JOURNAL OF POWER SOURCES
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2020
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IF 8.247
Danke Chen,Jiapeng Ji,Zhongqing Jiang,Min Ling,Zhongjie Jiang,Xinsheng Peng
Transition metal-nitrogen-carbon (M/N/C) catalysts, Fe/N/C in particular, with low cost, good tolerance to methanol and promising activity has great potential to replace Pt-based catalysts in oxygen reduction reaction (ORR). However, for metal atoms are easy to migrate and agglomerate during pyrolysis , it still remains a challenge to rationally design precursors to synthesize highly active M/N/C without significant agglomeration of metal sites. In this work, we propose a molecular-confinement strategy to synthesize sub-nano Fe/N/C catalysts by confinement [Fe(CN) 6 ] 3- in zeolitic imidazolate framework-8 (ZIF-8) crystals to minimize the agglomeration of Fe atoms during pyrolysis . The half-wave potential of the prepared sub-nano Fe/N/C is 40 mV superior to that of commercial 20% Pt/C in alkaline medium . Besides, it has electron transfer number close to 4.00, with below 0.5% H 2 O 2 yield, excellent long-term stability with only −5 mV shifts after 10000 cycles, and superb methanol tolerance. When utilized in Zn-air batteries as the cathode, it exhibits better activity, stability, and higher specific capacity than that of Pt–RuO 2 /C, showing a good potential for air cathode.
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Biomaterials Advances
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2025
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IF 6
Yang Guo,Xinyu Gao,Fang He,Sihan Wang,Jingting Li,Fan Yang,Zihan Zhou,Changsong Dai,Zhaohui Wen
When nano-enzymes are used in tumor therapy research, they usually exhibit only a single enzyme activity, which limits their therapeutic effect in hypoxic tumors. This paper designs a hyaluronic acid (HA)-modified Au-Pt-Fe trimetallic flower-like nanomaterial for tumor cascade catalysis integrated with low-temperature photothermal therapy. GOx activity exhibited by AuPt nanoparticles converts glucose in tumor cells into gluconic acid and H 2 O 2 . This process not only deprives tumor cells of their energy source but also produces H 2 O 2 . Iron single-atom nanomaterials can exhibit excellent CAT and POD activities, catalyzing H 2 O 2 reactions in tumor cells. Among them, a portion of H 2 O 2 is converted to O 2 by the activity of nanozyme CAT, which is used to alleviate tumor tissue hypoxia and serve as a substrate for the GOx-like activity reaction of AuPt NPs. The H 2 O 2 is continuously produced by the glucose catalytic reaction, and a portion of it can further decompose into toxic OH through POD activity, contributing to tumor cell destruction. The glucose-H 2 O 2 -O 2 cycle reaction is realized, that is, the self-supply of H 2 O 2 and O 2 in the catalytic process within tumor cells. The introduction of AuPt nanoparticles enhances the photothermal conversion ability of the material. By using near-infrared light irradiation, mild-temperature photothermal therapy (m-PTT) can be achieved, which further improves the treatment effect while protecting surrounding tissues. This work expands the application of multi-metal nanomaterials in cascade catalysis combined with low-temperature photothermal therapy, providing a novel strategy for integrated tumor treatment.
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ANALYTICAL CHEMISTRY
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2021
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IF 6.986
Li-Ping Zong,Junji Li,Guofang Shu,Xinye Liu,Robert S. Marks,Xue-Ji Zhang,Serge Cosnier,Dan Shan
In view of the shortcomings of the current coreactant electrochemiluminescence (ECL) and inspired by natural oxygen (O2) reduction metalloenzymes, a novel ECL amplification strategy was established. A pyrolytic iron- and nitrogen-doped (Fe–N–C) nanosheet rich in singly ionized oxygen vacancy (VO•) defects was rationally designed by destroying the highly saturated coordination with a preorganized ligand 1,10-phenanthroline-2,9-dicarboxylic acid (PDA). Extraordinary catalytic activity for O2 activation was obtained via screening a special pyrolysis temperature using spectroscopic and electrochemical methods. The high-spin ferric centers of highly dispersed FeC nanoclusters and abundant carbon and oxygen vacancy defects fully contributed to the inherent catalytic activity. ECL amplification was achieved by integrating the material with luminol to generate redox-active radicals in situ from dissolved O2 and simultaneously shorten the transferring distance of radicals. Tetracycline (TC), which posed a growing threat to aquatic biodiversity and environmental safety, as a model antibiotic was successfully detected with a detection limit of 3.88 nM (S/N = 3), clarifying a promising application prospect of this new effective ECL amplification strategy in biological analysis and environmental monitoring.
