Sustainable Energy & Fuels
·
2025
·
IF 4.1
Yongheng Xiong,Yang Yu,Huangang Shi,Jifa Qu,Wenyi Tan
Single atom Fe sites, doped in CN materials, exhibit outstanding electrochemical activity for CO2-to-CO conversion. The pyrolysis of ZIF8 is a controllable method for fabricating isolated single atom metal sites. In this study, we propose a new strategy to increase the ratio of Fe in ZIF8 precursors by synergistically replacing Zn2+ with Bi3+ and Fe3+. After precursor pyrolysis, the obtained Bi/Fe–N–C catalysts, consisting of Bi sites and pyrrole-type Fe–Nx sites, serve as efficient electrocatalysts for the CO2RR. The results show that the optimized catalyst loaded with 94.8 mg per kgCat Fe exhibits a high FECO of >90.1% over a wide potential range of −0.4 to −0.7 VRHE (98.2% at −0.5 VRHE). Insights into the electrochemical reaction mechanism show that this successful design of Bi/Fe–N–C catalysts can provide a stable catalytic site to form *COOH, thus achieving energy-efficient electrochemical CO2 reduction to CO.
研究领域:
材料科学
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电化学
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催化
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能量转换
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环境科学
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 13
·6058-6065
·
IF 3.3
Xu Zhang,Jingxian Zhang,Shi Zeng,Haifan Wang,Yiling Bai,Huaming Hou,Ke Zhang,Bin Li,Guangjin Zhang
Iron–nitrogen-doped carbon (Fe–N–C) catalysts have been theoretically and experimentally demonstrated as one of the most promising materials to promote the oxygen reduction reaction (ORR), but they still have drawbacks in terms of stability and longevity. Herein, a novel strategy of loading Fe–N–C on cerium oxide cyanamide (Ce2O2CN2) is proposed to increase the density of active sites and improve the activity effectively. Ce2O2CN2 provides a Ce4+/Ce3+ redox pair to regulate the oxygen density on the catalyst surface, and the π–π interactions between Ce2O2CN2 and Fe–N–C are beneficial for interfacial charge transport. Consequently, Fe–N–C@Ce2O2CN2 shows excellent ORR activity with a half-wave potential (E1/2) of 0.89 V vs RHE and satisfactory long-term durability in an alkaline medium, and significantly outperforms commercial Pt/C. The Zn–air batteries made using the prepared catalyst exhibited a high peak power density of 119.35 mW cm−2. This study provides a new perspective for the application of platinum group-metal (PGM)-free catalysts in next-generation energy storage devices.
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Nano Research
·
2020
·Vol. 13
·期 9
·2420-2426
·
IF 8.183
Luo Ergui,Wang Chen,Li Yang,Wang Xian,Gong Liyuan,Zhao Tuo,Jin Zhao,Ge Junjie,Liu Changpeng,Xing Wei
Fe/N/C material is the most competitive alternative to precious-metal catalysts for oxygen reduction. In view of the present consensus on active centers, further effort is directed at maximizing the density of single Fe atoms. Here, the imperfections in commonly used doping strategy of Fe for the synthesis of zeolitic imidazolateframework (ZIF)-derived Fe/N/C catalysts are revealed. More importantly, a strikingly improved catalyst is obtained by a ‘second pyrolysis’ method and delivers a half-wave potential of 0.825 V (vs. RHE) in acidic media. The strong confinement effect of carbonaceous host accounts for the formation of dense single-atom sites and thus the high activity. Our findings will potentially facilitate future improvement of M/N/C catalysts.
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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.
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ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Yingfang Yao,Yong You,Gaixia Zhang,Jianguo Liu,Haoran Sun,Zhigang Zou,Shuhui Sun
Tuna is one of the most rapid and distant swimmers. Its unique gill structure with the porous lamellae promotes fast oxygen exchange that guarantees tuna’s high metabolic and athletic demands. Inspired by this specific structure, we designed and fabricated microporous graphene nanoplatelets (GNPs)-based Fe/N/C electrocatalysts for oxygen reduction reaction (ORR). Careful control of GNP structure leads to the increment of microporosity, which influences the O2 adsorption positively and desorption oppositely, resulting in enhanced O2 diffusion, while experiencing reduced ORR kinetics. Working in the cathode of proton-exchange membrane fuel cells, the GNP catalysts require a compromise between adsorption/desorption for effective O2 exchange, and as a result, appropriate microporosity is needed. In this work, the highest power density, 521 mW·cm–2, at zero back pressure is achieved.
