Journal of Environmental Chemical Engineering
·
2025
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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.
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
ChemElectroChem
·
2020
·Vol. 7
·期 7
·1775-1780
·
IF 4.154
Xinyue Zhang,Qingtao Liu,Jianglan Shui
Graphical Balancing act : Polytetrafluoroethylene (PTFE) is added to different positions of the Fe−N−C catalyst layer by using three methods to adjust its hydrophobicity. An appropriate amount of PTFE in the Fe−N−C catalyst layer is beneficial to the power density of the PEM fuel cell. However, the hydrophobicity of the Fe−N−C catalyst layer does not affect the long-term durability of the fuel cells, although high hydrophobicity will improve the fuel cell initial durability. The hydrophobicity of the cathode catalyst layer (CCL) affects the performance of the proton exchange membrane fuel cell (PEMFC) by adjusting the water management of the catalyst layer, which has been extensively studied in Pt-based catalysts. Here, the effect of the hydrophobicity of Fe−N−C CCL on the performance of the PEMFC is investigated. The hydrophobicity of the Fe−N−C CCL is tuned by polytetrafluoroethylene (PTFE) by using three addition methods: 1) coat PTFE on Fe−N−C powder and heat-treat; 2) mix PTFE emulsion with Fe−N−C ink and then brush the electrode; and 3) transfer a ground PTFE/Fe−N−C composite film onto the gas diffusion layer by the decal method. For each PTFE addition method, the optimized PTFE amount can increase the power density of Fe−C−N PEMFC by 15.1 %, 26.6 %, and 87.2 %, respectively. At the same time, it is found that enhanced hydrophobicity reduces the initial current decay rate of the Fe−N−C CCLs, but their residual current densities are close after a 50 h durability test at 0.5 V in a H 2 -O 2 PEMFC. It can be concluded that the hydrophobicity of the Fe−N−C CLL has a great influence on the power density of the fuel cell, but the influence on the long-term durability of the fuel cell is negligible.
研究领域:
能源科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Meng Cheng,Junhao Liu,Hao Jiang,Chunling Li,Shuangqing Sun,Songqing Hu
In view of the critical importance of oxygen to corrosion evolution, to starve corrosion via depleting oxygen in coatings is a promising strategy. In this work, a novel nanocatalytic anticorrosion concept is proposed to design new coating with outstanding corrosion resistance . Different from the passive barrier of traditional coatings and self-repair after corrosion of current stimuli-feedback coatings, such coating could spontaneously eliminate internal diffused oxygen and greatly suppress the corrosion process. As a proof of concept, single-atom Fe-N-C electrocatalyst with isolated FeN 4 active sites is synthesized by a simple confined carbonization method, exhibiting excellent oxygen reduction performance (E 1/2 = 0.902 V). In composite coating , the evenly dispersed Fe-N-C compensates for the coating defects and serves as oxygen scavengers, which could actively adsorb and consume ambient oxygen, thereby preventing oxygen penetration to the metal substrate surface, eliminating the oxygen contribution to corrosion and significantly boosting the anticorrosion performance of epoxy coating. This in-situ mediation for oxygen in coating prevents metal substrate from receiving new supply of oxygen, while imparting active anticorrosion property to the coating.
