CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 23
·期 58
·14597-14603
·
IF 5.317
Xinghua Chen,Fei He,Yanfei Shen,Yiran Yang,Hao Mei,Songqin Liu,Toshiyuki Mori,Yuanjian Zhang
Graphical Interface effect : A study into the intrinsic role of carbon supports for Fe-N/C alternatives to Pt/C catalysts for oxygen reduction in fuel cells revealed that when immobilized on suitable support, the Fe−N/C demonstrated an improved mass J K that was comparable to that of Pt/C and higher than most reported M−N/C catalysts (see scheme). The mass kinetic current density (mass J K ) of most extensively reported M−N/C catalysts (M represents non-precious metal elements such as Fe, Co, and Cu), a potential alternative to noble metal catalysts in fuel cells, is poorer than that of commercial Pt/C. Thus, deep understanding of the intrinsic roles of carbon supports may contribute to the development of M−N/C catalysts from a practical point of view. Herein, the routinely used carbon supports, i.e. carbon black (CB) and carbon nanotubes (CNT) that have different morphology and crystallinity, were investigated to uncover the factors that affected the mass J K of Fe−N/C in electrocatalytic oxygen reduction. When immobilized on CB, the ionic liquids-derived Fe−N/C exhibited an enhanced mass J K (4.45 A g −1 at 0.80 V vs. RHE) by a factor of 2.14 times, comparable to that of Pt/C (5.79 A g −1 ) and higher than most reported M−N/C catalysts to our best knowledge. In contrast, the CNT support system showed no improvement. It was revealed that a compatible interface between the Fe−N/C precursors and the carbon supports was vital to ensure in-situ growth of a uniform catalyst layer on the supports during pyrolysis. This subsequently promotes the mass J K by exposing more embedded active sites and introducing favorable slit pores for effective mass-diffusion. This work would be promising to address the long-term overlooked challenge of the low mass J K of M−N/C catalysts in replacing noble-metal catalysts for practical fuel cell applications.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
PubMed
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 41
·19506-19511
·
IF 6.97
Ying Li,Tong Liu,Wenxiu Yang,Zhijun Zhu,Yanling Zhai,Wenling Gu,Chengzhou Zhu
Non-Pt catalysts with excellent performance regarding the oxygen reduction reaction (ORR) have aroused enormous interest in recent years. Herein, we propose a dual-template method to synthesize a multiscale porous Fe–N–C (FeNC) catalyst. SiO2 and Zn are used as co-templates to produce a multiscale porous structure. Chitosan and glutaraldehyde are used as building blocks to fabricate the frameworks of the hydrogel. After lyophilization and annealing treatments, FeNC aerogel with a multiscale porous structure could be obtained. The as-prepared FeNC catalyst annealed at 900 °C (FeNC-900) exhibits a larger electrochemically active surface area and an improved ORR activity compared to FeNC annealed at other temperatures. FeNC-900 shows a superior ORR performance in comparison with that of commercial Pt/C in terms of the onset potential and half-wave potential, i.e., 0.959 and 0.837 V, which are 28 mV and 10 mV higher than those of Pt/C, respectively. Multiscale porosity is responsible for the outstanding ORR performance of FeNC-900. The electron transfer number of FeNC-900 for the ORR was calculated to be 3.95, which is comparable with that of Pt/C. In addition, the FeNC-900 catalyst possesses an excellent long-term duration and anti-poisoning capacity against methanol crossover. All these results endow the FeNC catalyst with tremendous potential for use in fuel cells.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yuzhe Liu,Qi Li,Yuhan Liang,Junhao Liang,XuLei Sui,Zhenbo Wang
The non-precious metal Fe-N-C catalyst is regarded as a potential substitute for the precious metal catalysts for the oxygen reduction reaction (ORR) application. However, its catalytic activity and stability still fall short of those of the precious metal catalysts. Here, Fe-N-C catalyst with an ordered macroporous framework was achieved through using polystyrene (PS) as templates. The results indicate the particle size and structural orderliness of PS templates have great influence on the morphology and the catalytic performance of the obtained Fe-N-C catalysts. The optimized catalyst, derived from ordered PS with 200 nm, exhibits exceptional ORR activity in acidic media with a half-wave potential of 0.885 V (vs. RHE), surpassing commercial Pt/C (0.847 V) and Fe-N-C without PS counterparts (0.796 V), and superior mass activity (26.54 A g⁻¹, 0.8 V) and kinetic current density (14.7 mA cm⁻²,0.85 V), while maintaining outstanding durability under 30,000 potential cycles (18 mV loss). The catalyst, as the cathode in an H₂/O₂ fuel cell, exhibits a peak power density of 0.83 W cm⁻². This excellent activity arises from its regular morphology combined with ordered macroporous framework facilitating active site exposure and reactant diffusion. The regularly arranged template-induced structural ordering enhances the graphitization and integrity of carbon matrix during pyrolysis, promoting the stability. These findings establish a template-size-dependent design principle for non-precious metal catalysts, offering a viable pathway to balance activity-stability trade-offs in proton-exchange membrane fuel cells and related electrochemical energy technologies.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yangyang Liu,Fengdi Tu,Ziyu Zhang,Zigang Zhao,Pan Guo,Lixiao Shen,Yunlong Zhang,Lei Zhao,Guangjie Shao,Zhenbo Wang