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Jinchang Xu,Yinlong Wu,Tianli He,Ruizhong Chen,Siguo He,Jian Chen,Fangyan Xie,Yanshuo Jin,Ming-Hsien Lee,Nan Wang,Zhenyou Wang,Hui Meng
Dual nitrogen-doping strategies effectively regulate both the activity and durability of Fe-N-C catalysts. • Amino-functionalized precursors generate lower-coordinated Fe N sites, leading to enhanced ORR kinetics. • Ammonia-assisted pyrolysis boosts initial PEMFC performance by modulating spin state and increasing specific surface area. • The catalytic activity and stability of PEMFCs are strongly correlated with the spin state of the Fe active sites, where high-spin configurations offer higher activity but inferior stability. Nitrogen species play a crucial role in regulating the electronic structure of Fe-N-C catalysts, thereby governing the adsorption of oxygenated intermediates and ultimately determining proton exchange membrane fuel cell (PEMFC) performance. However, the intrinsic linkage among nitrogen configuration and catalytic performance remains insufficiently understood. To address this, we design four Fe-N-C catalysts with comparable structures but distinct nitrogen components by using amino-functionalized precursors and controlling the pyrolysis atmosphere. PEMFC testing and characterization show that amino groups in the iron precursor generate lower coordinated Fe-N x site, which density functional theory calculations show to possess more favorable adsorption energetics and reduced free-energy barriers for key reaction intermediates. In contrast, ammonia-assisted pyrolysis enhances initial performance primarily by introducing higher spin-state sites, abundant carbon defects, enlarging surface area, and increasing the density of accessible Fe-N x sites. Importantly, we find that both catalytic activity and durability can be regulated by Fe-N coordination by manipulating spin state of the Fe center: high-spin sites deliver higher intrinsic activity but suffer from accelerated degradation, whereas intermediate/low-spin sites offer improved stability. These findings suggest that a rational combination of precursor functionalization and pyrolysis atmosphere can simultaneously optimize Fe-N x site spin state, coordination environment, and carbon microstructure, providing a practical strategy to achieve both high activity and long-term durability in Fe-N-C catalysts for PEMFCs. Download: Download high-res image (57KB) Download: Download full-size image
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Green Chemical Engineering
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2026
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IF 11.9
Kexin Wei,Haoyang Yu,Fan Yang,Yang Sun,Shijia Li,Jiabao Guo,Yongfeng Li
To advance the development of high-performance rechargeable zinc-air batteries (ZABs) with efficient oxygen electrochemistry, significant progress is needed in research on Fe-based nanoparticle/single-atom bifunctional oxygen electrocatalysts. Nevertheless, the structure-activity relationship and synergy mechanism of Fe-based nnoparticle/single-atom hybrid catalysts are not well-known. Herein, Self-supported carbon nanofiber electrocatalysts with in-situ synthesized FeS, Fe 2 P, or Fe 3 C nanoparticles and atomically dispersed Fe-N x sites were prepared in this work by the coaxial electrospinning method. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) simulations showed that there was a significant change in charge distribution, an increase in the adsorption of *O intermediates, and a decrease in the *OH desorption energy barrier at the FeS/FeSA interface. It can be concluded that FeS/FeSA has better electronic and adsorption properties than Fe 2 P/FeSA and Fe 3 C/FeSA. Therefore, FeS/FeSA has an oxygen reduction reaction (ORR) half-wave potential of 0.89 V and an oxygen evolution reaction (OER) overpotential of 240 mV at 10 mA/cm 2 , which is relatively high compared with that of Fe 2 P/FeSA (0.79 V, 260 mV) and Fe 3 C/FeSA (0.77 V, 250 mV), and it has a small potential gap (Δ E ) of 0.58 V. FeS/FeSA can be used as the air cathode in liquid ZABs; it has a high peak power density of 116 mW/cm 2 and is stable for more than 150 hours. The above results have laid the foundation for the construction of high-performance air cathode catalysts by means of effective coupling of atomic nanoparticles and shown the direction for developing high-efficiency, long-life rechargeable zinc-air batteries.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Wen Song,Xinyu Xiao,Guanlong Wang,Xiaoli Dong,Xiufang Zhang
