JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.3
Geng Zhang,Bolong Jiang,Decheng Lu,Xueqin Wang,Yuanyuan Wang,Hua Song
The sluggish kinetics of the oxygen reduction reaction (ORR) at the cathode severely limits the electricity generation and pollutant degradation of microbial fuel cells (MFCs). Herein, we report a facile one-pot pyrolysis strategy for fabricating a highly dispersed iron-embedded N/S co-doped hierarchical porous carbon catalyst (FeSNC) with accessible Fe−N 4 −S active sites using tetramethylammonium hydroxide (TMAH)-optimized Fe-ZIF-8-N-H precursors. TMAH enables rapid synthesis (16 min), 3.6-fold yield enhancement, mesopore engineering for efficient Fe 2+ capture and dense Fe−N 4 −S site formation, and hierarchical pore construction for accelerated mass/electron transport. The Fe source (NH 4 ) 2 Fe(SO 4 ) 2 ·6 H₂O synchronously introduces N and S to optimize pyridinic N and Fe−N x coordination. Theoretical calculations reveal that S-doping modulates the electronic structure of the central Fe, while mesopore-induced defects act as a secondary modulator, collectively establishing a dual-modulation mechanism to optimize the adsorption/desorption of ORR intermediates. The 6 %FeSNC-N-H catalyst outperforms commercial Pt/C in ORR across neutral/alkaline/acidic media and, as an MFC cathode, delivers a peak power density of 987.0 ± 5.3 mW cm⁻², 96.75 % COD removal, and high degradation efficiency for phenol (93.4 %) and methylene blue (95.6 %). This work underscores the critical synergy between of metal centers electronic microenvironment and nanostructural pore engineering for advanced electrocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Shu-Hu Yin,Xiao-Yang Cheng,Yu Han,Ting Zhu,Zhong-Wei Yu,Rui Huang,Jun Xu,Yan-Xia Jiang,Shi-Gang Sun
Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions (ORR), yet their moderate intrinsic activity and susceptibility to reactive oxygen species (ROS)-induced degradation hinder practical implementation. Herein, we fabricate a Ru-Fe dual-site catalyst (RuFe-N-C) through a two-step pyrolysis strategy. Structural characterization reveals atomic-scale proximity between Ru single atoms and Fe-N 4 moieties, exhibiting a projected distance of ~1.7 Å. This configuration induces Fe–N bond elongation accompanied by 2.5% lattice distortion. The optimized RuFe-N-C catalyst exhibits high ORR performance, with a half-wave potential ( E 1/2 ) of 0.840 V and peak power density ( P max ) of 938 mW cm –2 under 150 kPa absolute H 2 -O 2 . These metrics signify substantial enhancements relative to conventional Fe-N-C benchmarks (+21 mV in E 1/2 and +42% in P max ). Moreover, the catalyst maintains outstanding stability, showing merely 17 mV E 1/2 decay after 10000 accelerated durability test (ADT) cycles. Experimental analyses reveal a bifunctional mechanism: (1) Adjacent Ru sites substantially enhance the intrinsic ORR activity of Fe-N 4 moieties, delivering a notable turnover frequency (TOF = 17.86 e site –1 s –1 at 0.85 V vs. RHE) that exceeds state-of-the-art Fe-N-C benchmarks by 1–2 orders of magnitude (< 1 e site –1 s –1 ); (2) Ru centers function as electron relays that facilitate ROS scavenging, thus suppressing degradation. This work establishes a paradigm for engineering bimetallic single-atom catalysts through synergistic electronic modulation to concurrently enhance activity and stability.
