JOURNAL OF POWER SOURCES
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2019
·
IF 7.467
Yunfeng Zhan,Hongbin Zeng,Fangyan Xie,Hao Zhang,Weihong Zhang,Yanshuo Jin,Yueli Zhang,Jian Chen,Hui Meng
This work reports a rational design of non-precious metal catalyst for oxygen reduction reaction in acidic media to be used in polymer electrolyte membrane fuel cell. A strategy is designed to avoid the agglomeration of metal compound during the pyrolysis of precursor. MgO template is introduced into a 1-10-phenanthroline-iron (II) precursor to promote the evolution of Fe-Nx active sites while avoiding the formation of inactive species. The template also contributes to the formation of micro/mesoporous structure. The as-prepared catalyst shows good performance in half-cell test with half-wave potential of 0.80 V in acidic media. The catalyst reaches a current density of 0.76 A cm −2 at 0.6 V iR-free along with encouraging durability in H 2 –O 2 fuel cell test.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Junhao Chen,Shutian Lin,Sisi Xiang,Yuanhong Zhong,Yingxia Zhao,Ming Sun,Lin Yu
A ZIF-8-derived Fe–N–C single-atom catalyst is developed for HMF-to-FFCA oxidation. • The catalyst obtained 99.4% HMF conversion and 94.2% FFCA yield under mild conditions. • O 2 • and 1 O 2 are identified as the key reactive species governing selective oxidation. • Fe–N x moieties are confirmed as the active centers for O₂ activation and selectivity. The catalytic valorization of 5-hydroxymethylfurfural (HMF) to high-value chemicals is critical for sustainable chemistry. However, 5-formyl-2-furancarboxylic acid (FFCA), a key oxidation intermediate, remains a significant challenge. Herein, a Fe N C single-atom catalyst derived from zeolitic imidazolate framework-8 (ZIF-8) is developed for efficient HMF-to-FFCA conversion under mild conditions (90 °C, 0.1 MPa O 2 ). It has been revealed that the isolated Fe–N x sites are dispersed on a nitrogen-doped carbon matrix. The optimized catalyst delivers 99.4% HMF conversion with 94.2% FFCA yield within one hour, and exhibits excellent catalytic and structural stability over consecutive reaction cycles. Mechanistic studies combining Electron paramagnetic resonance (EPR) spectroscopy and radical trapping experiments demonstrate that superoxide radicals (O 2 • ) and singlet oxygen ( 1 O 2 ) govern the selective oxidation pathway. Active-site poisoning with thiocyanate confirms the essential role of Fe–N x moieties in oxygen activation. This work presents a robust non-noble metal catalyst platform for HMF valorization and advances the fundamental understanding of single-atom catalyst design for biomass oxidation reactions. Download: Download high-res image (189KB) Download: Download full-size image
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MOLECULES
·
2023
·Vol. 28
·期 7
·2879
·
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
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Wenlu Yang,Bingran Guo,Ziyu Guo,Xue Wang,Yanli Zeng,Jianing Guo,Mingxing Wu
Designing low-cost and high-efficiency non-noble metal electrocatalysts for the oxygen reduction reaction (ORR) is critical for the development of renewable and sustainable energy devices. It is of essential importance to precisely design and rationally adjust the porous morphology and nanostructure of catalysts to improve mass transfer and the accessibility of active sites. Herein, we elaborately designed a unique hollow hierarchical porous carbon nanofiber with Fe3O4/Fe–N–C sites anchored as a high-efficiency electrocatalyst for ORR. The hollow porous carbon nanofibers (HPCNFs) were prepared via a facile convenient coaxial electrospinning technology to fabricate the hollow carbon nanofibers and through zinc nitrate-assisted pyrolysis to form a hierarchical porous structure. Benefiting from its unique hollow porous construction, facilitated mass transfer, and highly accessible active sites, the optimized Fe-HPCNFs catalyst exhibited significant ORR performance and stability, with a half-wave potential of 0.89 V outperforming the commercial catalyst (20% Pt/C). Remarkably, Zn–air batteries assembled with Fe-HPCNFs achieved excellent activity with a robust peak power density of 172 mW·cm–2 and a high specific capacity of 905.4 mAh·gZn–1. Furthermore, the ORR mechanism was investigated by density functional theory calculations, demonstrating that the synergistic effect of Fe3O4 nanoparticles and Fe–N–C active sites can effectively boost the electrocatalytic activity for ORR.