Iron and nitrogen co-doped carbon (Fe/N/C) electrocatalysts have great potential to catalyze the kinetically slow oxygen reduction reaction (ORR). Unfortunately, the ORR performance of existing Fe/N/C catalysts is seriously hindered by the insufficient density and accessibility of the atomic Fe-N x moieties. Herein, the carboxylate (OAc) molecular scissor is proposed to tailor Fe doped zeolitic-imidazolate-framework-8 (ZIF-8) at atomic scale and construct a multi-dimensional concave Fe@NC catalyst structure (Fe@MNC-OAc). This molecular scissoring strategy imparts Fe@MNC-OAc with dense accessible active sites, multidimensional mass transfer pathways, hierarchical porous structure, and entangled carbon nanotubes network. Therefore, the tailored Fe@MNC-OAc electrocatalyst exhibits excellent ORR activity in acidic media with a half-wave potential of 0.838 V, which is comparable to state-of-the-art non-precious metal catalysts. When assembled as cathode catalyst in a H 2 -O 2 proton exchange membrane fuel cell, it delivers a peak power density of 903 mW cm −2 . This work provides a new approach to tailoring the catalyst architecture and improving the accessibility of active sites.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2021
·Vol. 13
·期 11
·2683-2690
·
IF 5.686
Xinxin Jin,Yan Xie,Junhong Fu,Chaoyue Zhao,Yinghao Xu,Yang Lv,Bingsen Zhang,Keju Sun,Rui Si,Jiahui Huang
Graphical ORR : We fabricated a FeSA/HNPC electrocatalyst with well atomically dispersed FeN 4 species. DFT calculations uncovered that the single-atomic FeN 4 sites within FeSA/HNPC electrocatalyst present in the configurations of pyrrole-N 4 −Fe are more favorable than those of pyridine-N 4 −Fe for boosting ORR performances. Atomically dispersed Fe−N−C electrocatalysts have displayed excellent catalytic performances towards the oxygen reduction reaction (ORR), while the identification of the genuine active sites remains a challenge. Herein, we report a Fe−N−C electrocatalyst of FeSA/HNPC featuring single-atomic FeN 4 sites on hierarchically N-doped porous carbon (HNPC), which shows a very competitive ORR activity in alkaline solution even at a low electrocatalyst loading of 0.2 mg cm −2 on the working electrode. A comparison of energy barriers in ORR reveals that the single-atomic FeN 4 active sites in FeSA/HNPC existing in the form of pyrrole-N 4 −Fe is more favorable than that of pyridine-N 4 −Fe for the enhanced ORR activity. Understanding the nature of FeN 4 active sites will greatly benefit the design of Fe−N−C electrocatalysts with highly effective ORR performances.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
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 .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xing Li,Lei Xing,Chunyu Zhang,Shudan He,Fanghua Liu,Zhen Chen,Huazhen Chang,Junhua Li
Catalytic solvent regeneration is widely considered a promising solution for addressing the intensive heat duty of amine-based carbon dioxide (CO 2 ) capture. This highly challenging application has motivated researchers to develop excellent catalysts with high activity and durability. In this study, we engineered active and durable Fe − N − C catalyst coated with high-graphitization carbon layers (labeled Phen − Fe − N − C) through a secondary thermal pyrolysis treatment. The multiple graphite layers and atomic metal sties were verified by experimental characterization and coordination structure analysis. The improved graphite layers further enhanced the activity of Fe − N − C sites, providing more acid sites for proton-electron transfer and C − N breaking during solvent regeneration (or CO 2 desorption). Thus, the maximal CO 2 desorption rate increased by 50 % when Fe − N − C was used compared with that of the blank case, and the rate further increased by 27 % when Phen − Fe − N − C was used. After 15 days of hydrothermal testing, the single Fe atom over the spent catalysts presented no significant aggregation or dissolution in the solvent, validating the durability of Phen − Fe − N − C. This work demonstrates a feasible and novel strategy to improve M − N − C materials for efficient and robust CO 2 desorption from amine solvents toward energy-saving CO 2 capture.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Qingtao Liu,Weihao Liu,Xin Wan,Weiwei Chen,Xiaozhi Liu,Xiaofang Liu,Jiaxiang Shang,Jungang Miao,Dong Su,Xin Sun,Jianglan Shui
