JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Qiulin Li,Heng Liu,Long-Cheng Zhang,Hao Chen,Hongjiu Zhu,Yuanke Wu,Maowen Xu,Shu-Juan Bao
Fe-N and pyridinic-N generally are considered the active sites of Fe-N-C catalyst. In this featured work, small uniform Fe/N-rich polymer spheres are selected to prepare the Fe-N-C catalyst and study how the sintering atmosphere (NH 3 , Ar, and H 2 ) to engineer their products. The findings reveal that the sintering atmosphere greatly affected not only the composition , aggregate state, and morphology of Fe, but also the graphitization degree and pore structure of carbon. In addition, XPS results suggest that Fe-N-C-NH 3 possesses the highest Fe-N and pyridinic-N content. Combining its abundant pores, high graphitization, and large specific surface area, the catalyst obtained in NH 3 atmosphere delivers best ORR catalytic performance (E 0 = 0.97 V, E 1/2 = 0.85 V vs RHE), which is even comparable to commercial Pt/C (E 0 = 0.97 V, E 1/2 = 0.83V vs RHE). Moreover, the catalyst exhibits greater stability and methanol resistance than those of Pt/C.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2019
·
IF 4.914
Hao Wang,Xiaohao Liu,Guangyue Xu,Ziwei Guo,Ying Zhang
ABSTRACT Owing to Fe being the most abundant and least expensive transition metal on the earth, the utilization of Fe-based catalysts for catalytic hydrogenation has attracted worldwide attention. In this work, a series of N-doped C supported Fe catalysts (Fe-N-C) were prepared by co-pyrolysis of cellulose and ferric chloride under ammonia atmosphere. Characterization methods such as elemental analysis, atomic absorption spectroscopy, nitrogen adsorption-desorption isotherms, transmission electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were carried out to explore the physicochemical properties of the catalysts. Using hydrogenation of nitrobenzene as a model reaction, the catalysts prepared at different pyrolysis temperatures displayed different activities. Fe-N-C-700 exhibited the best activity among these catalysts, with the yield of aniline being up to 98.0% under 5 MPa H 2 at 120 °C after 12 h. Combined with the results of catalyst characterization and comparative tests, the transformation of Fe species and the generation of N-doped C, especially graphitized N-doped C, in the catalyst may be the main factors affecting the activity. A kinetic study was carried out and the apparent activation energy was obtained as 31.53 kJ/mol. The stability of the catalyst was also tested and no significant decrease in the activity was observed after 5 runs.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Feng-Di Tu,Zi-Yun Wu,Pan Guo,Li-Xiao Shen,Zi-Yu Zhang,Yun-Kun Dai,Miao Ma,Jing Liu,Bin Xu,Yun-Long Zhang,Lei Zhao,Zhen-Bo Wang
Platinum group metal (PGM)-free catalysts represented by nitrogen and iron co-doped carbon (Fe-N-C) catalysts are desirable and critical for metal-air batteries , but challenges still exist in performance and stability. Here, cerium oxides (CeO x ) are incorporated into a two-dimensional Fe-N-C catalyst (FeNC-Ce-950) via a host-guest strategy. The Ce 4+ /Ce 3+ redox system creates a large number of oxygen vacancies for rapid O 2 adsorption to accelerate the kinetics of oxygen reduction reaction (ORR). Consequently, the as-synthesized FeNC-Ce-950 catalyst exhibits a half-wave potential ( E 1/2 ) of 0.921 V and negligible decay (<2 mV for Δ E 1/2 ) after 5,000 accelerated durability cycles, significantly outperforming most of ORR catalysts reported in recent years and precious metal counterparts. When applied in a zinc-air battery, it demonstrates a peak power density of 175 mW cm −2 and a specific capacity of 757 mAh g Zn −1 . This study also provides a reference for the exploration of Fe-N-C catalysts decorated with variable valence metal oxides .
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
产品关联
DOI
PubMed
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
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Zhenyu Yan,Xiuyun Zhao,Chenkai Zhong,Wenyu Gao,Yujie Feng,Jia Liu
FeNx sites show significant superiority in the degradation of antibiotic contaminants, but there are difficulties in successfully constructing highly dispersed FeNx sites. In this work, Fe-N/C catalysts doped with hierarchical ordered pores structure and FeNx active sites were prepared by metal node exchange strategy. Among them, Fe-N/C-2 had more excite species for peroxymonosulfate (PMS) owing to the synergy between Fe and N coordination, which achieved 89.36 % tetracycline (TC) removal rate within 20 min, and its reaction kinetic ( k = 0.245 min −1 ) is 7.66 times more than original PMS system. Moreover, the material exhibited excellent activation performance in a variety of complex water environments, such as the coexistence of multiple anions, strong acids and alkalis (pH = 2.90 ∼ 10.73), and natural organic matter interference. Chemical bond detection confirmed the successful formation of FeNx sites, free radical trapping experiments showed that FeNx was the main catalytic site, and 1 O 2 was the main active component. Furthermore, the reaction principle of the FeNx site catalyzing the production of 1 O 2 from PMS was revealed in detail through mechanism exploration. Next, the probable pathways of TC decomposition were elaborated in terms of the intermediates identified by Liquid Chromatograph Mass Spectrometer (LC-MS). This study emphasized the significant potential of synthesizing Fe-N/C catalysts with activated FeNx sites, elucidated mechanism of FeNx in PMS activation, and confirmed its feasibility in TC degradation.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Tingting Xiang,Qingchao Zhu,Tanyu Zhou,Chenglong Chen,Ruibo Wang,Tieyu Hu,Bing Li,Ziwei Xu,Juan Yang
Graphical Fe−N−C catalysts, doped with phosphorus, show improved ORR activity. Fe-NPC catalyst exhibits high metal loading, excellent ORR performance (onset potential of 1.00 V, half-wave potential of 0.864 V), and promising application in Zn-air batteries (758.8 mAh g −1 Zn ). DFT calculations reveal that phosphorus enhances O 2 activation and reduces the energy barrier for the rate-determining step. Atomically dispersed iron and nitrogen co-doped carbon materials (Fe−N−C) represent promising non-precious metal catalysts for the oxygen reduction reaction (ORR), offering potential alternatives to noble metal-based benchmarks. In our study, we investigated the influence of phosphorus doping on the catalytic activity of Fe−N−C. The experimental research demonstrate that the doping of phosphorus significantly enhances the ORR activity. Specifically, the resulting Fe-NPC exhibits high metal loading and excellent ORR activity in 0.1 M KOH with an onset potential of 1.00 V and a half-wave potential of 0.864 V. Density functional theory (DFT) simulations reveal that phosphorus improves the electrocatalytic activity by activating O2 molecules and reducing the energy barrier (the hydrogenation reaction *OH→H2O) of the rate-determining step. Furthermore, Fe-NPC exhibits promising application prospects as an air cathode in Zn-air batteries, delivering a high maximum discharge power density of 180.3 mW cm −2 and outstanding discharge specific capacity (758.8 mAh g −1 Zn ) at a discharge current density of 10 mA cm −2 .