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CATALYSIS LETTERS
·
2023
·Vol. 153
·期 12
·3569-3580
·
IF 2.8
Lin Shanshan,Liu Jianguo,Ma Longlong
Aniline is a group of important platform molecules that has been widely used in the synthesis of other high-value chemicals and pharmaceutical products. How to produce high-value anilines as the high-value chemical intermediates more efficiently and environmentally has always been a research topic in the industry. Catalytic hydrogenation is an environmentally friendly method for preparing halogenated anilines. Traditional noble metal catalysts face the problems of cost and noble metals residue. To improve the purity of the product as well as the activity and recyclability of the catalyst, we prepared a Pd/Fe magnetic bimetallic catalyst supported on N-doped carbon materials to reduce nitrobenzene to aniline under mild conditions. The catalyst has a low Pd loading of 2.35%. And the prepared bimetallic Pd/Fe@N/C catalyst showed excellent catalytic reactivity with the nitrobenzene conversion rate of 99%, and the aniline selectivity of 99% under mild reaction conditions of 0.8 MPa H 2 and 40 °C. A variety of halogenated and aliphatic nitro compounds were well tolerated and had been transformed to the corresponding target amine products with excellent selectivity. In addition, the novel N-doped graphene-encapsulated bimetallic magnetic Pd/Fe@N/C catalyst not only had magnetic physical properties, which was easy to separate, recover, and used for the recycling of the catalyst without metal leaching but also catalyzed highly selective reductive amination of aromatics was a green, economical and environmentally friendly reaction with the only by-product of H 2 O. Graphical Abstract
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高影响因子
NANOTECHNOLOGY
·
2021
·Vol. 32
·期 30
·305402
·
IF 3.874
Yaqi Cui,Jiaoxing Xu,Yi Zhao,Lunhui Guan
The utilization of earth abundant iron and nitrogen doped carbon as a precious-metal-free electrocatalyst for oxygen reduction reaction (ORR) significantly depends on the rational design and construction of desired Fe−Nx moieties on carbon substrates, which however remains an enormous challenge. Herein a typical nanoporous nitrogen-rich single atom Fe−N/C electrocatalyst on carbon nanotube (NR-CNT@FeN-PC) was successfully prepared by using CNT as carbon substrate, polyaniline (PANI) and dicyandiamine (DCD) as binary nitrogen sources and silica-confinement-assisted pyrolysis, which not only facilitate rich N-doping for the inhibition of the Fe agglomeration and the formation of single atom Fe−Nx sites in carbon matrix, but also generate more micropores for enlarging BET specific surface area (up to 1500 m2·g−1). Benefiting from the advanced composition, nanoporous structure and surface hydrophilicity to guarantee the sufficient accessible active sites for ORR, the NR-CNT@FeN-PC catalyst under optimized conditions delivers prominent ORR performance with a half-wave potential (0.88 V versus RHE) surpass commercial Pt/C catalyst by 20 mV in alkaline electrolyte. When assembled in a home-made Zn−air battery device as cathodic catalyst, it achieved a maximum output power density of 246 mW·cm−2 and a specific capacity of 719 mA·h·g−1Zn outperformed commercial Pt/C catalyst, holding encouraging promise for the application in metal-air batteries.