Zeolitic imidazolate framework-8 (ZIF-8) is widely used as precursor for carbon-supported single-metal-atom catalysts (M–N–C), but typically yields amorphous carbon with poor stability in proton-exchange-membrane fuel cells (PEMFCs). Traditional methods would lose active site density while increasing the graphitization degree. Here, this study reports that ultra-small nano ZIF-8 can produce graphene-nanostacks-based Fe–N–C that has improvements on both activity and stability. First, anti-sintering nanoporous ZIF-8 (nano-ZIF8) particles are synthesized with unit size of 8 nm (the smallest so far) using a destruction-reconstruction strategy. In situ microscopy reveals that the volatilization of Zn has a decisive effect on the graphitization degree of ZIF-8 and such process is size-dependent. Nano-ZIF8 particles have completed Zn volatilization before graphitization process beginning, leading to graphene nanostacks. These nanostacks preferentially host edge-type FeN 4 sites, which have doubled intrinsic activity and much improved stability compared with conventional Fe−N−C. In PEMFC, the catalyst achieves an activity of 48.5 mA cm − 2 @0.9V iR -free , meeting the US Department of Energy 2025 activity target. In addition, quantitative analysis of active site density is conducted in PEMFC for the first time using nitrite stripping voltammetry. The unique graphitization behavior of nano-ZIF8 paves a new avenue for advancing M–N–C catalysts.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Chuanhui Geng,Qingguo Chen,Zhenzhen Li,Mei Liu,Zhi Chen,Hengcong Tao,Qiao Yang,Baikang Zhu,Lijuan Feng
In this study, we investigated the doping of Fe–N–C with ZnO (Fe–N–C@ZnO) to enhance its performance in the reduction of biological toxicity and degradation of enrofloxacin (ENR) in seawater. The steady-state/transient fluorescence analysis and free radical quenching test indicated an extremely low electron–hole recombination rate and the generation of reactive oxygen species in Fe–N–C@ZnO, leading to an improvement in the energy efficiency. We compared the ENR degradation efficiencies of Fe–N–C@ZnO and ZnO using both freshwater and seawater. In freshwater, Fe–N–C@ZnO exhibited a slightly higher degradation efficiency (95.00%) than ZnO (90.30%). However, the performance of Fe–N–C@ZnO was significantly improved in seawater compared to that of ZnO. The ENR degradation efficiency of Fe–N–C@ZnO (58.87%) in seawater was 68.39% higher than that of ZnO (34.96%). Furthermore, the reaction rate constant for ENR degradation by Fe–N–C@ZnO in seawater (7.31 × 10 −3 min −1 ) was more than twice that of ZnO (3.58 × 10 −3 min −1 ). Response surface analysis showed that the optimal reaction conditions were a pH of 7.42, a photocatalyst amount of 1.26 g L −1 , and an initial ENR concentration of 6.56 mg L −1 . Fe–N–C@ZnO prepared at a hydrothermal temperature of 128 °C and heating temperature of 300 °C exhibited the optimal performance for the photocatalytic degradation of ENR. Based on liquid chromatography–mass spectrometry analysis, the degradation processes of ENR were proposed as three pathways: two piperazine routes and one quinolone route.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 29
·11357-11364
·
IF 8.262
Teng Liu,Pingping Zhao,Xing Hua,Wei Luo,Shengli Chen,Gongzhen Cheng
A simple Zn/Fe bimetallic zeolitic–imidazolite framework (ZIF) carbonization method is developed to synthesize an Fe–N–C hybrid with hierarchical nitrogen-doped porous carbons crossed by carbon nanotubes. Both the specific ratios of Zn/Fe in the bimetallic metal–organic framework (MOF) precursors and the selected annealing temperature are essential for the formation of this unique hybrid structure with good conductivity and exposure of more active sites. The resulting FeNC-20-1000 hybrid electrocatalyst exhibits excellent oxygen reduction reaction (ORR) activity, with a half-wave potential of 0.770 V comparable to that of the commercial Pt/C catalysts in acidic media, and a half-wave potential of 0.880 V, ca. 50 mV more positive than that of Pt/C for ORR in alkaline solution. More importantly, the as-prepared Fe–N–C hybrid exhibits much more stability for the ORR in both acidic and alkaline solutions than Pt/C, which makes it among the best non-noble-metal catalysts ever reported for ORR under acidic and alkaline conditions.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Shuo Qin,Zongze Li,Boran Zhou,Bin Liu,Yuting Xue,Ruixue Zhao,Lirong Zheng,Zhengbo Chen,Xia Zuo
Overuse of benzoate as a preservative is bad for human health. Therefore, we need to achieve quantitative detection of benzoate. Colorimetric nanozyme sensors have garnered significant interest owing to their exceptional efficacy and affordability. In this article, Fe-N-C dodecahedral nanozymes with superior peroxidase-like catalytic activity are prepared using ZIF-8 as a precursor. Therefore, we construct a colorimetric sensor for benzoate detection with a detection limit of 0.33 μM through integrating the inhibitory impact of benzoate on D-amino acid oxidase activity with the Fe-N-C-catalyzed 3,3′,5,5′-tetramethylbenzidine (TMB)–H 2 O 2 system, and this reaction is completed within 10 min. It is noteworthy that a recovery rate of 96.8–109 % has been attained for the detection of benzoate in beverages.
研究领域:
食品安全
·
生物化学
·
纳米技术
✓ 已验证
产品关联
DOI
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.
研究领域:
能源材料
·
电化学
·
热能转换
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）