JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Shunlin Li,Hui Wang,Congcong Qiu,Jianan Ren,Yiyin Peng,Yang Liu,Fangyuan Dong,Zhaoyong Bian
An efficient cathode for a Fenton-like reaction based on hydrogen peroxide (H 2 O 2 ) has significant implications for the potential application of the advanced oxidation process. However, the low H 2 O 2 selectivity and efficient activation remain challenging in wastewater treatment. In the present study, a single Fe atom doped, nitrogen-coordinated molybdenum disulfide (Fe 1 /N/MoS 2 ) cathode that exhibited asymmetric wettability and self-absorption molecular oxygen was successfully prepared for pollutant degradation. The X-ray absorption near-edge structure and extended X-ray absorption fine structure of Fe 1 N 3 in the Fe 1 /N/MoS 2 catalyst were determined. The electronic structure demonstrated favorable H 2 O 2 selectivity (75%) in a neutral solution and the cumulative hydroxyl radical concentration was 14 times higher than the pure carbon felt. After 10 consecutive reaction experiments, the removal ratio of paracetamol still reached 97%, and the catalytic performance did not decrease significantly. This work deeply understands the catalytic mechanism of Fenton-like reaction between single Fe atom and MoS 2 double reaction sites, and proves that the regulation of the electronic structure of Fe single atom is an effective strategy to improve the activity of Fenton-like reaction.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Wei Zhang,Wei Wu,Fei Guo,Xinwei Dong
The control of morphology, structure and composition of metal–organic frameworks derived metal-nitrogen doped porous carbon (M–N–C) with high precision and accuracy is essential for the catalytic performance. While single-atom or small-sized nanometer catalysts show notable effects in catalysis, one catalyst combining the advantages of single-atom and nanometer catalysts may cultivate more benefits. Herein, we designed and successfully fabricated a series of Fe-doped ZIF–x with different morphologies (cube→truncated hexahedron→truncated octahedron) in one pot by simply adjusting the adding amount of vitamin C. After high-temperature calcination, Fe 3 C integrated with Fe single-atom planted in N -doped carbon (Fe SA /Fe NC –N–C–x) with various morphology, structure and composition could be acquired. Among them, Fe SA /Fe NC –N–C–0.75 exhibited the best catalytic performance for the transfer hydrogenation of halogenated nitrobenzenes with N 2 H 4 ·H 2 O under room temperature. Acid-leaching tests, poisoning experiments, and the density functional theory calculations showed that Fe 3 C integrated with Fe single-atom had a better catalytic effect than the separated Fe 3 C or Fe single-atom.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2024
·
IF 15.8
Qin Li,Jing Zhao,Peng Li,Zhengrong Xu,Jie Feng,Bo Chen,Rui Liu
Promotion of oxygen reduction reaction (ORR) kinetics, to a large extent, depends on the rational modulation of the electronic structure and mass diffusion of electrocatalysts. Herein, a ferrocene (Fc)–assisted strategy is developed to prepare Fc-trapped ZnMo–hybrid zeolitic imidazolate framework (Fc@ZnMo-HZIF-50) and the derived Fe single atom coupling with MoC nanoparticles, coembedded in hierarchically porous N-doped carbon cubes (MoC@FeNC-50). The introduced Fc is utilized not only as an iron source for single atoms but also as a morphology regulator for generating a hierarchically porous structure. The redistribution of electrons between Fe single atoms and MoC nanoparticles effectively promotes the adsorption of O2 and the formation of *OOH intermediates during the ORR process. Along with a 3D hierarchically porous architecture for enhanced mass transport, the as-fabricated MoC@FeNC-50 presents excellent activity (E1/2 = 0.83 V) and durability (only 9.5% decay in current after 40000 s). This work could inspire valuable insights into the construction of efficient electrocatalysts through electron configuration and kinetics engineering.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Shaorong An,Lina Wang,Qiang Jin
The Fe-N-C catalysts featuring abundant FeNx sites activating peroxymonosulfate (PMS) have been considered an attractive approach to water treatment and purification. It was reported that the coordination numbers of FeNx could be precisely controlled by varying the pyrolysis temperature, thereby affecting the catalytic activity . However, almost all Fe-N-C catalysts were prepared through energy-consuming high-temperature pyrolysis strategies, the activation performance and mechanism under low-temperature pyrolysis conditions are still unclear. In this work, three single-atom Fe catalysts (Fe SA -NC-300/500/1000) based on ZIF-8 were synthesized at different pyrolysis temperatures. Results showed that the degradation efficiency of sulfamethoxazole (SMX) in the Fe SA -NC-500/PMS and Fe SA -NC-1000/PMS systems could reach 100 % within 30 min, while only 91.9 % in the Fe SA -NC-300/PMS system. Combined with the turnover frequency (TOF) of the catalysts, it was found that the catalytic activity of Fe SA -NC-500 prepared by low-temperature pyrolysis was close to that of Fe SA -NC-1000, which was superior to many reported Fenton-like catalysts. Mechanism analysis manifested that both radical (·OH, SO 4 − ·, and ·O 2 − ) and nonradical ( 1 O 2 , high-valent Fe-oxo species, and electron transfer) pathways coexisted in the Fe SA -NC/PMS systems. Impressively, the larger production intensity of reactive species occurred in Fe SA -NC-500/PMS and Fe SA -NC-1000/PMS systems. The difference between these Fe SA -NC catalysts in actual printing and dyeing wastewater treatment offered some guidance for wider environmental applications. This work also provided a direction on the design and understanding of green and energy-saving Fe-N-C catalysts.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Tenglong Jin,Wenmiao Chen,Hongyan Zhuo,Wenjuan Li,Zhen Fu,Linlin Feng,Yanli Chen
