JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xin Kang,Jiancong Liu,Dongxu Wang,Chungui Tian,Honggang Fu
CO 2 hydrogenation to hydrocarbons under high space velocity is crucial for industrial applications, but traditional Fe-based catalysts often suffer from the low activity and poor stability. Herein, we report a new tandem catalyst system combining Pt/TiO 2 catalysts with Fe 3 C catalysts for the direct conversion of CO 2 into C 2 -C 4 hydrocarbons under high space velocity. The Pt/TiO 2 component promotes *CO intermediate production with an enhanced Reverse Water-Gas Shift (RWGS) reaction efficiency, providing a highly reactive species for the Fe 3 C catalyst to achieve Fischer-Tropsch synthesis (FTS). By maximizing the contact interface between the Pt/TiO 2 and Fe-based components through a granule mixing configuration, we achieve significant enhancements in both CO 2 conversion rate (24.0 %) and C 2 -C 4 hydrocarbons selectivity (51.1 %) under the gaseous hourly space velocity (GHSV) of 100000 mL g cat −1 h −1 . Besides, excellent stability is achieved by the tandem catalysts with continuous catalysis for up to 80 h without significant decrease in activity. Through modulation of the reduction states of iron oxide, we effectively tune the composition of Fe-based catalyst, thereby tailoring the product distribution. Through this work, we not only offer a promising avenue for reducing CO 2 for efficient CO 2 utilization but also highlight the importance of catalyst design in advancing sustainable chemical synthesis.
研究领域:
催化化学
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环境科学
·
能源化学
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产品关联
DOI
PubMed
高影响因子
Materials Today Energy
·
2022
·
IF 9.257
Quan Zhou,Yue Yang,Qitong Ye,Tong Xue,Mudong Tu,Yipu Liu,Hua Li,Xiang-Hui Yan,Zhong-Li Zou,Bei-Ping Wang,You-Jun Lu,Feng-Lan Han
Combining catalytic active materials with nitrogen-doped carbon structure has been an effective strategy for designing high-performance electrocatalysts , where N species plays a vital role in modulating the electronic structure of composite material. The N dopant in the carbon structure exists in different states, but it has been ambiguous which type of N structure contributes the most to the overall catalytic activity. Here, Fe 3 C nanoparticles embedded in graphitic nitrogen-dominated carbon framework (Fe 3 C@NC) has been successfully fabricated from Fe@ZIF-8 and exhibits excellent oxygen reduction reaction (ORR) activity and stability. Experiments and theoretical calculations confirm the interaction between Fe 3 C and N-doped carbon. Moreover, graphitic nitrogen is proved to exhibit the highest promotion contribution among different N states, which can effectively reduce the energy barrier of the potential determining step (from O 2 to ∗OOH) for ORR. The Fe 3 C@NC composite is applied as the air cathode in a Zn-air battery, which shows a high E OCV (open-circuit voltage) of 1.48 V, a power density of 155.6 mW/cm 2 , and a specific capacity of 798 mAh/g Zn . This work suggests the synergy of Fe 3 C, N species, and carbon layer in promoting the performance of ORR catalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2024
·
IF 8.1
Yihui Zhou,Jin Qian,Zhe Qiang,Weiqing Kong,Changhuai Ye,Meifang Zhu
Heterogeneous interfaces are crucial for enhancing the polarization loss in composite materials, thereby improving microwave absorption capabilities. However, creating well-defined multiple heterogeneous interfaces essential for optimal absorber performance presents a significant challenge. Herein, Fe/Fe 3 C@C magnetic-carbon composites featuring Fe-Fe 3 C-C multiple heterogeneous interfaces were fabricated through in-situ growth of Fe 3 O 4 on polydopamine nanospheres, followed by thermal reduction and carbonization. Owing to the controllable Fe-Fe 3 C-C multiple heterointerface design, the outer-layer magnetic components not only significantly improve impedance matching but also enhance the interface polarization loss. The optimized Fe/Fe 3 C@C-9–1 composite exhibits excellent microwave absorption performance, achieving a minimum reflection loss (RL min ) of −64.4 dB and a broad effective absorption bandwidth (EAB) of 6.0 GHz at a thin matching thickness of only 1.5 mm, surpassing neat carbon nanospheres and most magnetic-carbon materials. Additionally, simulations conducted using Computer Simulation Technology (CST) demonstrate that the Fe/Fe 3 C@C-9–1 coating significantly reduces radar cross-section (RCS), with values below −20 dB across nearly the entire frequency range of 2–18 GHz, highlighting its potential for radar stealth applications. This work provides a simple yet effective approach for tuning the interface properties of carbon-based materials, underscoring the promise of Fe-Fe 3 C-C multiple heterogeneous interfaces in the development of broadband, thin microwave absorbers.