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Materials Today Energy
·
2020
·
IF 5.604
Kuofeng Xu,Huayuan Bao,Chaoyun Tang,Kristina Maliutina,Fengjiao Li,Liangdong Fan
The development of non-platinum electrocatalysts for the quick oxygen reduction reaction (ORR) is highly desirable in electrochemical energy conversion technologies such as fuel cells and metal-air batteries. In this work, we synthesize Fe 3 O 4 /Fe–N–C-CNT (FeNC) using Fe 3+ adsorbed ZIF-8 as a chemical precursor that is obtained with a green and sustainable procedure. FeNC possesses impressive ORR activities, stability and selectivity over that of the commercial Pt/C electrocatalyst in alkaline media, and demonstrates a better peak power density of 118.05 mW cm −2 over that with Pt/C cathode and quicker reaction kinetics when integrated as air electrode catalyst into a primary zinc-air battery. In-depth investigation confirms that the presence of Fe 3 O 4 increases the wettability of carbon-based composite that promotes the adsorption of the dissolved O 2 in the electrolyte solution and extends the triple-phase boundary for ORR, and also protect the active site of Fe–N–C from poisoning. This work sheds light on a sustainable method to synthesize highly efficient non-precious metal-based electrocatalyst from metal-organic-framework precursors and understanding the reaction mechanism of the ORR process for efficient chemical energy to electricity conversion.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Zhiyan Huang,Pingxiao Wu,Chenhui Liu,Meiqing Chen,Shanshan Yang,Zhi Dang,Nengwu Zhu
Understanding the origin of high activity of graphene layers encapsulated Fe-N-C catalysts in Fenton-like reaction is critical, but still challenging for developing catalysts with high activity and durability. Therefore, we prepared a highly active Fe-N-C catalyst (Fe x Mn y -Fe@NCs) containing FeN 4 coordination to activate peroxymonosulfate (PMS) toward 4-aminobenzoic acid ethyl ester (ABEE) degradation, and revealed the multiple catalytic reaction sites by investigating the composition and the structure of the catalyst. The relationship between the catalytic degradation performance and multiple catalytic reaction sites was performed on the basis of both experiments and density functional theory (DFT) calculations. The catalytic performance of Fe 2 Mn 1 -Fe@NCs was found to show optimal catalytic degradation performance. Pyrrolic N served as adsorption site as well as singlet oxygen generation site to promote the catalytic degradation. Fe-pyridinic N-C acted as hydroxyl radical and sulfate radical generation site. Both singlet oxygen and superoxide radical were dominated the catalytic reaction. The insight achieved from this study may be further applied to other Fe-N-C catalysts design and further efficient organic pollution remediation.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Fei He,Li Mi,Yanfei Shen,Toshiyuki Mori,Songqin Liu,Yuanjian Zhang
Developing highly efficient biomimetic catalysts that directly use O2 as the terminal oxidant to dehydrogenate and monoxygenate substrates with high selectivity under mild conditions has long been pursued but rarely achieved yet. Herein, we report that heterogeneous Fe–N–C, which is commonly used as an electrocatalyst for oxygen reduction reaction, had unusual biomimetic catalytic activity in both dehydrogenation and monoxygenation of a series of organic molecules (∼100% selectivity) by directly using O2. The Fe–Nx center was verified to be the active site that reductively activated O2 by spontaneously generating specific reactive oxygen species (ROS) (1O2, O2•–, and H2O2). Aided by these ROS, under physiological conditions, the Fe–N–C was further successfully exampled to kill proliferative lung cancer cells. Fe–N–C had several striking superior features with respect to natural enzymes, classical heterogeneous nanozymes, and homogeneous artificial enzymes incapable of working under harsh conditions (extreme pH and high temperature), ease of separation and recycling, and direct use of O2. It would open up a new vista of Fe–N–C as an artificial enzyme in biomimetic catalysis, ranging from fundamental simulation of oxidase/oxygenase metabolism to industrial oxidation processes and to disease treatment.
