-solid-state lithium-sulfur batteries (ASSLSBs) with high theoretical energy have attracted much attention benefiting from fundamentally addressing the adverse shuttling effect. However, the development of stably operated ASSLSBs remains a great challenge due to the low conductivity and utilization of sulfur. Inspired by the polar single-atom catalyst with 100 % theoretical atomic utilization, a simple and effective strategy is proposed to improve the electrochemical performance of ASSLSBs by introducing Fe nanoparticles into the carbon host material (Ketjen black, KB). The in-situ grown Fe nanoparticles not only enhance the conductivity of the host material, but also promotes the conversion reaction of sulfur, resulting in the improvement of sulfur utilization and redox kinetics. Therefore, the initial discharge capacity of the assembled Fe-KB/S cell reaches 976 mA h g −1 at 50 mA g −1 , which is significantly higher than that of the KB/S cell (727 mA h g −1 ). Moreover, the Fe-KB/S cell maintains a reversible specific capacity of 520 mA h g −1 after 150 cycles, which is almost twice that of the KB/S cell. This study provides a valuable reference for the further development of ASSLSBs.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 21
·12712-12720
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IF 10.7
Tianhao Yu,Peng Gao,Hong Du,Ling Dong
Metal–organic frameworks (MOFs) have recently been reported as promising catalysts for the oxygen evolution reaction (OER). Hence, we chose hydroxyl-rich 2,5-dihydroxyterephthalic acid as the ligand to prepare a novel MIL-100 and wrapped it on the NiCo-ZIF-67 surface to obtain an amorphous hollow material (NiCo-ZIF-67@Fe-MIL-100, denoted as NiCo-ZIF@MIL). The composite material presents a low overpotential (η ≈ 139 mV @ 10 mA cm−2), a small Tafel slope (119 mV dec−1) and great stability for the OER in 1 M KOH solution. Density Functional Theory (DFT) calculations show that the hydroxyl-rich structure, which accelerates OH− transfer and promotes the formation of the Co–O–Fe bridge, effectively reduces the reaction energy barrier (from 2.67 eV for NiCo-ZIF-67 to 2.08 eV for NiCo-ZIF@MIL). This work provides an important reference for the development of double-MOF materials.
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CHEMOSPHERE
·
2024
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IF 8.1
Jingyuan Yue,Xiaojin Hu,Huijun Xie,Zhen Hu,Haiming Wu,Jian Zhang,Bo Sun,Lushan Wang
Bisphenol A (BPA) in seawater tends to be deposited in coastal sediments. However, its degradation under tidal oscillations has not been explored comprehensively. Hydroxyl radicals (·OH) can be generated through Fe cycling under redox oscillations, which have a strong oxidizing capacity. This study focused on the contribution of Fe-mediated production of ·OH in BPA degradation under darkness. The removal of BPA was investigated by reoxygenating six natural coastal sediments, and three redox cycles were applied to prove the sustainability of the process. The importance of low reactivity Fe(II) in the production of ·OH was investigated, specifically, Fe(II) with carbonate and Fe(II) within goethite, hematite and magnetite. The degradation efficiency of BPA during reoxygenation of sediments was 76.78–94.82%, and the contribution of ·OH ranged from 36.74% to 74.51%. The path coefficient of ·OH on BPA degradation reached 0.6985 and the indirect effect of low reactivity Fe(II) on BPA degradation by mediating ·OH production reached 0.5240 obtained via partial least squares path modeling (PLS-PM). This study emphasizes the importance of low reactivity Fe(II) in ·OH production and provides a new perspective for the role of tidal-induced ·OH on the fate of refractory organic pollutants under darkness.
