ACS Catalysis
·
2014
·
IF 7.572
Mei-Qing Wang,Wei-Hua Yang,Hong-Hui Wang,Chi Chen,Zhi-You Zhou,Shi-Gang Sun
Aimed at developing a highly active and stable non-precious metal catalyst (NPMC) for oxygen reduction reaction (ORR) in acidic proton-exchange membrane fuel cells (PEMFCs), a novel NPMC was prepared by pyrolyzing a composite of carbon-supported Fe-doped graphitic carbon nitride (Fe–g-C3N4@C) above 700 °C. In this paper, the influence of the pyrolysis temperature and Fe content on ORR performance was investigated. Rotating disk electrode (RDE) and rotating ring-disk electrode (RRDE) studies reveal that, with a half-wave potential of 0.75 V [versus reversible hydrogen electrode (RHE)] and a H2O2 yield of 2.6% at 0.4 V, the as-synthesized catalyst heat-treated at 750 °C with a Fe salt/dicyandiamide (DCD) mass ratio of 10% displays the optimal ORR activity and selectivity. Furthermore, the pyrolyzed Fe–N–C composite exhibits superior durability in comparison to that of commercial 20 wt % Pt/C in acidic medium, making it a good candidate for an ORR electrocatalyst in PEMFCs.
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高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Xu Chao,Hou Jingting,Tang Zeming,Lai Qingxue,Liang Yanyu
Iron–nitrogen co-doped carbon (Fe/N/C) catalysts derived from zinc-based zeolite imidazole frameworks (ZIF-8) have been ideal alternatives to platinum group metals (PGM) and shown great potential to catalyze oxygen reduction reaction (ORR). Unfortunately, the ORR performance is seriously suppressed by the insufficient density and accessibility of the electrochemical active Fe–N sites. The precise regulation of ZIF-8 to the formation of Fe/N/C catalysts with the desired Fe–N sites for ORR is a critical challenge. Herein, a citric acid assisted reconstitution strategy is proposed to design Fe doped ZIF-8 frameworks and construct multi-dimensional Fe/N/C catalysts composed of inner concave and entangled carbon nanotubes outer moieties for efficient acid-resistant ORR reaction. The introduction of citric acid imparts Fe/N/C catalysts with dense accessible active sites and highly opened multi-dimensional mass transfer pathways. Therefore, the optimized Fe/N/C catalysts dominant half-wave potential of 0.785 V and great acid stability were obtained in 0.5 M H 2 SO 4 with a high number of transferred electrons and a low yield of H 2 O 2 ( \(\overline{{\text{n}}}\) = 3.97 and average yield = 4%). This work provides a novel and feasible approach to design and tailoring of Fe/N/C catalysts with improved distribution density and accessibility of the Fe–N active sites. Graphical Abstract
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Guangchao Li,Youbin Zheng,Hao Guo,Ze Li,Guohao Zhu,Liang Dong,Xin Liu,Jianbing Zang
In this paper, we present a method to enhance the stability of Fe–N–C electrocatalysts, known for their significant oxygen reduction reaction (ORR) activity and positioned as promising alternatives to commercial noble metal-based catalysts. Despite the favorable ORR activity, Fe–N–C suffers from inadequate stability in acidic media, primarily attributed the loss of active FeN 4 sites resulted from Fe-demetalation. However, recent investigation reveals that pyridine N exhibits remarkable stability in retaining Fe atoms. To address this, we achieved a high proportion of pyridine N doping in carbon nanofibers through a process involving nano-SiO 2 shell coating and electrospinning. The nano-SiO 2 shell coating method demonstrates efficacy and versatility in transforming pyrrole-type FeN 4 into pyridine-type FeN 4 , irrespective of the origin material being trivalent or divalent Fe, whether organic or inorganic.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yu Shi,Guanhua Ren,Jiajie He,Wei Yang,Jingjing Bao,Licheng Sun,Zhengyu Mo,Min Du
With the growing global demand for sustainable energy solutions, there is increasing interest in the conversion of low-grade heat into useful electrical energy. Thermoelectrochemical cells (TECs) are a promising technology for low-grade heat harvesting. However, sluggish reaction kinetics limit the power generation and efficiency of the TECs. In this study, we propose a Fe–N–C catalyst in situ grown on three-dimensional graphite felt as a self-supporting electrode for TECs. The graphite felt substrate provides a multidimensional structure to facilitate mass transport, while the Fe–N–C catalyst enhances electrode activity for redox reactions. The physicochemical properties and electrochemical performance of the electrode are characterized. The results demonstrate that the optimized electrode achieves a maximum power density of 1938 mW/m2 and a Carnot-relative efficiency of 2.29%, representing 11-fold and 12-fold improvements over graphite felt, respectively. These metrics surpass recent benchmarks in the field of TEC research. Furthermore, the electrode maintains a Carnot-relative efficiency of 2.0% in solar-driven TEC operation, demonstrating feasibility in photothermal and thermoelectrochemical conversion. Modeling analysis reveals that ion transport dominates heat and mass transfer processes, critically influencing power generation and stability, thereby highlighting the need for future optimization of ion transport pathways. This work validates the feasibility of in situ-grown Fe–N–C catalysts on graphite felt as high-performance TEC electrodes, offering a strategic framework for advancing waste heat recovery systems through rational electrode design and transport engineering.