研究领域:
催化化学
·
材料科学
·
电化学
·
能源材料
·
表面科学
·
纳米催化
·
质子交换膜燃料电池
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2026
·
IF 9.2
Fancang Meng,Huan Wu,Boyu Jia,Kexiang Li,Zhihua Wang,He Zhu,Chao Chen,Qingmin Ji
The development of Fe-N-C electrocatalysts for the oxygen reduction reaction (ORR) is crucial for sustainable energy technologies, yet achieving a high density of atomically dispersed Fe-Nx sites remains a challenge. Herein, we proposed a novel spatial confinement strategy based on the molecular-level infiltration of iron-coordinated, water-soluble fullerene (Fe/wsC60) into self-assembled fullerene microbelts (FMB). The -NH2/-OH functionalized C60s act as molecular metal chelator and nitrogen source, while the flexible FMB framework facilitates their effective permeation. This nanoscale confinement effectively mitigates Fe aggregation during pyrolysis, yielding a catalyst with abundant atomically dispersed curved Fe-N4 sites alongside fine Fe3C nanoparticles. The resultant (Fe/N@FMB) catalyst demonstrates an exceptional ORR activity and stability in alkaline media with a half-wave potential of 0.891 V, surpassing Pt/C and control samples derived solely from wsC60 or FMB. When integrated into a zinc-air battery, it also achieves a higher open-circuit voltage and power density than Pt/C. Theoretical calculations reveal that the curved carbon matrix and adjacent Fe3C synergistically modulate the electronic structure of the Fe-N4 moiety, thereby boosting the ORR kinetics. This work highlights the importance of nanoscale architectural design for precise precursor confinement in developing advanced electrocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Junhui Wang,Shimin Yin,Qinhua Zhang,Fengliang Cao,Yicheng Xing,Qingshan Zhao,Yang Wang,Wengang Xu,Wenting Wu,Mingbo Wu
Polymeric carbon nitride materials show intriguing prospects in numerous light-to-energy conversion applications, but seldom studies focus on their triplet energy transfer, leading to the insufficient lifetime for the photochemical process. Inspired by the porphyrin molecular photocatalyst, single-atom sites (Fe-N 4 ) as triplet sensitizing sites were fabricated in g-C 3 N 4 for the preparation of Fe-g-C 3 N 4 , which processes a long-lived triplet emissive state (τ PH = 4.93 μs). But under realistic condition for the large-scale production of catalyst, single atoms are inevitable to sinter, resulting in the formation of other metal species. Therefore, the photooxidation of 1,5-dihydroxynaphthalene (1,5-DHN) and the photocatalytic E-Z Isomerization of stilbene were selected as the model reactions to evaluate the influence of various Fe species on the triplet energy transfer. It was found that Fe-N 4 sites promote the triplet energy transfer process, while Fe nanoclusters (Fe 0 ) promote the electron transfer and inhibit triplet energy transfer. This finding provides guidance for the rational design of photocatalysts to efficiently improve triplet energy transfer process and its application.
研究领域:
材料科学
·
光化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Tianping Wang,Yining Liang,Jingle Wang,Xikui Liu,De Ning,Zhengjian Chen
Covalent organic polymers have emerged as promising platforms with tailorable structures for electrocatalytic oxygen reduction reaction (ORR). However, their catalytic activities are often limited by dense stacking and low conductivities. Herein, we report an arylamine-linked iron-phthalocyanine (AAm-FePc) in situ grown on Ketjenblack (KB) (AAm-FePc/KB) via a condensation reaction between 2,9,16,23-tetraaminophthalocyaninato iron and dimethyl succinyl succinate. Characterizations reveal that AAm-FePc is uniformly distributed on the surface of KB, which provides a large accessible surface area and efficient electrical conductivity. Owing to abundant arylamine linkages present in the skeletons and precisely designed highly active Fe–N4 sites, the AAm-FePc/KB catalyst exhibits excellent ORR characteristics in alkaline media, including a half-wave potential of 0.883 V, fast kinetics (Tafel slope = 33 mV dec–1), a nearly four-electron reduction pathway and excellent methanol resistance and electrochemical stability. The AAm-FePc/KB-catalyzed Zn–air battery exhibits a high power density (177.8 mW cm–2), a large specific capacity (727 mAh g–1), and outstanding cycling stability (375 cycles, 125 h), which are superior to those of commercial Pt/C catalyst.
研究领域:
材料科学
·
电化学
·
催化
·
能量存储与转换
·
聚合物化学
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2024
·
IF 10.5
Yinghua Wang,Lingmin Wu,Konggang Qu,Xiujun Wang,Baitao Li
The oxygen reduction reaction (ORR) is a crucial step in the energy transformation devices, which requires the fabrication of a cost-effective and energy-efficient Fe single-atom catalyst (SAC) to substitute platinum. However, achieving a controllable synthesis of Fe SAC is a formidable challenge. In this study, a Fe SAC with a novel 3D-on-2D architecture was fabricated by coating 3D metal-organic frameworks (MOFs) over the surface of 2D reduced graphene oxide (rGO). In-situ combining MOF and rGO in a composite structure by adjusting their weight proportion is a key to preparing an active 3D-on-2D structured catalyst with FeN 4 active sites. Thanks to the favorable conductivity of the 2D rGO-derived carbon structure and the 3D MOF structure exposing an enhanced density of FeN 4 sites, FeNC@rGO-2 demonstrates exceptional ORR activity. It performs more effectively than commercial Pt/C, exhibiting excellent half-wave potentials of 0.887, 0.705, and 0.741 V in alkaline, neutral, and acidic solutions respectively. Impressively, FeNC@rGO-2 exhibits excellent stability and methanol tolerance. When FeNC@rGO-2 is assembled as cathode catalyst in Zinc-air batteries (ZAB) and microbial fuel cells (MFC), FeNC@rGO-2-ZAB reveals outstanding power density (393 mW cm −2 ) and good charge/discharge cycling stability. Amazingly, FeNC@rGO-2-MFC also shows superior power density (2810 ± 19 mW m −2 ) and efficiency of electron recovery. This study reveals that FeNC@rGO-2 has extremely high application value in energy conversion devices oriented for alkaline and neutral electrolytes.