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MICROCHEMICAL JOURNAL
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2025
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IF 5.1
Renjie Wang,Yifan Zhu,Shanshan Liu,Kai Jiang,Runan Wang,Shuangshuang Ji,Mengyao Ma,Qianqian Chen,Huijuan Ran,Xudong Song
Uric acid (UA) levels serve as pivotal health biomarkers, underscoring the need for accurate detection methodologies. This paper presents a novel and straightforward electrochemical approach for UA detection, utilizing a sensing platform that integrates hybrid electrodes of Fe-MOF and polypyrrole (PPy). The findings reveal that the sensor shows exceptional sensitivity to UA across a wide concentration range of 1–300 µM, featuring an impressively low limit of detection (LOD) at 0.212 µM. Moreover, the sensor retains a peak current response of 87.2 % even after one month, underscoring its excellent stability and robust anti-interference properties. The improved sensing performance is due to the composite material’s retention of PPy’s superior electronic transport characteristics, combined with the enhanced specific surface area, active sites, and porosity contributed by the Fe-MOF component, leading to a substantial enhancement in electrochemical sensing capabilities. This research paves the way for the utilization of MOF nanomaterials in electrochemical sensing, thereby facilitating the practical application of nanocomposites.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2024
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IF 4.1
Bolong Liang,Ming Su,Zhe Zhao,Shu-xuan Liang
Microbial fuel cell (MFC), simultaneously degrading organic pollutants and harvesting electricity, suffers from a sluggish oxygen reduction reaction (ORR) on cathode. The catalysts for Pt substitution are crucial to enhance the ORR performance and power output. Thus, a Co and Fe co-doped carbon derived from ZIF-67 (Co/Fe-NC) is prepared, which is proved to have excellent electrochemical properties. When the catalyst Co/Fe-NC is equipped in microbial fuel cell, the maximum power density of 1831 ± 57 mW m −2 is achieved, which is 13.5 % higher than that of Fe@Co-NC and 49.3 % higher than that of Co-NC. Moreover, the electrochemical tests show that Co/Fe-NC has a smaller charge transfer resistance and a higher exchange current density, which implies the faster kinetics of ORR. The enhanced performance of Co/Fe-NC can be attributed to the rougher rhombic dodecahedral interface, larger surface area, various types of nitrogen species, critical roles of cobalt and iron species, both high graphitization and defects. All these characteristics are responsible for the significant increase in ORR activity and power output. This work designs and compares different catalysts derived from iron-involved ZIF-67, and demonstrates a superior ORR electrocatalyst of Co/Fe-NC, which can be a potential alternative to Pt in the MFC practical application.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Dongli Shang,Binze Zhang,Lijie Zhang,Jin Li,Yongtao Zhao,Yuhu Huang,Kaibin Tang,Changrong Xia
Perovskite oxide La 0.5 Sr 0.5 FeO 3-δ (LSF) is a potential Co-free electrocatalyst for oxygen reduction reaction (ORR) in solid oxide fuel cells (SOFCs). To improve its catalytic activity, this work performs multi-element doping to the A-site elements La and Sr, forming a high-entropy oxide Ba 0.2 Sr 0.2 La 0.2 Pr 0.2 Sm 0.2 FeO 3-δ (H-LSF) and a medium-entropy material Ba 0.35 Sr 0.35 La 0.1 Pr 0.1 Sm 0.1 FeO 3-δ (M−LSF). The multi-element doping effects are investigated on various physicochemical properties including crystalline structure, chemical compatibility with electrolyte, valence state of B-site Fe, amount of adsorbed oxygen species, oxygen nonstoichiometric value, sinterability, thermal expansion coefficient, electrical conductivity, chemical oxygen surface exchange coefficient ( k chem ), and electrochemical performance. While the multi-element doping does not change the phase structure and compatibility, it decreases the electronic conductivity, increases the oxygen vacancy concentration and k chem . Consequently, it improves ORR activity such as reduces interfacial polarization resistance and elevates peak power density. The best performance is observed with the medium-entropy perovskite rather than the high-entropy material. M−LSF shows k chem of 21.5 × 10 − 5 cm s −1 at 750 °C, 32 % higher than H-LSF and 4 times as high as LSF. In addition, M−LSF electrode exhibits interfacial polarization resistance of 0.090 2 at 750 °C, about 1/2 of H-LSF and 1/5 of LSF. Furthermore, single cell with M−LSF cathode demonstrates peak power density of 1.72 W cm −2 at 800 °C, 25 % higher than H-LSF and more than twice as LSF. Therefore, multi-element doping to the A-site of ferrite-based cobalt-free perovskite could be an effective method to improve the cathode performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Xiaotong Yang,Kaiyu Dong,Zhe Zheng,Yuehuan Zhang,Qiang Yuan
Efficient C C bond cleavage and the complete oxidation of alcohols are key to improving the efficiency of renewable energy utilization. Herein, we successfully prepare porous Fe-doped hexagonal close-packed ( hcp )-PtBi/face-centered cubic ( fcc )-Pt heterostructured nanoplates with abundant grain/phase interfaces ( h -PtBi/ f -Pt@Fe 1.7 PNPs) via a simple solvothermal method. The open porous structure, abundant grain/phase interface and stacking fault defects, and the synergistic effect between intermetallic hcp -PtBi and fcc -Pt make h -PtBi/ f -Pt@Fe 1.7 PNPs an effective electrocatalyst for the glycerol oxidation reaction (GOR) in direct glycerol fuel cells (DGFCs). Notably, the h -PtBi/ f -Pt@Fe 1.7 PNPs exhibit an excellent mass activity of 7.6 A mg Pt −1 for GOR, 4.75-fold higher than that of commercial Pt black in an alkaline medium. Moreover, the h -PtBi/ f -Pt@Fe 1.7 PNPs achieve higher power density (125.8 mW cm −2 ) than commercial Pt/C (81.8 mW cm −2 ) in a single DGFC. The h -PtBi/ f -Pt@Fe 1.7 PNPs can also effectively catalyze the electrochemical oxidation of 1-propanol (17.1 A mg Pt −1 ), 1,2-propanediol (7.2 A mg Pt −1 ), and 1,3-propanediol (5.2 A mg Pt −1 ). The in-situ Fourier-transform infrared spectra further reveal that the C C bond of glycerol, 1-propanol, 1,2-propanediol, and 1,3-propanediol was dissociated for the complete oxidation by the h -PtBi/ f -Pt@Fe 1.7 PNPs. This study provides a new class of porous Pt-based heterostructure nanoplates and insight into the intrinsic activity of different C3 alcohols.
