WATER RESEARCH
·
2025
·
IF 12.4
Quan Liao,Lianpeng Sun,Huanzhong Deng,Siru Zhou,Mingxuan Li,Xinzhe Zhu,Chao Yang,Xiao-yan Li,Lin Lin,Ruo-hong Li
The bio-iron system effectively overcomes the bottleneck in the biosynthesis of medium-chain fatty acids (MCFAs) by enhancing extracellular electron transfer capability. However, the key structural characteristics and dynamic evolution of iron-based electron shuttles remain unclear, limiting system optimization and mechanistic understanding. Among the tested iron species in this study, Fe 3 O 4 exhibited the most favorable extracellular electron transfer performance and MCFAs production, highlighting its potential as an efficient electron shuttle. In addition, this study revealed that microorganisms can induce partial transformation of iron powder and Fe 2 O 3 into Fe 3 O 4 through redox cycling. In contrast, FeCO 3 lacked both structural reconfiguration ability and electron transfer activity, thus limiting MCFAs biosynthesis. Partial least squares regression model, combined with characterization analysis, identified the Fe(III)-O-Fe(II) structure as the key structural characteristics of the electron shuttle. Moreover, X-ray absorption fine structure analysis, interpreted through Marcus theory, demonstrated that bio-driven Fe O bond shortening reduces reorganization energy, while Fe Fe bond elongation expands the electron transfer network. This study elucidates, at the atomic level, the microbial mechanisms underlying the construction and regulation of iron-based electron shuttles, providing a theoretical foundation for the design of bioinspired materials and the optimization of bio-iron systems.
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PubMed
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Sheraz Muhammad,Bowen Yao,Aling Zhou,Zhiyang Huang,Sumayya Khan,Fengli Wei,Zuyang Luo,Tayirjan Taylor Isimjan,Xiulin Yang
Unlocking the full potential of metal-organic frameworks (MOFs) for water-splitting applications requires innovative strategies to enhance their catalytic efficiency and stability. Here, we introduce a Mo-doped Fe-based MOF (MoFe-NH2-BDC) with a unique 2D nanosheet and plate-like morphology to revolutionize the oxygen evolution reaction (OER). Mo incorporation optimizes electronic properties, accelerates charge transfer, and dynamically reconstructs the catalyst surface into highly active FeOOH species, ensuring long-term performance. This next-generation electrocatalyst achieves an ultra-low overpotential of 254 mV at 20 mA cm‒2, with a rapid Tafel slope of 66 mV dec‒1, surpassing conventional RuO2 catalysts. Operando Raman and ATR-FTIR spectroscopy reveal that Mo facilitates an adsorbate evolution mechanism (AEM), stabilizing intermediates and boosting reaction kinetics. In a practical two-electrode system, MoFe-NH2-BDC (+) || Pt/C (−) demonstrates an exceptional cell voltage of 1.58 V at 100 mA cm‒2, maintaining stability for 85 h. These results underscore the transformative impact of Mo doping in MOFs, paving the way for highly efficient, durable, and scalable electrocatalysts for sustainable energy applications.
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RENEWABLE ENERGY
·
2024
·
IF 9
Yuming Huang,Wei Zhou,Liang Xie,Junfeng Li,Xiaoxiao Meng,Xuewei Zhang,Yang Yu,Miaoting Sun,Jiaxiang Chen,Lijie Wang,Jihui Gao,Guangbo Zhao
Integrating the hydrogen evolution reaction (HER) with the carbon oxidation reaction (COR) is a promising method for producing H₂ with lower energy consumption. However, due to the passivation effect of oxygen functional groups (OFGs) for COR and Fe³⁺, achieving efficient and sustainable carbon oxidation to assist water electrolysis for hydrogen production remains a challenge over the past decades. This study introduced [EDTA·Fe(III)] – as a mediator to promote COR. [EDTA·Fe(III)] – effectively prevented the oxidation layer on the carbon surface from anchoring Fe (III) and reactivated the carbon that had been passivated by the oxidation layer. Density functional theory calculations indicated that the notable COR activity resulted from [EDTA·Fe(III)] – effectively lowering the vertical ionization potential of carbon, without being affected by OFGs. Notably, in the HER||COR-[EDTA·Fe(III)] – system, a cell voltage of merely 0.74 V is sufficient to reach a current density of 10 mA cm −2 , with the corresponding energy consumption being 1.76 kWh Nm −3 (H 2 ). This strategy offers new insights into achieving stable, low-energy hydrogen production via water electrolysis.