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Lizhang Chen,Xuan Wang,Tingyu Lu,Huan Pang,Songtao Zhang,Lin Xu,Gaixiu Yang,Qixing Zhou,Yawen Tang
As one of the most competitive alternatives to precious Pt-based electrocatalysts towards the oxygen reduction reaction (ORR), Fe-N-C single atom catalysts (SACs) are still eagerly anticipated to undergo further performance enhancement to advance their practical applications in diverse renewable energy systems. The regulation of energy level of Fe site through the manipulation of d-orbital splitting manner provides a novel route to improve the intrinsic activity, yet still in its infancy. We herein present a Fe d-orbital splitting modulation strategy via crafting atomically dispersed Fe-N 5 moieties with axial N ligand anchored on “lotus root”-like N-doped multichannel carbon nanofibers (abbreviated as FeN 5 @NMCNFs hereafter). Symmetrical experimental and theoretical findings reveal that near-range coordinated effect of axial N ligand results in the deformation of local symmetry, deep valence band spin-polarization of d orbitals and downshifted d-band center of Fe center site, endowing the optimized adsorption energetics of ORR intermediates and reduced reaction energy barrier. Accordingly, the as-developed FeN 5 @NMCNFs deliver Pt-competitive ORR activity and extraordinary long-term durability in KOH electrolyte with a halfwave potential of 0.87 V, exceeding a majority of recently reported non-precious SACs. Furthermore, when incorporated into liquid and flexible all-solid-state Zn air batteries (ZABs), the FeN 5 @NMCNFs||RuO 2 -assembled ZABs demonstrate superior electrochemical performance to the state-of-the-art Pt/C||RuO 2 counterpart. This work offers a new perspective for the performance optimization of SACs via the manipulation of the local coordination manner and the precise spin-polarization regulation strategy.
研究领域:
材料科学
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电催化
·
能源化学
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高影响因子
Joule
·
2024
·
IF 38.6
Jia-Ning Liu,Chang-Xin Zhao,Juan Wang,Xuan-Qi Fang,Chen-Xi Bi,Bo-Quan Li,Qiang Zhang
Refreshing the record of the electrocatalytic activity for bifunctional oxygen electrocatalysis is the first priority of developing next-generation rechargeable zinc-air batteries. A Δ E indicator to evaluate the bifunctional electrocatalytic activity has stagnated with a record of Δ E > 0.60 V for decades. Herein, a bifunctional oxygen electrocatalyst is developed to afford an ultrahigh bifunctional electrocatalytic activity of Δ E = 0.57 V and realize high-performance rechargeable zinc-air batteries. Specifically, atomically dispersed Fe-N-C sites and NiFeCe layered double hydroxides are integrated to afford a composite FeNC@LDH electrocatalyst, following the guidance of the data-driven analysis. The FeNC@LDH electrocatalyst demonstrates a record-breaking electrocatalytic activity of Δ E = 0.57 V, far exceeding the state-of-the-art level by ca. 60 mV. Practical ampere-hour-scale zinc-air batteries are constructed with a capacity of 6.4 Ah and cycle under 1.0 A and 1.0 Ah conditions. This work affords a record-breaking bifunctional electrocatalyst for ampere-hour-scale zinc-air batteries in future application scenarios.