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Nanoscale
·
2024
·Vol. 16
·期 48
·22273-22282
·
IF 5.8
Feng Li,Kairen Zhao,Yan Jin,Baoxin Li
Currently, water treatment usually requires additional light illumination or oxidants for the degradation of organic pollutants, which increases the costs and is not conducive to practical application. In this study, carbon vacancy-modified Fe–N–C single-atom catalysts (Cv-Fe–N–C SACs) were prepared through one simple acid-etching and pyrolysis process. Interestingly, we found that Cv-Fe–N–C SACs could degrade organic pollutants without any external assistance (such as oxidants or light illumination). The Cv-Fe–N–C SACs could remove over 99% of Rhodamine B (RhB) within 10 min at room temperature. The degradation of organic pollutants with the Cv-Fe–N–C SACs was attributed to their ability to activate dissolved oxygen for producing superoxide (O2˙−). In addition, the catalysts showed high activity over a broad pH range (3–11) and held rather good stability after 5 recycles. This study proved that the Cv-Fe–N–C SACs are highly efficient catalysts for degrading organic pollutants. These catalysts have the potential to make sewage treatment more efficient and less expensive.
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Environmental Science-Nano
·
2020
·Vol. 7
·期 12
·3814-3823
·
IF 7.683
Hanfeng Zhou,Zhibo Deng,Tianbao Liu,Tao Liu,Lijuan Zhang,Xintai Su,Zhang Lin
The science linking thermochemical conversion of large-scale industry oily sludge with applied materials has been improved in the last ten years. However, with the traditional converting methods it is hard to precisely control the composition and structure of oily sludge-based products during pyrolysis due to the complexity of the composition of the oily sludge. Here, a chlorinating calcination method using sodium chloride (NaCl) as a chlorinating salt and template was first developed to prepare porous Fe–N–C materials (FCN-500) through pyrolysis of oily sludge containing iron-bearing minerals and pyridine. The formation mechanism of FCN-500 was proposed, where iron ions (Fe3+) from the inorganic component (anorthite) in the sludge were rapidly dissociated with the assistance of NaCl, followed by coordination with the organic component (pyridine nitrogen) in the oily sludge to form the pyridine nitrogen–iron ((C5H6N)n–Fe) complex, and then carbonization. As-obtained FCN-500 exhibited higher specific capacitance (286.3 F g−1 at a current density of 0.5 A g−1), enhanced energy density (33.5 W h kg−1 at a power density of 606.1 W kg−1) and more excellent stability and durability (more than 80.1% capacitance retention after 10 000 cycles) compared with two other electrodes. The reasonably better performance of the obtained FCN-500 in supercapacitors (SCs) is attributed to its large surface area, hierarchically porous channels, high conductivity, and unique Fe–N–C structure. Therefore, this work not only provides a feasible way to solve the bottleneck problem in sludge pyrolysis, but also provides a method to design large scale porous Fe–N–C materials for practical applications.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yuzhe Liu,Qi Li,Yuhan Liang,Junhao Liang,Wenliang Feng,Bin Wu,XuLei Sui,Zhenbo Wang
The inherently low active site accessibility of single-atom Fe-N-C catalysts severely compromises their catalytic activity relative to Pt-based catalysts, thereby hindering their practical implementation in critical applications. This work systematically investigates the synergistic effects of physical confinement and chemical induced growth strategy on optimizing active site accessibility of Fe-N-C catalysts for oxygen reduction reaction. Through a physical confinement strategy, the catalyst particle size is successfully reduced from the micrometer scale to the nanometer scale. Subsequently, by employing chemical-induced growth, the particle size is precisely controlled within the range of 623 nm to 421 nm, simultaneously establishing an optimal balance between the catalyst particle size threshold (420 nm) and the ordered macroporous framework. This approach maximized the accessibility of active sites and significantly enhanced the catalytic activity of the Fe-N-C catalyst. The optimized catalyst (OM-Fe-NC-4) exhibits outstanding performance, achieving a remarkable half-wave potential of 0.888 V, surpassing both commercial Pt/C and most state-of-the-art Fe-N-C catalysts. Additionally, it demonstrates excellent four-electron selectivity and delivers a kinetic current density of 14.7 mA cm −2 at 0.85 V in acidic medium. This dual-dimensional modulation strategy offers a paradigm for enhancing the accessibility of active sites for non-precious metal catalysts.
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