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Catalysts
·
2025
·Vol. 15
·期 9
·850
·
IF 4
Qiongqiong He,Xuewen Wu,Ping Ma,Zhaoyang Song,Xiaoqi Wu,Ruize Gao,Zhenyong Miao
Phenol is a refractory organic pollutant that is difficult to degrade in wastewater treatment, and efficiently and stably degrading phenol presents a significant challenge. In this study, iron-doped humic acid-based nitrogen–carbon materials were prepared to activate peroxymonosulfate (PMS) for the degradation of phenol. The Fe-N-C/PMS system achieved a phenol degradation rate of 99.71%, which follows a first-order kinetic model, with the reaction rate constant of 0.1419 min−1. The phenol degradation rate remained above 92% in inorganic anions (Cl−, SO42−, HCO3−) and humic acid and the system maintained a 100% phenol removal rate over a wide pH range (3–9). The iron in the catalyst predominantly exists in the forms of Fe0and Fe3C, and Fe0, Fe2+/Fe3+are the main active sites that promote PMS activation during the reaction. Additionally, Fe-N-C has a large specific surface area (1041.36 m2/g). Quenching experiments and electron spin resonance (ESR) spectroscopy detected the active free radicals in the Fe-N-C/PMS system: SO4•−, •OH, O2•−, and1O2. The mechanism for phenol degradation was discussed, involving radical pathways (SO4•−, •OH, O2•−) and the non-radical pathway (1O2), in the Fe-N-C/PMS system activated by Fe0, Fe2+/Fe3+, sp2hybridized carbon, C-O/C-N, C=O, and graphitic nitrogen active sites. This study provides new insights into the synthesis of efficient carbon-based catalysts for phenol degradation and water remediation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Zhaoxu Li,Xinyi Luo,Meifang Luo,Yuan Qin,Chaozhong Guo,Yao Liu,Zhongli Luo
To design inexpensive carbon catalysts and enhance their oxygen reduction reaction (ORR) activity is critical for developing efficient energy-conversion systems. In this work, a novel Fe-N-C hybrid electrocatalyst with carbon nanolayers-encapsulated Fe 3 O 4 nanoparticles is synthesized successfully by utilizing the molecular-level confinement of graphitic C 3 N 4 structures via hemin biomaterial. Benefiting from the Fe-N structure prevalent on the carbon nanosheets and large mesopore-dominated specific surface area, the synthesized catalyst under optimized conditions shows excellent electrocatalytic performance for ORR with an E ORR at 1.08 V versus reversible hydrogen electrode (RHE) and an E 1/2 at 0.87 V vs. RHE, and outstanding long-term stability, which is superior to commercial Pt/C catalysts (E ORR at 1.04 V versus RHE and E 1/2 at 0.84 V versus RHE). Moreover, the low hydrogen peroxide yield (<11%) and average electron transfer number (~3.8) indicate a four-electron ORR pathway. Besides, the maximum power density of the home-made Zn-air battery using the obtained catalyst is 97.6 mW cm −2 . This work provides a practical route for the synthesis of cheap and efficient ORR electrocatalysts in metal-air battery systems.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Ting Huang,Jinhui Wei,Xiaoting Zhu,Enren Zhang
The development of microbial fuel cells (MFCs) into a new type of carbon-neutral wastewater treatment technology requires efficient and low-cost oxygen reduction reaction catalysts in air cathodes. The use of raw soybean powder was investigated for synthesizing Fe–N–C ORR catalysts in a sacrificial SiO 2 support method. ZnCl 2 etching in the synthesis was found to facilitate the formation of hierarchical porous structures of Fe–N–C catalysts. Fe–N–C(1-1) catalyst synthesized with an optimal soybean/ZnCl 2 mass ratio of 1:1 exhibited the highest ORR activity in air cathodes. The use of the obtained Fe–N–C(1-1) catalyst enables a maximum power production of ~0.480 mW cm −2 in MFCs, higher than commercial Pt/C (0.438 mW cm −2 ) with the same catalyst loading of 2 mg cm −2 . Long-term MFC operations demonstrated that the Fe–N–C synthesized from raw soybean have high stability and toxic tolerance, indicating that abundant low cost soybean biomass is a potential material for ORR catalyst development in MFC applications.