研究领域:
材料科学
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电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
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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
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电化学
·
热能转换
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2019
·Vol. 3
·期 12
·3455-3461
·
IF 4.912
Bomin Feng,Xiuju Wu,Yanli Niu,Wei Li,Yunxi Yao,Weihua Hu,Chang Ming Li
Fe/N–C catalysts show great potential for the oxygen reduction reaction (ORR) but their catalytic activity should be further improved for practical application. Here, we report a high performance Fe/N–C hollow sphere with excellent ORR activity in both alkaline and acidic solutions. It is synthesized via pyrolysis of a melamine/Fe-incorporated polydopamine nanosphere precursor at 800 °C in an argon atmosphere. The N-rich melamine in the precursor affords abundant N dopants to form dense Fe–Nx active sites and also facilitates the formation of micropores in the catalyst via the gasification effect, together improving the ORR activity. The as-reported Fe/N–C catalyst outperforms the Pt/C catalyst in basic media (45 mV more positive half wave potential), approaches the Pt/C catalyst in acidic media (55 mV lower half wave potential), and exhibits impressive performance in Zn–air primary batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Meng Cheng,Junhao Liu,Hao Jiang,Chunling Li,Shuangqing Sun,Songqing Hu
In view of the critical importance of oxygen to corrosion evolution, to starve corrosion via depleting oxygen in coatings is a promising strategy. In this work, a novel nanocatalytic anticorrosion concept is proposed to design new coating with outstanding corrosion resistance . Different from the passive barrier of traditional coatings and self-repair after corrosion of current stimuli-feedback coatings, such coating could spontaneously eliminate internal diffused oxygen and greatly suppress the corrosion process. As a proof of concept, single-atom Fe-N-C electrocatalyst with isolated FeN 4 active sites is synthesized by a simple confined carbonization method, exhibiting excellent oxygen reduction performance (E 1/2 = 0.902 V). In composite coating , the evenly dispersed Fe-N-C compensates for the coating defects and serves as oxygen scavengers, which could actively adsorb and consume ambient oxygen, thereby preventing oxygen penetration to the metal substrate surface, eliminating the oxygen contribution to corrosion and significantly boosting the anticorrosion performance of epoxy coating. This in-situ mediation for oxygen in coating prevents metal substrate from receiving new supply of oxygen, while imparting active anticorrosion property to the coating.
研究领域:
材料科学
·
腐蚀科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Qi Sun,Zhaoyang Wang,Min Zhou,Jiantao Li,Ruihu Lu,Yuhan Wang,Xiaobin Liao,Yan Zhao
Fe-N-C catalysts have been recognized as the most satisfactory candidates alternatively to Pt-based catalysts for oxygen reduction reaction (ORR). However, fine-tailoring of their intrinsic ORR catalytic activity still remains a great challenge due to the inferior accessibility and intrinsic activity of FeN x moieties. Herein, one order of magnitude activity enhancement of pristine Fe-N-C through cooperating with nitrogen-doped carbon micro-flower is achieved. The axial coordination effect between Fe active center and nitrogen atoms in support can break the electronic distribution symmetry of FeN x moieties and induce the electron delocalization on Fe active center and the electron localization on N, respectively, which favor the adsorption behavior of *OH intermediate. As a result, the catalyst exhibits a remarkable half-wave potential of 0.9 V and a high kinetic current density of 74.04 mA cm −2 at 0.85 V. In addition, when utilized as a cathode catalyst of liquid Zn-air batteries (ZABs), it possesses excellent electrochemical performance, for example, a high open circuit voltage (OCV) and peak power density of 1.59 V and 170.09 mW cm −2 , respectively. This work provides a new understanding into the activity enhancement mechanism of Fe-N-C catalysts, and inspires electronic delocalization of active sites for adjusting catalytic activity.
研究领域:
材料科学
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电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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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
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
危险品化学品经营许可证（带存储）