Supporting Fe catalysts on N doped carbon (Fe-N-C) renders a promising way towards peroxymonosulfate (PMS) activation for water decontamination , but constructing high-efficiency Fe-N-C remains challenging due to the insufficient understanding of the structure-performance relationship. Herein, the N doped carbon nanotube supported Fe catalysts (Fe-NCNT) were prepared towards PMS activation for organic pollutants removal, in which the Fe-N coordination number and Fe species were tuned through changing the pyrolysis temperature to study their roles in PMS activation. Results showed increasing the pyrolysis temperature converted the Fe-N 4 structure in Fe-NCNT to low-coordinated Fe-N 3 structure and produced Fe nanoparticles (FeNP, encapsulated in carbon). The Fe-NCNT with Fe-N 3 and FeNP exhibited a remarkably high specific activity (0.119 L min −1 m −2 ), which was 1.8 times higher than that of Fe-NCNT with only Fe-N 4 and obviously outperformed those of the state-of-the-art PMS activators. The low-coordinated structure and FeNP promoted the PMS reduction on Fe 2+ of Fe-N x for •OH and SO 4 •− production, which served as major oxidants for pollutants degradation . The experimental results and theoretical calculation corroborated the low-coordinated structure and FeNP jointly enhanced the PMS adsorption and electron density on Fe center, which accelerated electron transfer from Fe center to PMS for radical production.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Ting Yang,Shisuo Fan,Yang Li,Qi Zhou
A high-efficient iron-based heterogeneous catalyst is desired to active peroxymonosulfate (PMS). Due to a large catalytic contribution of atomically dispersed Fe-N x sites, single-atom iron–nitrogen-carbon catalysts exhibit superior performance in the catalytic activation of PMS. Herein, a sequence of Fe-N-C SACs with atomically dispersed Fe-N x sites, Fe SA -N-C and Fe SA -N/C, were prepared from Fe-doped ZIF-8 and FePc@ZIF-8, respectively. Single-atom Fe-N x sites were confirmed to be the main active sites for PMS activation. Fe SA -N/C-20 with a higher density of Fe-N x sites exhibited superior catalytic performance to N/C, Fe SA -N-C, Fe SA -N/C-15, and Fe SA -N/C-25 for BPA degradation. Integrated with chemical quenching experiments, electron spin resonance (ESR), in-situ Raman spectra, and electrochemical analysis, a nonradical pathway was demonstrated to dominate the degradation of BPA in the PMS + Fe SA -N/C-20 system. More importantly, the nature of this nonradical pathway was found to be an electron-transfer regime instead of a high-valent iron or singlet oxygenation process. The BPA was adsorbed onto the Fe-N x site by a “donor–acceptor complex” mechanism to form a nonradical PMS* intermediate during the process. Benefiting from this mechanism, the PMS + Fe SA -N/C-20 system showed wide pH adaptation and high resistance to inorganic anions.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Lu Zheng,Yifan Gu,Fengting Li
The rational design of transition metal and nitrogen co-doped carbon-based catalysts for the efficient removal of antibiotics through non-radical pathway of peroxymonosulfate (PMS) activation has attracted widespread attention. Herein, a magnetic hierarchical porous Fe-N-C catalyst (FeBDC-NH 2 -800) was successfully constructed by pyrolyzing the hierarchical porous precursor metal–organic framework gel (FeBDC-NH 2 ) consisting of nitrogen-containing ligands. Benefiting from the defective heterojunction structure, the catalyst exhibited effective and efficient degradation towards amoxicillin (AMX) by activating PMS to produce 1 O 2 . The degradation of AMX was up to 97.4 % within 30 min, which was 2.48 and 2.16 times more than that of FeBDC-NH 2 /PMS and nanosized Fe 3 O 4 /PMS respectively. The high degradation performance could be maintained toward low pollutant concentration conditions and cycle experiments, manifesting its possibility for practical application. Combining the data of quenching experiments, electron spin resonance spectra, electrochemical experiments, X-ray photoelectron spectra and density functional theory calculation, the mechanism was revealed that radical pathway contributed little during degradation while singlet oxygen played a significant role. The cleavage of lattice oxygen and defective heterogeneous structure of FeBDC-NH 2 -800 contributed together to promote PMS for 1 O 2 production.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Wenyu He,Jinhui Wei,Ting Huang,Enren Zhang
For practical applications of microbial fuel cells (MFCs), 5H-dibenz [b,f] azepine-5-carboxamide (Carbamazepine, CBZ) was used as the organic precursor for the synthesis of catalysts composed of Fe–N–C complexes (named as Fe-CBZ-Cats) through a sacrificial support method. Characterizations by SEM, XPS and TEM-EDS elemental mapping show that the synthesized Fe-CBZ-Cats have porous structure and uniformly dispersed Fe/N/C complex centers which could play key roles in effective ORR . Linear scanning voltammetry (LSV) measurements show that the synthesized Fe-CBZ-Cats exhibits ORR activity comparable to commercial Pt/C catalysts under the same catalyst loading (2 mg cm −2 ). The maximum power density produced by cathode-limiting MFCs with Fe-CBZ-Cats air cathodes was 431 ± 23 μW cm −2 , higher than those in the control MFCs with Pt/C air cathodes (403 ± 13 μW cm −2 ) and activated carbon air cathodes (296 ± 24 μW cm −2 ). In addition, the toxicity tolerance of the synthesized Fe-CBZ-Cats is much higher than Pt/C.