研究领域:
材料科学
·
电化学
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Xiaojing Jiang,Jianian Chen,Fenglei Lyu,Chen Cheng,Qixuan Zhong,Xuchun Wang,Ayaz Mahsud,Liang Zhang,Qiao Zhang
Controllable fabrication of Fe-N-C based single-atom catalysts (SACs) for enhanced electrocatalytic performance is highly desirable but still challenging. Here, an in situ surface-confined strategy was demonstrated for the synthesis of single atomic Fe-N 4 on N-doped carbon nanoleaves (L-FeNC). The in situ generated Zn 3 [Fe(CN) 6 ] 2 could not only serve as a protection layer against collapse of nanoleaves but also provide abundant Fe source for the formation of Fe-N moieties during pyrolysis, leading to high surface area and high graphitization degree of L-FeNC simultaneously. Benefiting from abundant Fe-N 4 active sites, enhanced mass and charge transfer, the as-prepared L-FeNC manifested a half-wave potential of 0.89 V for oxygen reduction reaction (ORR) in 0.1 M KOH. A maximum power density of 140 mW cm −2 and stable discharge voltage even after operation for 50,000 s have been demonstrated when the L-FeNC was used as air cathode for Zn-air battery. This work not only provided a unique surface-confined strategy for the synthesis of two-dimensional nanocarbons, but also demonstrated the significant benefit from rational design and engineering of Fe-N-C SACs, thus offering great opportunities for fabrication of efficient energy conversion and storage devices.
研究领域:
材料科学
·
电化学
·
能源存储与转换
·
纳米科技
·
催化化学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2026
·
IF 5.8
Yanling Wu,Hui He,Zhitong Liu,Wenkai Fu,Yue Hu,Yixuan Wang,Yijie Wang,Qin Zhang
As leading nonprecious metal electrocatalysts for ORR, Fe–N–C systems still face critical limitations. The insufficient density of accessible metal active sites and the intrinsic balance conflict between activity and durability largely constrain their practical application. In this study, we employed a coupled strategy of electrostatic assembly and defect confinement, followed by two-step high-temperature pyrolysis under distinct activation atmospheres. Cobalt clusters were in situ grown on the surface of carbon nanotubes to form a micro–nano anchoring structure with edge defects, enabling the simultaneous immobilization of Fe–N4 moieties and uniform dispersion of Co clusters on nitrogen-doped carbon nanotube substrates. The resulting nanotube-shaped Co@Fe/NC-a catalyst (prepared at 1100 °C with hydrogen activation) exhibited markedly improved ORR activity and stability in 0.1 M KOH compared with Fe/NC-a. X-ray absorption spectroscopy revealed that the Co clusters modulate the electron distribution at the Fe–N4 sites. Further, density functional theory (DFT) calculations confirmed that the Co clusters alter the electronic structure of Fe–N4 sites, reducing the reaction energy barrier and improving catalytic performance. Overall, this work offers a viable strategy for improving ORR catalysts by electronically tuning Fe–N4 sites through adjacent metal clusters.
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Jun-Sheng Jiang,He-Lei Wei,Ai-Dong Tan,Rui Si,Wei-De Zhang,Yu-Xiang Yu
Iron-based single-atom catalysts with nitrogen-doped carbon as support (Fe-SA/NPC) are considered effective alternatives to replace Pt-group metals for scalable application in fuel cells. However, synthesizing high-loading Fe-SA catalysts by a simple procedure remains challenging. Herein, we report a high-loading (7.5 wt%) Fe-SA/NPC catalyst prepared by carbon-assisted pyrolysis of metal complexes. Both the nitrogen-doped porous carbon (NPC) support with high specific surface area and ο -phenylenediamine ( o -PD) play key roles role in the preparation of high-loading Fe-SA/NPC catalysts. The results of X-ray photoelectron spectroscopy, high-angle annular dark-field scanning transmission electron microscopy, and X-ray absorption fine structure spectroscopy experiments show that the Fe atoms are anchored on the carbon carriers in a single-atom site configuration and coordinated with four of the doped nitrogen atoms of the carbon substrates (Fe-N 4 ). The activities of the Fe-SA/NPC catalysts in the oxygen reduction reaction increased with increasing iron loading. The optimized 250Fe-SA/NPC-800 catalyst exhibited an onset potential 0.97 V of and a half-wave potential of 0.85 V. Our study provides a simple approach for the large-scale synthesis of high-loading single-atom catalysts.