The development of efficient and facile nonprecious metal catalysts for the oxygen reduction reaction (ORR) holds great significance. Among these, the single-atomic metal–nitrogen–carbon (M–N–C) catalysts are emerging candidates due to their high activity and prolonged lifespan. However, traditional preparation of M–N–C catalysts suffers from thermal aggregation and low space–time yield, limiting their application in industry. Inspired by the “chainmail protection” in carbonaceous materials, here we propose an “armor protection” strategy for the large-scale synthesis of a highly active Fe single-atom ORR catalyst (Fe-8/8-CN) by pyrolyzing a well-designed precursor Fe-ZIF-8/ZIF-8. In this precursor, the 2-methylimidazole zinc MOF (ZIF-8) loaded with iron (Fe-ZIF-8) is encased in an additional ZIF-8 armor layer (Fe-ZIF-8/ZIF-8) that effectively shields the aggregation of Fe species within the inner ZIF-8 during the pyrolysis process, ultimately yielding the Fe single-atom ORR catalyst (Fe-8/8-CN). Furthermore, the facile approaches for the construction of Fe-ZIF-8/ZIF-8 make it efficiently scale up with a high space–time yield of 18.7 kg m–3 day–1. In particular, the armor protection strategy for preparing the Fe single-atom catalyst is universally applicable to leaf-shaped ZIF-L and other ZIFs with diverse morphologies. Thanks to the presence of the outer ZIF-8 layer and the inner ZIF-8 core to dispersing Fe single-atom catalytic sites with the porous and defect-rich characteristics from the volatilization of Zn in ZIF-8, the resulting Fe-8/8-CN demonstrates superior ORR performance in alkaline electrolyte (E1/2 = 0.93 V, JL = −5.89 mA cm–2). Finally, Fe-8/8-CN, as the cathode material for flexible zinc–air batteries, exhibits a high peak power density (97 mW cm–2) and excellent durability superior to Pt/C.
研究领域:
材料科学
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电化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2022
·
IF 4.177
Weifeng Su,Ning Yan,Fan Liu,Zigeng Liu,Guangqi Zhu,Songrui Wang,Xingjiang Liu,Wei Wang
The attenuation process of the oxygen reduction reaction (ORR) catalytic performance for Fe SAC@G catalysts under different discharging conditions, including KOH concentrations, solution temperatures, and discharging potentials, was investigated by electrochemical measurements. The ORR catalytic activity attenuation resulting from the change in KOH concentration and temperature becomes apparent in a negative discharging potential range and elevated discharging temperature. In addition, the more negative discharging potential significantly causes the ORR catalytic activity attenuation. Scanning electron microscopy (SEM), energy-dispersive spectrometry (EDS), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy analyses indicate that, with the prolongation of the discharge time, the nanocolumns of the as-prepared catalyst gradually dissolve, while a flowerlike discharge byproduct composed of elements C and N keeps growing on the surface of the catalyst. The weakest Fe–N bonds first break, resulting in the attenuation of the ORR catalytical performance. Then, the weak C–Cunit bonds connecting the structural units of the catalysts break, leading to the gradual collapse in the structure of the catalysts. The Fe–N4 coordination structure gradually transforms into Fe–N3, Fe–N2, and Fe–N coordination structures. Based on the analyses combined with the density functional theory (DFT) calculations of bond strength, a discharge attenuation mechanism of the structural collapse of the catalyst for the formation of the discharge byproduct with ring structure is proposed.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Qinqin Yu,Youzhi Dai,Zhu Zhang,Bo Feng
A novel photo-Fenton coupling system was constructed in this paper to address the problems of low visible light utilization, narrow pH applicability range and difficult separation and recovery of common photo-Fenton. Fe single-atom material with high activity was used as a bridge connecting photocatalysis and Fenton oxidation, and the performance and mechanism of the coupling system were investigated using a typical antibiotic ciprofloxacin (CIP) as the target pollutant. It was found that the degradation performance of the photo-Fenton coupling system is significantly improved, and can be maintained in acidic, neutral and alkaline wastewaters; the main active species of the coupling system are ·O 2 – , 1 O 2 and h + , and the enhancement mechanism is a combination of Fe single atoms, S-scheme heterojunction and multiple active species.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Chen Yuanxing,Qin Ying,Liu Mingwang,Yang Wenhong,Qiu Yiwei,Li Wen,Zheng Lirong,Gu Wenling,Zhu Chengzhou,Hu Liuyong
Energy level mismatches between semiconductors and cocatalysts often induce carrier recombination, limiting photocatalytic and photoelectrochemical (PEC) efficiency. Here, we integrate Pt nanocluster-Fe single-atom pairs with CuO to regulate both solid-solid and solid-liquid interfaces in PEC systems. Experimental and theoretical analyses reveal that an Ohmic contact at the CuO/Pt interface accelerates electron extraction, while Pt-to-Fe charge transfer enhances oxygen reduction at Fe sites, collectively boosting reaction kinetics. Leveraging this, we construct a PEC biosensor exploiting chelating effect of glyphosate on CuO to impede electron transfer, achieving a detection limit of 0.41 ng/mL. This interface engineering strategy advances cocatalyst design for enhanced energy conversion and sensing applications by simultaneously addressing carrier dynamics and interfacial reaction barriers.