研究领域:
材料科学
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腐蚀科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2023
·Vol. 15
·期 39
·16188-16198
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IF 6.7
Qingxue Lai,Hongmei Zheng,Wanying Zhang,Yi Sheng,Luanjie Nie,Jing Zheng
Fe–N–C catalysts with highly dispersed metal active centers were developed as promising non-precious metal materials for acidic oxygen reduction reaction (ORR) electrocatalysis. However, such kind of novel catalysts still suffer from major challenges in the manipulation of dispersion, utilization, and stability of the Fe-based metal centers. Herein, a N-rich molecular dual-guided pyrolysis strategy was proposed to develop an efficient yolk-shelled Fe–N–C ORR electrocatalyst. A unique yolk-shelled nanostructure with a relatively ordered shell and disordered yolk of a carbon skeleton was controllably constructed via this guided-pyrolysis route from the precursor of Fe-doped zeolitic imidazolate framework-8 (Fe-ZIF-8). Moreover, the atomic-level dispersion of Fe element in the carbon skeleton could be achieved via the dual guidance from phenanthroline and melamine molecules. The optimized Fe–N–C catalyst demonstrated a half-wave potential of 0.78 V vs. RHE in acid media, close to commercial 30% Pt/C, along with a small negative shift of 19 mV after an accelerated durability test. These enhanced electrocatalytic properties could be attributed to the preferred transformation of the Fe precursors to atomically dispersed Fe–Nx active configurations, as well as the enhanced three-phased interfacial reaction kinetics.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
MOLECULES
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2023
·Vol. 28
·期 7
·2879
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IF 4.6
Sensen Li,Yan Lv,Sawida Elam,Xiuli Zhang,Zhuojun Yang,Xueyan Wu,Jixi Guo
The rational design of morphology and structure for oxygen reduction reaction (ORR) catalysts still remains a critical challenge. Herein, we successfully construct defect-rich and hierarchically porous Fe-N-C nanosheets (Fe-N-CNSs), by taking advantage of metal-organic complexation and a mesoporous template. Benefiting from the advantages of high density of active sites, fast mass transfer channels, and sufficient reaction area, the optimal Fe-N-CNSs demonstrate satisfactory ORR activity with an excellent half-wave potential of up to 0.87 V, desirable durability, and robust methanol tolerance. Noteworthy, the Fe-N-CNSs based zinc–air battery shows significant performance with a peak power density of 128.20 mW cm−2and open circuit voltage of 1.53 V, which reveals that the Fe-N-CNSs catalysts present promising practical application prospects. Therefore, we believe that this research will provide guidance for the optimization of Fe-N-C materials.Keywords:electrocatalytic;Fe-N-C materials;oxygen reduction reaction;two-dimensional materials
研究领域:
材料科学
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能源化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Feng-Di Tu,Zi-Yun Wu,Pan Guo,Li-Xiao Shen,Zi-Yu Zhang,Yun-Kun Dai,Miao Ma,Jing Liu,Bin Xu,Yun-Long Zhang,Lei Zhao,Zhen-Bo Wang
Platinum group metal (PGM)-free catalysts represented by nitrogen and iron co-doped carbon (Fe-N-C) catalysts are desirable and critical for metal-air batteries , but challenges still exist in performance and stability. Here, cerium oxides (CeO x ) are incorporated into a two-dimensional Fe-N-C catalyst (FeNC-Ce-950) via a host-guest strategy. The Ce 4+ /Ce 3+ redox system creates a large number of oxygen vacancies for rapid O 2 adsorption to accelerate the kinetics of oxygen reduction reaction (ORR). Consequently, the as-synthesized FeNC-Ce-950 catalyst exhibits a half-wave potential ( E 1/2 ) of 0.921 V and negligible decay (<2 mV for Δ E 1/2 ) after 5,000 accelerated durability cycles, significantly outperforming most of ORR catalysts reported in recent years and precious metal counterparts. When applied in a zinc-air battery, it demonstrates a peak power density of 175 mW cm −2 and a specific capacity of 757 mAh g Zn −1 . This study also provides a reference for the exploration of Fe-N-C catalysts decorated with variable valence metal oxides .