研究领域:
材料科学
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电磁学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 36
·20614-20623
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IF 10.733
Wei Kou,Guohui Chen,Yang Liu,Weixin Guan,Xiangcun Li,Ning Zhang,Gaohong He
To realize an Al-free cathode and to push forward the Li–S battery technology for practical applications, a multifunctional three-layer-structured Fe3C/C membrane was prepared at a large-scale via a facile phase-inversion method. The scalable yet flexible self-supporting Fe3C/C membrane is an ideal Al foil-free cathode material for high-energy and long cycling Li–S batteries. The conductive dense layer of the Fe3C/C membrane can replace the Al foil as a current collector and the finger-like macropores can host most of the sulfur active material (1.5–3.0 mg cm−2), thus buffering the volume expansion of the sulfur species and facilitating the ion/electrolyte transport for fast reaction kinetics; meanwhile, the sponge-like pores in the top layer of the composite membrane enable further S slurry loading. Density functional theory simulation (DFT) and Li2S6 adsorption measurements reveal that the doped Fe3C species in the composite membrane could effectively immobilize the S species and suppress the shuttle effect of the soluble polysulfides (LiPSs). The rationally designed Fe3C/C membrane cathodes could deliver a capacity of ∼601 mA h g−1 at 1C after 200 cycles even at a high sulfur loading of 3.4 mg cm−2, with a high areal capacity of 2.1 mA h cm−2. The cell with the sulfur loading of 3.4 mg cm−2 delivered a gravimetric energy density and volumetric energy density of 850 W h kg−1 and 1223 W h L−1, respectively. The self-supporting membrane cathode with simultaneous commercial S filling and S/C slurry coating provides an alternative sulfur loading approach for battery assembly, thus presenting a useful strategy for practical applications in high energy-density and long cycling Li–S batteries.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2024
·Vol. 14
·期 10
·687
·
IF 3.8
Na Zhang,Yudong Huo,Chun Pei,Ying Zhang,Lijie Xu,Lu Gan
Percarbonate (SPC) as a promising substitute for liquid H2O2has many advantages in the application of in situ chemical oxidation (ISCO). Developing efficient, cost effective and environmentally friendly catalysts for SPC activation plays the key role in promoting the development of SPC-based ISCO. Herein, the walnut shell biomass was combined with ferric nitrate for the catalytic synthesis of Fe3C@biochar composite (Fe3C@WSB), which demonstrated high efficiency in activating SPC for the removal of diclofenac (DCF). The Fe3C showed average crystallite size of 32.6 nm and the composite Fe3C@WSB demonstrated strong adsorptivity. The prepared Fe3C@WSB could activate both SPC and H2O2with high efficiency at ca. pH 3 with extremely low leaching of iron, while in a weak acidic condition, higher efficiency of DCF removal was obtained in the Fe3C@WSB/SPC process than in the Fe3C@WSB/H2O2process. Moreover, the Fe3C@WSB/SPC and Fe3C@WSB/H2O2processes did not show significant differences when supplied with varying amounts of catalyst or oxidant, but the Fe3C@WSB/SPC process exhibited stronger capability in dealing with relatively highly concentrated DCF solution. Based on quenching experiments and electron spin resonance (ESR) analysis, heterogeneous activation of SPC was assumed as the dominant route for DCF degradation, and both the oxidation by radicals, including •OH, •O2−and CO3•−, combined with electron transfer pathway contributed to DCF degradation in the Fe3C@WSB/SPC process. The cycling experiment results also revealed the stability of Fe3C@WSB. This work may cast some light on the development of efficient catalysts for the activation of SPC.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Guangjun Gou,Yu Liu,Qi Wan,Wanlu Hua,Xiaoli Xie,Bin Zhu,Zhen Tao
Three-dimensional (3D) porous carbon-based materials are commonly considered to be a hopeful microwave absorbing materials owing to their lightweight and broadband absorption. However, the structure between dissipation mechanism is still not clear. Therefore, in this work, the nitrogen-doped porous Fe 3 C@C nanocomposites derived from Fe(NO 3 ) 3 ·9 H 2 O and polyvinyl pyrrolidone (PVP) were fabricated through pre-blowing followed by in situ carbonization method with various temperatures. The obtained material treated at 600 °C, which the content of N was 4.07 %, exhibits the most excellent microwave absorption (MA) property with the minimal reflection loss of − 63.1 dB at 5.0 GHz while the matching thickness is 4.6 mm. The MA performance of the composite is originated from the synergy of magnetic-dielectric loss and improved interfacial polarization. This research provides a way to prepare high-property MA absorbers.