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高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Jiangang Kang,Haihong Zhang,Yuehui He,Liang Wu,Hengdi Ye,Jinchao Wei
The novel Ni-Si intermetallic compounds are fabricated by elemental powder metallurgy. This study explores the synthesis of a series of catalysts (Ni-Si-M, M=Co, Fe, Mn) by alloying to augment the low-temperature efficiency of CO oxidation using Ni-Si intermetallic compounds. It is found the low-temperature catalytic activity of Ni-Si-Co, Ni-Si-Fe, and Ni-Si-Mn catalysts are significantly enhanced compared to the original Ni-Si. The catalytic activity among the catalysts ranks as follows: Ni-Si-Co > Ni-Si-Fe > Ni-Si-Mn > Ni-Si. The apparent activation energy (Ea) for Ni-Si-Co was the lowest at 57.3 kJ/mol, suggesting its efficient catalytic oxidation of CO. Additionally, the addition of Co, Fe and Mn elements actually promotes the generation of Ni 2+ as the CO adsorption site in the original Ni-Si. The addition of Co element also leads to the formation of Co 2+ as the adsorption site of O 2 in the process of CO oxidation reaction. The synergistic adsorption of Ni 2+ and Co 2+ to CO and O 2 promotes the CO oxidation reaction. Additionally, the catalysts demonstrate robust long-term stability in atmospheres containing H 2 O and SO 2 , with CO conversion initially suppressed but subsequently recovering and stabilizing at over 90%. This investigation offers novel insights into enhancing the low-temperature activity and stability of catalysts.
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高影响因子
MOLECULES
·
2025
·Vol. 30
·期 8
·1708
·
IF 4.6
Yashu Li,Nan Wang,Lu Zhao,Xuanhe Liu,Lin Wang,Chengcheng Xie,Jing Li
Developing low-cost, efficient, and scalable non-precious metal electrocatalysts for the oxygen reduction reaction (ORR) remains a critical challenge in the field of energy conversion. Among various candidates, Fe-N-doped carbon materials have garnered attention as promising alternatives to commercial Pt/C catalysts for ORR. In this study, we report an Fe-N catalyst synthesized by incorporating iron phthalocyanine withCinnamomum longepaniculatumwaste leaves as the carbon source. This catalyst exhibited an excellent four-electron ORR activity and the half-wave potential (E1/2) reaches 0.875 V, which was superior to that of commercial Pt/C (E1/2= 0.864 V). Additionally, the catalyst exhibits superior methanol tolerance and stability compared to commercial Pt/C. This approach, which utilizes biomass waste for the synthesis of electrocatalysts, not only provides an effective solution for reducing environmental waste but also addresses the issue of sluggish cathodic ORR kinetics in fuel cells, making it suitable for low-cost, large-scale industrial production.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Yihe Qin,Run Yuan,Shaojun Luo,Haiming Huang,Xuwen He
Catalysts with high catalytic performance are crucial for the catalytic ozonation of organic wastewater. This study synthesized an efficient, stable, and practical Fe-Mn/Al 2 O 3 ozone catalyst for wastewater treatment using an impregnation calcination method, and applied it in the catalytic ozonation of wastewater. When the concentration of manganese nitrate was 0.15 mol/L, the Mn/Fe ratio was 3:1, the immersion time was 24 hours, the calcination temperature was 500 ℃, and the calcination time was 4 hours, the prepared Fe-Mn/Al 2 O 3 had the best catalytic effect on simulated wastewater, with a chemical oxygen demand (COD) removal efficiency of 73.6%. At the same time, the physicochemical properties of the catalyst were investigated, and the catalytic effect of the catalyst on actual coking wastewater was investigated on a laboratory scale. When the ozone concentration was 20 mg/L, the gas flow rate was 0.5 L/min, the catalyst concentration was 400 g/L, and the pH was 7.02, the actual COD removal efficiency of coking wastewater was 71.6%. The pilot test results showed that the COD of the treated coking wastewater could stably meet the standard (COD<80 mg/L), with an average COD removal rate of about 58.3%, indicating that the Fe-Mn/Al 2 O 3 had high catalytic activity and good stability. Kinetic analysis showed that the degradation process of organic pollutants followed the pseudo-second-order kinetic equation. The results of water quality analysis such as conventional water quality indicators, fluorescence spectroscopy, and molecular weight classification indicated that the large molecular organic pollutants were efficiently degraded. Mechanism analysis indicated that the active components of the catalyst reacted with ozone through electron transfer to enhance the ozone utilization efficiency and efficiently remove organic pollutants. This study can provide theoretical support and technical reference for the standardized discharge of coking wastewater in the future.