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高影响因子
Frontiers in Energy
·
2025
·
IF 6.2
Tang Wenbin,Xia Shuyue,Chou Haiwen,Zhao Jianan,Zhou Yi,Huang Qinghong,Yu Nengfei,Wu Yuping
The oxygen reduction reaction (ORR) plays a crucial role in key processes of fuel cells and zinc-air batteries. To enable commercialization, reducing the platinum (Pt) content and increasing the specific activity per unit mass is essential. A promising approach involves synthesizing of Fe-N-C precursors via the polyaniline (PANI) pathway, which ensures a uniform distribution of Fe-N-C species and facilitates the subsequent adsorption of platinum ions. This leads to the formation of Pt-Fe bimetallic alloys. The synergistic interaction between Pt and Fe-N-C sites promotes the homogeneous dispersion of Pt and the formation of smaller particle sizes, which in turn enhances intrinsic activity and stability of the catalyst. Notably, the Pt/Fe-N-C catalyst, featuring an ultra-low Pt loading of just 1.79 wt%, exhibits a remarkable doubling of mass activity compared to conventional catalysts. Moreover, zinc-air batteries using this catalyst achieve an impressive peak power density of 200 mW/cm 2 .
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RSC Advances
·
2016
·Vol. 6
·期 93
·90797-90805
·
IF 3.289
Jingjing Xi,Fang Wang,Riguo Mei,Zhijie Gong,Xianping Fan,Hui Yang,Liang An,Qixing Wu,Zhongkuan Luo
In this work, a graphene supported Fe–N–C composite catalyst, synthesized by pyrolysis of graphene oxide (GO), graphitic carbon nitride (g-C3N4), ferric chloride (FeCl3) and carbon black (Vulcan XC-72), was evaluated for oxygen reduction reaction (ORR) in acid media. The introduction of carbon black was to separate the graphene sheets to enhance the specific surface area and thus improve the catalytic activity of the catalyst. The experimental results showed that the composite catalyst could yield an average electron transfer number of 3.85 and its onset and half-wave potentials for acidic ORR were only 56 and 69 mV smaller than those of Pt/C (40 wt% Pt) catalyst, respectively. The as-prepared catalyst was applied in an acid direct methanol fuel cell as the cathode catalyst and a peak power density of 11.72 mW cm−2 at 30 °C was demonstrated when feeding the anode and cathode with a 1 M methanol solution and air, respectively, suggesting its promising application.
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高影响因子
RARE METALS
·
2026
·Vol. 45
·期 5
·e70350
·
IF 12.1
Lijuan Wang,Jie Hou,Wubo Wan,Yongjie Mo,Zhijian Liao,Shengkui Zhong,Linhua Zhu
en This link goes to a English section zh This link goes to a Chinese section Atomically dispersed iron–nitrogen–carbon (Fe-N-C) catalysts have emerged as promising alternatives for oxygen reduction reaction (ORR) owing to their highly atomic utilization. However, maintaining both Fe atomic dispersion and dense Fe-N x sites (typically below 2 wt%) in Fe-N-C catalysts is still a key challenge. In this investigation, a template (1,2-dicyanobenzene; DCB) assisted strategy has been reported to achieve hierarchically porous Fe-N/C DCB0.2 -900°C catalysts, which have atomically dispersed Fe-N 4 C active sites with a 5.45 wt% Fe loading and served for robust ORR. 1,2-dicyanobenzene containing abundant nitrogen source not only efficiently enhances the coordinated environment for dense Fe sites, but also facilitates the formation of a hierarchical porous structure in Fe-N/C DCB0.2 -900°C catalyst. Computational analysis demonstrated that template-assisted structural modification effectively reduces the energy barrier associated with *OOH intermediate formation while simultaneously adjusting the d-band center position of Fe-N 4 C coordination sites within the Fe-N/C DCB0.2 -900°C system. This optimization enhances the stabilization of oxygen-bearing intermediates and promotes accelerated kinetics of the ORR. Consequently, the Fe-N/C DCB0.2 -900°C exhibited a half-potential of 0.9 V versus RHE when evaluated in 0.1 M KOH electrolyte and achieved a peak power density of 220 mW cm −2 in a zinc–air battery, surpassing commercial Pt/C (0.88 V vs. RHE, 194 mW cm −2 ). Such methodology provides a new avenue for constructing dense metal active sites for achieving functional, but not limited to, ORR, catalysts and applications. 