研究领域:
材料科学
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电化学
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能源存储与转换
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产品关联
DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
·
2021
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IF 6.558
Liping Sun,Chao Li,Yong Yan,Yue Yu,Hao Zhao,Zijue Zhou,Feng Wang,Yi Feng
Single atom nanozymes (SAzymes) represent the state-of-the-art technology in nanomaterial-based catalysis, which have attracted attentions in catalysis, cancer treatment, disinfection and biosensing fields. However, numerous SAzymes suffered from low aqueous dispersion and without recognition capacity, which impeded their applications in bioanalysis . Herein, we engineered DNA onto SAzymes to obtain the DNA/SAzymes conjugates , which significantly improved the aqueous dispersion and recognition ability of SAzymes. We synthesized iron SAzymes (Fe–N–C SAzymes) as the catalytic nanomaterials, and investigated the interactions between Fe–N–C SAzymes and DNA. We compared A 15 , T 15 and C 15 adsorption of Fe–N–C SAzymes in HEPES containing 2 mM MgCl 2 . We found that 50 μg mL −1 Fe–N–C SAzymes produced nearly 100% A 15 adsorption, 90% T 15 adsorption and only 69% C 15 adsorption, indicating that adenine and thymine had higher adsorption affinity on Fe–N–C SAzymes. More importantly, DNA modification did not affect the peroxidase-like activity of Fe–N–C SAzymes and the bioactivity of the adsorbed DNA. Taking the advantage of the diblock DNA with one DNA sequence (adenine) binding to Fe–N–C SAzymes and the other DNA sequence (i.e., aptamer) binding to cancer cells, we designed Apt/Fe–N–C SAzymes for colorimetric detection of cancer cells, which offered new insights for the use of SAzymes in biomedicine .
研究领域:
生物医学
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纳米技术
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催化科学
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DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
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2019
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IF 6.35
Lei Jiao,Weiqing Xu,Hongye Yan,Yu Wu,Chunrong Liu,Dan Du,Yuehe Lin,Chengzhou Zhu
Recently, in situ detection of hydrogen peroxide (H2O2) generated from live cells have caused tremendous attention, because it is of great significance in the control of multiple biological processes. Herein, Fe–N–C single-atom nanozymes (Fe–N–C SAzymes) with intrinsic peroxidase-like activity were successfully prepared via high-temperature calcination using FeCl2, glucose, and dicyandiamide as precursors. The Fe–N–C SAzymes with FeNx as active sites were similar to natural metalloproteases, which can specifically enhance the peroxidase-like activity rather than oxidase-like activity. Accordingly, owing to the excellent catalytic efficiency of the Fe–N–C SAzymes, colorimetric biosensing of H2O2 in vitro was performed via a typical 3,3′,5,5′-tetramethylbenzidine induced an allochroic reaction, demonstrating the satisfactory specificity and sensitivity. With regard to the practical application, in situ detection of H2O2 generated from the Hela cells by the Fe–N–C SAzymes was also performed, which can expand the applications of the newborn SAzymes.
研究领域:
生物化学
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纳米医学
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分析化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2022
·Vol. 169
·期 5
·053505
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IF 4.386
Yanfang Song,Jinxiong Wu,Jiliang Zheng,Yiwei Sun,Andrei Ivanets,Guangming Du,Xintai Su
The doping of multiple heteroatoms can improve the electrochemical properties of carbon substrates. However, in existing studies, carbon, iron and nitrogen sources are generally mixed directly and then pyrolyzed for secondary activation. This tends to form aggregates of metal particles or metal oxides and requires the consumption of large amounts of alkali and energy. Therefore, there is an urgent need to develop an environmentally friendly technology capable of uniformly doping iron and nitrogen into carbon materials. In this work, porous Fe–N–C composites were prepared at 600 °C using potassium humate (HA-K) obtained from cotton straw by low-temperature pyrolysis as the carbon source, and urea-iron complexes formed by the pre-coordination of urea and Fe as the iron and nitrogen sources. In the absence of secondary activation, the best sample Fe-NHPC-2 had a good mesoporous structure with high specific surface area (889. 01 m2 g−1). It had a high specific capacitance of 256.8 F g−1 at a current density of 0.5 A g−1. The capacitance retention was 92.6% after 10,000 cycles at a current density of 10 A g−1. In the symmetric supercapacitor application, the energy density reached 33.16 Wh kg−1 when the power density was 600.2 W kg−1.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 23