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高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Ziyi Wang,Xin Lian,Rongyan Yang,Xiaomeng Guo,Shengjie Wei,Jijie Zhang,Xian-He Bu
Introducing polarity in traditional metal-N4 catalytic sites and strengthening the adsorption of polar NO2* intermediate are advantageous for the deep reduction of nitrate into ammonia. Herein, the planar chlorination engineering strategy successfully introduced the C–Cl bonds adjacent to the Fe–N4 catalytic site with higher polarity, effectively boosting the catalytic activity for the nitrate reduction reaction (NO3RR). The maximal NH3 yield rate and the corresponding turnover frequency (TOF) value catalyzed by the Fe–N4/CNCl catalyst were 1.82 mg h–1 cm–2 and 245 h–1 at −0.83 V vs RHE, which were 3.4 times and 2.7 times those of the traditional Fe–N4/CN catalyst without polarity, respectively. The Fe–N4/CNCl catalyst also exhibited satisfactory stability during consecutive 15 cycles. The density functional theory (DFT) calculation revealed that the planar chlorination engineering of the Fe–N4 site with higher polarity strengthened the adsorption of polar NO2* intermediate, facilitated the deep reduction of nitrate into ammonia, lowered the energy barrier of rate-determining step (RDS) and thus improved the catalytic activity. This work exhibited the enormous advantage of a planar chlorination engineering strategy for enhancing the activity of electrocatalysis by introducing polarity in the traditional metal-N4 catalytic site.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Shichao Cai,Yurou Tan,Hongyi Li,Liwei Yang,Bo Chen,Feng He
Zero-valent iron (ZVI, Fe0) can effectively reduce a variety of chlorinated hydrocarbons. However, ZVI is incapable of dechlorinating 1,2-dichloroethane (1,2-DCA), a commonly found contaminant in groundwater, and the existing ZVI modification methods have little effect on this predicament. In this study, we prepared ZVI composites modified with Fe–N4 coordination structure (Fe0@FeNC), which exhibited outstanding dechlorination performance toward 1,2-DCA. Fe0@FeNC (1 g/L) can degrade 94% of 1,2-DCA (10 mg/L) within 37 days, with an ethene selectivity of nearly 100%, whereas nanoscale ZVI (nZVI) or even Pd-doped nZVI and sulfidated ZVI cannot degrade 1,2-DCA. The results from X-ray diffraction patterns and Mössbauer spectra confirmed the presence of Fe0 and Fe–N4 coordination structure in the Fe0@FeNC, which were proven to be the electron donor and dechlorination active center for 1,2-DCA dechlorination, respectively. Theoretical calculation reveals that the Fe–N4 coordination structure can reduce the free energy required for 1,2-DCA reduction, thus allowing 1,2-DCA to utilize electrons provided by Fe0 to achieve dechlorination. These findings can guide the design of ZVI-based materials to achieve in situ abiotic remediation of 1,2-DCA-contaminated groundwater.
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高影响因子
FUEL
·
2025
·
IF 7.5
Xudong Leng,Luxuan Huang,Yongjin Sun,Xuekun Jin,Fengjuan Chen,Haiming Duan,Biaobing Cao
Platinum-based alloy catalysts have achieved notable progress in oxygen reduction due to their unique electronic structures, but conventional alloying often causes nanoparticle agglomeration and sintering. Here, PtM (M = Fe, Co, Ni) alloys are synthesized using XC-72R carbon black as support. PtFe nanoparticles (∼3.1 nm) are uniformly dispersed and exhibit strong electronic interactions, optimizing the Pt electronic structure. The Pt 2 Fe 1 /C catalyst delivers a half-wave potential of 0.849 V, with mass and specific activities 1.57 and 3.31 times higher than commercial Pt/C, retaining 94.4 % activity over 9 h. It also exhibits excellent hydrogen evolution performance, requiring only 36 mV overpotential at 10 mA cm −2 . Density functional theory indicates that alloying downshifts the Pt d-band center, reducing *OH adsorption energy and enhancing catalytic activity. This work demonstrates a synthesis strategy for stable Pt alloys with superior bifunctional performance in both oxygen reduction and hydrogen evolution reactions.