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高影响因子
Journal of Geophysical Research-Biogeosciences
·
2025
·Vol. 130
·期 3
·e2024JG008675
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IF 3.5
Zhengqi Su,Huaming Guo,Zhipeng Gao,Tiantian Ke,Xiaojun Feng,Lingzhi Zhang
Although the reduction of pentavalent arsenic (As(V)) bound to Fe(III) (hydr)oxides (As(V)-containing FeOOH) coupled with organic matter (OM) degradation has received extensive attention, little is known about in situ reduction of FeOOH mineral-bound As(V) (As(V) (s) ) via electron shuttling in the presence of As(V)-reducing bacteria (AsRB). Here, anthraquinone-2,6-disulfonate (AQDS), Suwannee River humic acid (SRHA), and fulvic acid (SRFA) were used to establish an agar electron shuttle system with ferrihydrite-As(V)/goethite-As(V) and AsRB, which was isolated from high-As groundwater as the candidate strain (RA-1). We found that AQDS was more efficient in shuttling electrons to reduce As(V) (s) and Fe(III) than SRHA and SRFA. High contents of quinone moieties in AQDS indicated that quinone moieties were conducive to As(V) (s) and Fe(III) reduction. The reduction kinetic rates ( K red ) of As(V) (s) were higher than those of Fe(III), indicating the occurrence of in situ As(V) (s) reduction via electron shuttling. Furthermore, K red of As(V) (s) for ferrihydrite-As(V) systems was greater than that of goethite-As(V) systems, demonstrating that As(V) bound to ferrihydrite via monodentate was more easily reduced than that bound to goethite via bidentate. The relative expression levels of As metabolic genes ( ars C, arr A, and ars B) initially increased and then decreased in the late stage of experiments. High As concentrations in suspension inhibited the transcriptional activity of As metabolic genes in the late stage, reducing the electron production efficiency of RA-1 and subsequently slowing in situ reduction of As(V) (s) . This study highlights the importance of OM electron shuttling in the reduction of As(V) (s) , offering new perspectives in As enrichment in groundwater. Plain Language Summary OM can promote microbial As(V) reduction in high As groundwater systems. As a result, we explored how FeOOH mineral-bound As(V) could be in situ reduced via electron shuttling between AsRB and different OM. Our findings showed that AQDS was more effective than other two natural organic matter (NOM, i.e., SRHA and SRFA) in reducing both As(V) (s) and Fe(III), due to its high content of quinone moieties. The results of kinetic analysis demonstrated in situ reduction of As(V) (s) , and As(V) bound to ferrihydrite was more readily reduced than As(V) bound to goethite. In addition, the transcriptional activities of three As metabolic genes initially increased but later declined due to high As concentrations, which further slowed the As(V) (s) reduction process. Overall, these findings provide new insights into organic-mediated As cycling in contaminated groundwater. Key Points High quinone contents in AQDS led to a higher reduction extent of As(V) (s) than in SRHA and SRFA The values of K red, As were greater than those of K red, Fe , demonstrating in situ reduction of As(V) (s) Changes in As metabolic genes affected the electron production efficiency of RA-1 and As(V) (s) reduction
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Surfaces and Interfaces
·
2024
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IF 5.7
Yitong Guo,Yukai Chang,Libo Wang,Qixun Xia,Aiguo Zhou
In this work, two−dimensional Mo 2 CT x MXene pillared with transition metal complexes [Fe(III), Co(III), or Ni(II)] was prepared, which shows ultra−high performance as the anode of lithium−ion batteries (LIBs). Firstly, Mo 2 CT x was pretreated with hexadecyl trimethyl ammonium bromide (CTAB) as a surfactant and then mixed with hydrated chloride (FeCl 3 ·6H 2 O, CoCl 2 ·6H 2 O, or NiCl 2 ·6H 2 O) at room temperature. The molar ratio of MXene to hydrated chloride was 1:1. In this process, metal ions (Fe 3+ , Co 2+ , or Ni 2+ ) were successfully loaded on the nanosheets of Mo 2 CT x . The ions were combined with the surface terminated oxygen of MXene to form transition metal complexes by liquid phase agitation method. Moreover, transition metal complexes contribute a portion of their capacity and help Mo 2 CT x enhance its own capacity to a large extent. However, the electrochemical effects on Mo 2 CT x vary depending on the type of transition metal ions. As anodes of LIBs, the final discharge specific capacities after 100th cycles at 2 A g −1 were 511.68 mAh g −1 , 229.22 mAh g −1 and 78.19 mAh g −1 for Fe(III)@Mo 2 CT x , Co(III)@Mo 2 CT x , and Ni(II)@Mo 2 CT x , respectively, while the capacity of pure Mo 2 CT x after delamination was only 31.17 mAh g −1 . At 6 A g −1 , the final discharge capacity of Fe(III)@Mo 2 CT x was 227.4 mAh g −1 after 500th cycles. Therefore, Mo 2 CT x MXene pillared by the complexes, especially Fe(III) complexes, is a promising anode material with high−performance for lithium−ion batteries.