摘要 en This link goes to a English section zh This link goes to a Chinese section 原子分散的铁-氮-碳(Fe-N-C)催化剂因其高原子利用率,已成为很有前景的氧还原反应(ORR)替代催化剂。然而,在Fe-N-C催化剂中同时保持铁的原子分散性和密集的Fe-N x 位点(通常低于2 wt%)仍是一个关键挑战。在本研究中,我们报道了一种模板(1,2-邻苯二甲腈; DCB)辅助策略,以制备具有分级多孔结构的Fe-N/C DCB0.2 -900°C催化剂,该催化剂具有原子分散的Fe-N 4 C活性位点,铁负载量为5.45 wt%,可用于高效的ORR。含有丰富氮源的1,2 -邻苯二甲腈不仅能有效改善密集铁位点的配位环境,还有助于在Fe-N/C DCB0.2 -900°C催化剂中形成分级多孔结构。理论计算分析表明,模板辅助的结构修饰有效降低了与*OOH中间体形成相关的能垒,同时调整了Fe-N/C DCB0.2 -900°C体系中Fe-N 4 C位点的d带中心位置。这种优化增强了含氧化合物中间体的稳定性,并促进了ORR的动力学反应速度。因此,在0.1 M KOH电解质中测试时,Fe-N/C DCB0.2 -900°C的半波电位为0.9 V,在锌空气电池中实现了220 mW cm −2 的峰值功率密度,超过了商用Pt/C(0.88 V,194 mW cm −2 )。这种方法为构建密集的金属活性位点提供了新途径,可用于制备功能性催化剂(不仅限于ORR)及相关应用。
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高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Junhao Huang,Ruixue Shi,Andrei Ivanets,Alexander A. Ratko,Tatyana Kouznetsova,Haixin Wu,Xintai Su
Hexavalent chromium (Cr(VI)) contamination in water poses a significant threat to human health. In this work, Fe and N co-doped biochar (Fe-N-C) was fabricated from municipal sludge using urea as a nitrogen source via the acidification-one-step pyrolysis method. This approach overcame the low adsorption capacity of self-carbonated sludge and achieved high Cr(VI) removal efficiency. Batch experiments and characterization techniques were employed to investigate the synthesis mechanism of Fe-N-C and its Cr(VI) removal mechanisms. At a urea/sludge mass ratio of 0.5, Fe-N-C-0.5 demonstrated superior Cr(VI) adsorption capacity (205.92 mg g⁻¹), primarily governed by spontaneous monolayer chemisorption and intraparticle diffusion. The adsorption process was unaffected by coexisting ions, and it exhibited excellent regeneration stability as well as substantial potential for practical applications. In addition, Fe-N-C-0.5 exhibited high biosafety before and after Cr(VI) removal. Urea doping facilitated nitrogen incorporation and anchored free Fe³⁺, forming the Fe-N-C structure that promoted the transformation of Cr(VI) to Cr(III) through electrostatic adsorption, reduction, and cation-π interactions. These results suggest Fe-N-C is an effective adsorbent for Cr(VI)-contaminated wastewater treatment.
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高影响因子
Journal of Energy Storage
·
2026
·
IF 10.7
Hao Lu,Jiale Niu,Jingjing Xie,Xiu He,Weiming Wang,Zhengyi Fu,Zhaoyong Zou
The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are key cathode reactions in clean energy storage devices such as zinc–air batteries. However, their sluggish kinetics severely limit device efficiency and large-scale application. Currently, M–N–C catalysts are considered the most promising candidates, yet they still suffer from issues such as mass transport limitations and insufficient stability. Inspired by the dynamic regulation of organic–inorganic interfaces during the formation of biological materials, we developed a novel method using 1,3,5-trimethylbenzene (TMB) as a mediating molecule to dynamically regulate the organic-inorganic interface between templates and ZIF-8 precursors, achieving the micro-meso-macropores of ZIF-8, which synergistically enhanced mass transport and active site accessibility. Meanwhile, phosphorus doping modulated the electronic structure of the Fe centers, forming Fe-N-P active sites and thereby significantly enhancing both catalytic activity and stability. Electrochemical tests showed that HPZIF-8-FeNP 5 exhibited excellent ORR performance in alkaline medium, with a half-wave potential of 0.8595 V (vs. RHE), outperforming commercial Pt/C while demonstrating good methanol tolerance and cycling stability. Furthermore, the catalyst also showed promising OER activity, with an over-potential of 284 mV at 10 mA cm −2 . When applied in a zinc–air battery, the device delivered a high open-circuit voltage (1.52 V), a high power density (227.4 mW cm −2 ), and long-term cycling stability (>400 h), surpassing the Pt/C-RuO 2 benchmark. This work provides a new material design strategy to advance rechargeable zinc-air battery technology, enabling efficient and durable energy storage.
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