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ELECTROCHIMICA ACTA
·
2023
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IF 6.6
Tianfang Yang,Ye Chen,Miao Tian,Xupo Liu,Fengxian Zhang,Jing Zhang,Kun Wang,Shuyan Gao
ABSTRACT Heteroatom doping is considered as an effective approach that manipulates the local bonding environment to improve the electroactivity of Fe-N/C catalysts. Herein, the oxidation polymerization-pyrolysis approach is applied to fabricate the uniformly F-doped porous Fe-N/C catalysts (F-FeNC) through utilizing 4-fluoroaniline as a “self-doping” precursor with N and F elements simultaneously. The synergistic effect between ligand trapping and long-range interaction of F atoms provides high density of Fe-N x active sites. The F-FeNC catalyst demonstrates superior ORR performance in alkaline media with a positive half-wave potential ( E 1/2 ) of 0.82 V, low H 2 O 2 yield of ∼3.4% and rapid 4e − transfer process. The liquid-state Zn-air battery (ZAB) assembled with F-FeNC catalyst as air cathode delivers excellent rate capability, power density (141 mW cm −2 ), specific capacity (760 mAh g − 1 ) and long-term cycle durability over 120 h. Moreover, the as-assembled all-solid-state ZAB shows excellent cycle stability at 0°∼180° bending conditions, revealing great prospects in flexible electronic device applications. Engineering the electronic structure of active sites via F self-doping provides an insightful route for designing multi-heteroatom doped Fe-N/C catalysts.
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ACS Applied Materials & Interfaces
·
2019
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IF 8.456
Yinling Wang,Juan Wang,Dandan Wei,Maoguo Li
M–N–C electrocatalysts for the oxygen reduction reaction (ORR) have been considered as the most promising alternatives to precious metal catalysts. However, the catalytic activity of M–N–C especially in an acidic medium is still unable to meet the practical requirement, and the corresponding ORR mechanism also remains unclear. Herein, an “MOF-protective-pyrolysis” strategy was adopted to synthesize an Fe–N–C catalyst (P-FeMOF@ZIF-8) with Fe–N4 as the predominant Fe species. The P-FeMOF@ZIF-8 displays high catalytic activity in both acidic and alkaline mediums. The experimental results further reveal the different importance of the Fe species in different mediums. Based on the results, a distinct mechanism of the ORR the in acidic medium was proposed, where the synergistic effect of the Fe–N4 site and carbon in improving the kinetics of the ORR were well explained. The findings and the corresponding perspective may provide a new guidance for the design of highly efficient ORR electrocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Cheng Hou,Jiang Zhao,Libin Yang,Jiabin Chen,Xuefen Xia,Xuefei Zhou,Yalei Zhang
A single-atom Fe-N-C catalysts (Fe-N-C) was successfully prepared through a facile synthesis route using microalgae to drive hydrogen peroxide (H 2 O 2 )-based Fenton-like reactions. The detailed characterization analyses confirmed the simultaneous presence of Fe/Fe compounds and Fe-N x coordination sites in the optimal catalyst (Fe-N @ MBC) obtained through the pyrolysis of FeCl 3 ·6 H 2 O and Chlorella vulgaris . Surprisingly, when applied in H 2 O 2 -based advanced oxidation processes (AOPs), Fe-N @ MBC demonstrated excellent proficiency for both H 2 O 2 and O 2 activation, with the contribution of the original dissolved oxygen for sulfamethoxazole removal reaching up to 47.59%. The experiment and density functional theory (DFT) calculation results indicated that the Fe/Fe compounds significantly boosted the activity of Fe-N x by lowering the energy barrier of the reactive oxygen species formation and promoting the electron transfer between Fe-N x and the oxidants (H 2 O 2 and O 2 ). These findings provide new insights into the facile synthesis, rational design, and catalytic mechanisms of Fe-N-C used in H 2 O 2 -based AOPs.
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危险品化学品经营许可证（带存储）