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LANGMUIR
·
2024
·
IF 3.7
Liyun Zhang,Xin Wen,Qingxia Ming,Xue luo,Tianfeng He,Tian Chen,Minghang Jiang,Mengjun Wang,Lan Ma
With environmental pollution becoming more serious, developing efficient treatment technologies for all kinds of organic wastewater has become the focus of current research. In this work, the coaxial electrospinning technology was used to one-step fabricate a porous and underwater superoleophobic polyacrylonitrile nanofibrous membrane with an Fe-based metal–organic framework (MIL-100(Fe)). Benefiting from the synergistic effect of two jets, the nanofibers are smaller and denser, which prompt the exposure of more nanomaterial additives (MIL-100(Fe)). The BET surface area increased to 202.888 m2/g, and the membranes demonstrated outstanding underwater superoleophobicity. Moreover, compared with traditional blended matrix membranes by the single-axis method, separation of the modifier and membrane matrix material by coaxial methods also maintained excellent mechanical properties, which enhanced Young’s modulus 3.4 times (∼1.34 MPa). As a result, facing soluble dyes, the porous C-PAN/MIL-100(Fe) membrane can demonstrate outstanding and fast adsorptive property (the Qm of MB and CR reached 44.71 and 88.74 mg g–1, respectively). For oily emulsion, the hydrophilic and oleophobic nanofibrous reticular surface provided excellent separation performance (flux: 1124.0–1549.3 L m–2 h–1, R > 98%). Moreover, the porous and underwater superoleophobic C-PAN/MIL-100(Fe)-0.5 membrane can synchronously purify the dye/oil mixture emulsions by one-step filtration. Based on the above performance, we believe that the modified nanofibrous membrane prepared by one-step coaxial electrospinning technology can promote more studies of the development of membrane preparation technology in the field of oily wastewater treatment.
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Small
·
2024
·
IF 13
Hongliang Fu,Yue Lian,Yongfeng Hu,Jing Zhao,Huaihao Zhang
The development of highly stable and strongly active electrode materials for sodium-ion batteries (SIBs) and overall water splitting (OWS) is critical in sustainable energy storage and conversion systems. Here, a new electrode material N-Fe-C@Nb 2 CT x is introduced, with a layered sandwich structure consisting of N-doping Fe-MOF derived-nanorods (Fe-C) and Nb 2 CT x MXenes. Specifically, Nb 2 CT x obtained by etching Nb 2 AlC with HF acid is used as the main body to construct the layered sandwich structure with Fe-C as the filler. Benefiting from this structure, Fe-MOF grows in situ within Nb 2 CT x , which restrains MXenes aggregation and stacking and also alleviates the bulk effect of sodium-ion embedding/de-embedding, thus improving its stability. Again, the more exposed active sites from the layered sandwich structure and N-doping introduction ensure high reactivity as electrode materials. In addition, Fe-C nanorods strengthen the linkage between the Nb 2 CT x layers and N-doping enhances the ion/electron transport rate, thereby boosting the effective mass transfer and electrical conductivity. Density functional theory (DFT) calculations show that Fe-C and N-doping help increase the density of states (DOS) and material electrical conductivity. Meanwhile, the generated oxygen species (*OH and *O) in OER are captured by in situ FT-IR test. As a result, the N-Fe-C@Nb 2 CT x electrochemical test displays good electrochemical performance in SIBs and OWS.
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