研究领域:
材料科学
·
电化学
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高影响因子
NANOTECHNOLOGY
·
2019
·Vol. 30
·期 30
·305402
·
IF 3.399
Tong Wu,Yaying Li,Yuntong Li,Jing Hong,Haiyang Wu,Jie Mao,Yuzhe Wu,Qipeng Cai,Conghui Yuan,Lizong Dai
Simultaneous introduction of both transition metal and other inorganic elements into the carbon matrix has attracted great attention in the fabrication of carbon materials with high electrochemical properties. Herein, rational design of ligand-iron coordinative supramolecular precursors is achieved for the fabrication of Fe-N/C catalysts, which possess high oxygen reduction reaction (ORR) performance. A series of precursors are prepared by a simple coordination reaction between a three armed catechol monomer and iron ions. Particular interest is focused on tuning the doping species, surface area and morphology of the Fe-N/C catalysts through a simple selection of iron resources. We show that an Fe-N/C catalyst derived from Fe2(SO4)3 at a carbonization temperature of 800 °C, has the optimized ORR performance with an onset potential of 0.930 V and half-wave potential of 0.801 V. Detailed investigation indicates that the synergistic effect among doping elements of nitrogen and sulfur and the unique carbon structure determines the performance of the Fe-N/C catalysts. Our findings may be of significance for the fabrication of doped carbon materials using coordinative supramolecular polymers as precursors.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Youyou Feng,Jing Qin,Yu Zhou,Qin Yue,Jing Wei
Nanozyme has been regarded as an efficient antibiotic to kill bacteria using the reactive oxygen species (ROS) generated by Fenton-like reaction. However, its activity is still unsatisfied and requires large amount of hydrogen peroxide with side effects toward normal tissues. Herein, spherical mesoporous Fe-N-C single-atom nanozyme (SAzyme) is designed for antibacterial therapy via photothermal treatment enhanced Fenton-like catalysis process. Due to the large pore size (4.0 nm), high specific surface area (413.9 m 2 g −1 ) and uniform diameter (100 nm), the catalytic performance of Fe-N-C SAzyme is greatly improved. The Michaelis-Menten constant ( K m ) is 4.84 mmol L −1 , which is similar with that of horseradish peroxidase (3.7 mmol L −1 ). Moreover, mesoporous Fe-N-C SAzyme shows high photothermal conversion efficiency (23.3 %) owing to the carbon framework. The catalytic activity can be enhanced under light irradiation due to the elevated reaction temperature. The bacteria can also be killed via physical heat effect. Due to the synergistic effect of nanozyme catalysis and photothermal treatment, the antibacterial performance is much higher than that using single antibacterial method. This work provides an alternative for combined antibacterial treatment via photothermal treatment assisted catalytic process using spherical mesoporous single-atom nanozyme as an antibiotic.
研究领域:
材料科学
·
纳米技术
·
生物医学工程
·
化学工程
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DOI
PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2026
·
IF 5.9
Xiaofei Guo,Zhongyao Guo,Chen Wang,Candong Liu,Honghui Cheng,Kuikui Wang
The highly active and stable oxygen reduction reaction (ORR) process is essential for driving the development of zinc-air batteries (ZABs). Therefore, by integrating the precise regulation of precursors, the tannic acid (TA) etching and nitrogen coordination strategy, a nitrogen-rich hierarchical porous Fe-N-C catalyst was successfully constructed. The uniform dispersion of particles was achieved by controlling the formation of the Fe-ZIF-8 precursor. Subsequent TA etching formed a rich mesoporous/microporous structure to improve active-site exposure. During the high-temperature pyrolysis process with melamine as the nitrogen source, a highly dispersed Fe-N X coordination structure was formed. Based on this rational design, the obtained catalyst presents a hierarchical porous structure, high nitrogen content and superior ORR activity, with a half-wave potential of 0.91 V in 0.1 M KOH solution. When applied to liquid and flexible ZABs, the catalyst delivers peak power densities of 186 mW cm −2 and 75 mW cm −2 , respectively, and cycling stability of over 1486 h is maintained in the liquid system-surpassing the performance of commercial Pt/C + RuO 2 . This research offers a fresh perspective on the design and synthesis of efficient ND-FeNC-TA catalysts and promotes the practical application of ZABs.
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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.
研究领域:
材料科学
·
电化学
·
能量转换
·
高分子化学
·
催化
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lingfeng Li,Yandi Wen,Guokang Han,Yuxin Liu,Yajie Song,Wei Zhang,Jia Sun,Lei Du,Fanpeng Kong,Yulin Ma,Yunzhi Gao,Jiajun Wang,Chunyu Du,Geping Yin
Developing advanced non-precious metal catalysts towards acidic oxygen reduction reaction (ORR) is critical for electrochemical energy conversion devices. Fe-N-C catalysts are demonstrated to be the most promising alternatives to platinum-based catalysts for ORR. Herein, Fe single atoms (SAs) coordinated by pyridinic nitrogen catalysts (denoted as Fe-pyridinic N-C) are synthesized through pyrolysis of ZIF-8 encapsulating ferrocene. Owing to the synergistic effects between Fe SAs and pyridinic N, Fe-pyridinic N-C exhibits remarkable ORR activity and outstanding stability in acid media, evidenced by golden kinetic current density of 9.71 mA cm −2 at 0.8 V, along with only 21 mV decrease in half-wave potential after 20,000 cycles. Theoretical calculations demonstrate that pyridine-type N possesses stronger binding energy with Fe SAs compared with pyrrole-type N, in other words, high pyridinic N content will help stabilize the catalyst. This study will be of great significance for the development of non-noble metal catalysts towards ORR with enhanced stability in acidic media.
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