研究领域:
材料科学
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光催化
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生物传感
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2025
·
IF 9.8
Shu Yang,Yijun Ren,Ganbing Zhang,Hui Xu
Single-atom nanozymes (SAzymes) exhibit superior catalytic activity, making it a promising candidate for constructing biosensors. Herein, we constructed a hollow carbon nanocages supported, N and O double-coordinated Fe SAzymes (HCNs@Fe SAs) through a template and pyrolysis strategy. Abundant oxygen atoms in pre-modified template SiO 2 @resorcinol-formaldehyde provided enough binding sites and promoted the dispersion and stabilization of metal atoms. Compared with non-O modified nanozymes, HCNs@Fe SAs exhibited an 8-fold enhancement in catalytic efficiency. Benefiting from its exceptional peroxide-like activity, a straightforward and dependable colorimetric sensing platform was developed to assess the activity of Acetylcholinesterase and its inhibitor organophosphorus pesticide (OP) in real water samples and fruit substrates, with the limit of detection of 0.02318 mU mL −1 and 0.85 ng mL −1 , respectively. An OPs test paper was also designed for point-of-care determination of OP with satisfactory sensitivity. This study provides a new strategy of template pre-modification to design SAzymes with enhanced catalytic efficiency.
研究领域:
生物传感
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催化材料
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环境检测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
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.
研究领域:
催化
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材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Diejing Feng,Bingxu Lu,Wenjing Wu,Shenggang Yang,Yukun Sun,Bo Bai,Shijie Li
The regulation of heterogeneous material properties to strengthen the peroxymonosulfate activation to destroy refractory pharmaceuticals remains a challenge. Herein, a promising nitrogen-deficient catalyst (FeCN) with single atom Fe and Fe 2 O 3 nanoparticles dispersing on g -C 3 N 4 matrix was synthesized and applied as a competent peroxydisulfate (PDS) activator for tetracycline (TC) degradation under visible light. The K-edge X-ray absorption fine structures and 57 Fe Mössbauer measurements confirmed the unique configuration of Fe 2 O 3 and single atom Fe active sites (pyrrolic and pyridinic FeN 4 ) induced by the neighbouring nitrogen vacancies. The theory calculations and experiments provided a deep insight into the PDS activation and TC degradation via radical and non-radical pathways. The pyrrolic FeN 4 active sites dominated the electron transfer, while the pyridinic FeN 4 and Fe 2 O 3 decomposed PDS to produce free radicals. The synergistic effect between the Fenton-like oxidation and photocatalysis is responsible for efficient TC degradation. This study offers a new strategy by integrating novel catalysts and advanced oxidation technology for effective wastewater purification.
研究领域:
环境科学
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材料科学
·
污染控制
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2023
·Vol. 10
·期 5
·1284-1296
·
IF 7.3
Yuxuan Lin,Weihua Qin,Yuwei Lu,Mingye Ren,Pan Gao,Feng Xiao,Shaoxia Yang
Improving the performance of single-atom catalysts (SACs) is still challenging in Fenton-like reactions for degrading refractory organic pollutants. Here, we designed P and N co-doped Fe SACs to regulate the electronic structure of Fe active sites and enhance the reaction kinetics of peroxymonosulfate (PMS) activation. The obtained heteroatom-doped Fe SACs for the first time exhibited an ultra-low activation energy (ca. 3.7 kJ mol−1) and excellent degradation efficiency for bisphenol A (BPA) in a wide pH range (4.3–9.2). The superior reaction kinetics of the Fe SACs were attributed to enriching the electron density of atomic Fe and then forming dual electron-rich/-deficient sites, which accelerated the electron transformation to generate reactive oxygen species (ROS). In this study the heteroatom-doped Fe SACs with rapid reaction kinetics are achieved, and provides an idea to design SACs with superior performance in heterogeneous Fenton-like reactions.
研究领域:
环境科学
·
催化
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）