研究领域:
材料科学
·
电化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2022
·
IF 11.307
Wenjie Wei,Fenghong Lu,Lixiu Cui,Yu Zhang,Yanze Wei,Lingbo Zong
Tuning of the coordination environment of atomically dispersed single atoms (SAs) by heteroatom doping is a promising strategy to boost the electrocatalytic activity for oxygen reduction reaction (ORR). The synergistic effect of dual heteroatom doping provides additional degrees of freedom to achieve higher ORR efficiency through decreased energy barriers of the intermediates in catalytic processes. Herein, Fe–SAs anchored within the N, S co-doped porous nanosized carbonaceous spheres (Fe–SAs@N/S-PCSs) was fabricated through the pyrolysis of anchored heteroatom sources and ferric precursors. Under the low catalyst loading capacity of 0.255 mg cm −2 , the obtained Fe–SAs@N/S-PCSs exhibits exceptionally high performance with ORR onset potential (E onset ) of 1.02 V, and half wave potential (E 1/2 ) of 0.90 V (vs. RHE) in 0.1 M KOH solution, outperforming benchmark Pt/C (E onset = 1.01 V, E 1/2 = 0.86 V). Superior oxygen evolution reaction (OER) activity (450 mV at 10 mA cm −2 ) is also demonstrated, thus displaying outstanding performance for Zn-air battery. The porous structure , rich accessible Fe SAs, and the optimal binding of ORR-related species induced by S doping in carbon matrix generate the excellent ORR activity and durability. This work provides insights into the rational design of cost-effective single atom catalysts (SACs) with impressive electrocatalytic activities for efficient energy conversion applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2021
·Vol. 8
·期 22
·2101824
·
IF 16.806
Jun Wang,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
Fenton-like reactions with persulfates as the oxidants have attracted increasing attentions for the remediation of emerging antibiotic pollutions. However, developing effective activators with outstanding activities and long-term stabilities remains a great challenge in these reactions. Herein, a novel activator is successfully synthesized with single iron atoms anchored on porous N-doped carbon (Fe-N-PC) by a facile chemical vapor deposition (CVD) method. The single Fe atoms are coordinated with four N atoms according to the XANES, and the Fe-N 4 -PC shows enhanced activity for the activation of peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). The experiments and density functional theory (DFT) calculations reveal that the introduction of single Fe atoms will regulate the main active sites from graphite N into Fe-N 4 , thus could enhance the stability and tune the PMS activation pathway from non-radical into radical dominated process. In addition, the N atoms connected with single Fe atoms in the Fe-N 4 -C structure can be used to enhance the adsorption of organic molecules on these materials. Therefore, the Fe-N 4 -C here has dual roles for antibiotics adsorption and PMS activation. The CVD synthesized Fe-N 4 -C shows enhanced performance in persulfates based Fenton-like reactions, thus has great potential in the environmental remediation field.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-15
·
IF 16.6
Wei Shengjie,Sun Yibing,Qiu Yun-Ze,Li Ang,Chiang Ching-Yu,Xiao Hai,Qian Jieshu,Li Yadong
Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, and revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect engineering of single Fe-N 4 sites in ZnO-Carbon nano-reactor, as efficient catalyst in Fenton-like reaction for degradation of phenol. The carbon vacancies are easily constructed adjacent to single Fe-N 4 sites during synthesis, facilitating the formation of C-O bonding and lowering the energy barrier of rate-determining-step during degradation of phenol. Consequently, the catalyst Fe-NCv-900 with carbon vacancies exhibits a much improved activity than the Fe-NC-900 without abundant carbon vacancies, with 13.5 times improvement in the first-order rate constant of phenol degradation. The Fe-NCv-900 shows high activity (97% removal ratio of phenol in only 5 min), good recyclability and the wide-ranging pH universality (pH range 3-9). This work not only provides a rational strategy for improving the Fenton-like activity of metal single-atom catalysts, but also deepens the fundamental understanding on how periphery carbon environment affects the property and performance of metal-N 4 sites.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）