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高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2025
·
IF 4.6
Huiping Wu,Hui Sun,Bin Yu,Afang Gao,Gaoyuan Chen,Xinyu Liu,Shijie Wang,Yutong Feng
Recently, the rapid growth of the textile, printing, and dyeing industries has led to severe pollution from dye wastewater. Bimetallic metal-organic frameworks (bimetallic MOFs) have emerged as promising adsorbents for dyes removal. Herein, Fe-HKUST-1 with an octahedral structure was anchored on the surface of viscose spunlaced nonwoven material (VSN) via an in situ solvothermal method to prepare Fe-HKUST-1@VSN. After carbonization, Fe-HKUST-1@VSNC was obtained for the adsorption of organic dyes in water. When the carbonization temperature is no more than 240 ο C, the morphologies and structures of Fe-HKUST-1@VSNC are not changed. And the adsorption efficiencies and capacities of Fe-HKUST-1@VSNC-240 for Congo red (CR) and crystal violet (CV) are the optimal. At an initial dye concentration of 10 mg L −1 , a temperature of 35 °C, and pH 7, Fe-HKUST-1@VSNC-240 shows its highest performance, reaching 98.17 % removal of CV in 90 min and 98.65 % removal of CR in 120 min. The adsorption processes of Fe-HKUST-1@VSNC-240 for both CV and CR are slightly affected by coexisting ions. The adsorption efficiency of Fe-HKUST-1@VSNC-240 for CV and CR declines to 50.10 % (after 6 cycles) and 56.76 % (after 22 cycles), respectively. Moreover, Fe-HKUST-1@VSNC-240 also demonstrates good adsorption performance in real water environment. The adsorption processes of Fe-HKUST-1@VSNC-240 for both CV and CR are endothermic, spontaneous, and monolayer adsorption, primarily through chemical adsorption and intra-particle diffusion. The synthesized Fe-HKUST-1@VSNC-240 can adsorb various organic dyes, along with excellent structural stability and recyclability, offering a promising solution for dye-contaminated wastewater remediation.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Mengxue Li,Juanjuan Wang,Nana Zhu,Yang Zong,Rui Jiao,Zhaoqi Zhu,Hanxue Sun,An Li
Fe–N–C catalysts are some of the most promising catalysts for the oxygen reduction reaction (ORR). However, there are still some problems in the pyrolysis of precursors, such as the destruction of the carbon skeleton and low utilization of active sites. In this work, we synthesized hollow pyridine N-containing conjugated microporous polymers (CMPs) by coupling polymerization. The bipyridine units in CMPs’ skeleton can anchor Fe3+ to form a stable coordination structure, which was effectively converted into Fe–N–C catalysts by one-step pyrolysis. Due to the rigid skeleton of precursors, the hollow structure was preserved in catalysts, which is favorable to O2 diffusion and mass transport of intermediates. X-ray photoelectron spectroscopy and Fe K-edge X-ray near-edge spectroscopy revealed approximate FeN4 structures within the framework of the catalysts. As a result, the resulting CMP-derived catalysts exhibited satisfactory ORR activity in alkaline media with a limiting current density of 4.40 mA cm–2. Furthermore, the Fe,N–C1–900 catalyst demonstrated exceptional methanol immunity with a mere negative shift of 0.01 mA cm–2 in limiting current density compared with the commercial Pt/C catalyst, indicating remarkable stability.
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高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 5
·1232-1238
·
IF 2.726
Chen Weijie,Xia Huicong,Guo Kai,Jin Wangzhe,Du Yu,Yan Wenfu,Qu Gan,Zhang Jianan
Lithium-sulfur(Li-S) batteries have been puzzled by the “shuttle effect”. In the recent years, catalytic materials present a huge potential for solving this problem. However, the exploitation for catalytic activity was still challenging in Li-S batteries. In this article, we put forward a single atom catalyst (SAC) of FeN 4 coupled with Fe 3 C on the N-doped carbon (FeN 4 /Fe 3 C@NC) by one-step pyrolysis method. The FeN 4 and Fe 3 C synergistically catalyze the polysulfides conversion when the N-doped carbon provides the high conductive three-dimensional skeleton in Li-S batteries. As a result, the FeN 4 /Fe 3 C@NC shows a specific capacity of 1100 mA·h/g at 0.2 C(1 C=1675 mA/g). In addition, the FeN 4 /Fe 3 C@NC maintains 99.01% of the pristine specific capacity after 100 cycles at 0.5 C, indicating the improved electrochemical performance in Li-S batteries. This work sheds new lights on the design of engineering catalysts for developing high-performance Li-S batteries.
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高影响因子
危险品化学品经营许可证（带存储）