·5557-5564
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IF 5.6
Yi Sheng,Hongmei Zheng,Jingting Hou,Wanying Zhang,Hong Chen,Luanjie Nie,Jing Zheng,Qingxue Lai
Fe–N–C materials as popular non-Pt group metal (non-PGM) electrocatalysts demonstrated huge potential for replacing Pt-based materials for efficient oxygen reduction reaction (ORR) electrocatalysis in acidic media. Herein, a metal–organic-framework (MOF)-based dual ligand strategy is proposed to develop advanced Fe–N–C materials with a controllable density of Fe-Nx sites and electrochemically active surface area, attributed to the synergistic effect from secondary ligand manipulation and Zn evaporation during pyrolysis. As a result, the optimized catalyst exhibits an ORR half-wave potential of 0.747 V vs. RHE and long-term stability with only a 29 mV negative shift after 3000 potential cycles in 0.5 M H2SO4 electrolyte. More far-reaching, this MOF-based dual ligand strategy opens a novel avenue to the precise fabrication of efficient catalysts.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Hong Yu,Chen Wang,Xinhe Xiong,Bitao Dai,Yang Wang,Zhijie Feng,Hao luo,Jiangxiong Zhu,Guoqing Shen,Yun Deng,Xueqing Geng,Danfeng Wang,Lumei Wang
Acetamiprid (Ace), extensively employed in agricultural production as a substitute for organophosphorus pesticides, poses a potential threat to the environment and human health due to excessive residues. Hence, the development of reliable and convenient techniques to determine Ace levels in the environment holds significant importance. Among various assay methods, nanomaterial-based aptamer-based biosensors (aptasensors) have emerged as efficient and promising tools. In this study, we successfully developed a novel aptasensor for monitoring Ace in the environmental water, utilizing advanced nanomaterials known as Fe-N-C single-atom nanozymes (SAzymes). Fe-N-C SAzymes exhibited excellent catalytic activity, high stability, and complete atom utilization. A facile dual-confinement route was employed for the synthesis of Fe-N-C SAzymes, and their performance as oxidase-like nanozymes was investigated. The synthesized Fe-N-C SAzymes presented distinct oxidase-like activity and demonstrated the capability to interact with a chromogenic indicator-TMB, serving as the signal transduction element in our assay. Furthermore, we found that thiol-modified aptamers could effectively dampen the oxidase-like activity of Fe-N-C SAzymes.Therefore, we successfully developed a Fe-N-C SAzymes assisted detection method for Ace, which exhibited high sensitivity (LOD = 16.9 nM) and selectivity. Overall, this work provides new insights into the design of multifunctional Fe-N-C SAzymes for environmental and biological applications.
研究领域:
环境科学
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生物技术
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纳米材料科学
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产品关联
DOI
高影响因子
ANALYST
·
2020
·Vol. 146
·期 3
·896-903
·
IF 3.978
Xiaolei Xie,Yufei Wang,Xiaobin Zhou,Junyang Chen,Mengke Wang,Xingguang Su
Single-atom nanozymes have drawn wide attention in bio-sensing for their remarkable merits such as low cost, high stability, and maximum atom utilization. Herein, a colorimetric strategy based on Fe–N–C single-atom nanozymes (Fe/NC-SAs) was established for the detection of alkaline phosphatase (ALP) activity. The Fe/NC-SAs prepared by pyrolysis have excellent peroxidase-like activity and can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to a blue color product in the presence of hydrogen peroxide (H2O2). When ascorbic acid (AA) is added to the system, the blue color fades, and the absorbance has a linear relationship with the concentration of AA. Alkaline phosphatase (ALP) can catalyze the hydrolysis of ascorbic acid 2-phosphate (AAP) to produce AA. Thus, a strategy based on Fe/NC-SAs for the detection of ALP activity was established, which provided a linear range of 0.1–1.5 U L−1 and a limit of detection as low as 0.05 U L−1. Besides, Fe/NC-SAs showed high stability under harsh conditions. Moreover, an Fe/NC-SA-based assay was successfully validated using human serum samples for ALP determination with satisfactory results, and has broad prospects in the field of biosensing.
研究领域:
生物传感
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医学检测
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纳米材料
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）