研究领域:
材料科学
·
电磁学
✓ 已验证
产品关联
DOI
高影响因子
DIAMOND AND RELATED MATERIALS
·
2023
·
IF 4.1
Yi Chen,Rong Qiang,Yulong Shao,Xiao Yang,Qian Ma,Rui Xue,Bowen Chen,Shijiang Feng,Fangjie Ren,Yuancheng Ding,Lijuan Sun,Zheng Guo,Zishuo Ma,Zihan Liu,Xinyu Chen
Porous carbon materials typically exhibit excellent microwave absorption performance and lightweight characteristics, providing a positive significance for controlling the composites weight. This work employed a one-step method, and in situ growth techniques to fabricate a foam-structure Fe 3 C/Fe/C with a density of only 0.142 g/cm 3 . The carbon skeleton encapsulates Fe 3 C/Fe nanoparticles to slow down its oxidation in the natural environment. Remarkably, the Fe 3 C/Fe/C composite achieves an impressive effective bandwidth of 5.73 GHz with a 2.2 mm thickness and only 10 wt% filling ratio. The outstanding performance can be ascribed to the enhanced interfacial polarization caused by high porosity. Additional nitrogen doping provides active sites to enhance dipole polarization. Additionally, after in-depth analysis of the various magnetic loss mechanisms present in Fe 3 C/Fe/C, we have revealed the promotion of introducing magnetic nanoparticles on the microwave absorption performance of foam-like carbon. This work provides an effective reference for reducing the weight of microwave absorbers, simplifying preparation methods, and understanding the mechanisms of magnetic nanoparticles in foam-like carbon.
研究领域:
材料科学
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电磁学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2019
·Vol. 30
·期 15
·14573-14579
·
IF 2.195
Teng Zhen,Zeng Sifan,Feng Wanlin,Zhu Lini,Tan Yongqiang,Han Xiaochun,Chen Chen,Zhang Haibin
Fe-Fe 3 C@C composites are successfully synthesized via a facile pyrolysis process. Experimental results indicate that Fe-Fe 3 C nanoparticles are closely parceled among amorphous carbon and exhibit a core–shell structure. The obtained materials display excellent microwave absorption performance with an optimal reflection loss of − 35.6 dB at 17.2 GHz, and an effective absorbing bandwidth of 4 GHz (from 12.4 to 16.4 GHz) with the coating thickness of 2 mm. The magnetic loss derived from Fe core and dielectric loss on carbon materials as well as a good impedance matching are believed to play decisive roles for this favorable microwave absorbing properties. The composites are considered to be good candidates for microwave absorption applications.
研究领域:
材料科学
·
电磁学
✓ 已验证
DOI
高影响因子
Heliyon
·
2024
·
IF 3.4
Jun Dong,Qiqi Jiao,Hao Wang,Hong Wang,Yi-ke Ren
The shortcomings of precious metal based catalysts have limited the development of novel energies. So, developing low-cost and high performance transition metal based catalysts is one of the most feasible way to substitute the precious metal based catalysts. In all of the developed catalysts for oxygen reduction reactions (ORR), the iron-based nitrogen doped carbon nanotube (N-CNT) show great promise. In this paper, N-CNT with Fe 3 C encapsulated based catalysts (Fe 3 C@N-CNT) were synthesized. The encapsulation structure of Fe 3 C@N-CNT was confirmed by HAADF-STEM, XANES, XPS, XRD, SEM and other methods. XANES tests show that the doped nitrogen of Fe 3 C changed the length of Fe-C bond and furtherly influenced the electron transfer between encapsulated Fe 3 C and outer layer N-CNT. Electrochemical tests showed that the half-wave potential and onset potential ORR of 750 °C calcined Fe 3 C@N-CNT were 90 mV higher than that of 20 wt% Pt/C. The additional electric field between Fe 3 C and N-CNT modulated the C-N bond of surface N-CNT and enhanced the catalytic performance for ORR. This paper reveal that constructing encapsulated additional electron providing center is an effective way to design high performance catalysts.
研究领域:
材料科学
·
电化学
·
催化材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 19
·7594-7608
·
IF 10.182
Yuanyuan Wang,Linlin Zhang,Yongjian Niu,Dong Fang,Jiao Wang,Qingxiao Su,Cheng Wang
Clear structure–performance relationships are helpful for the design of efficient catalysts and the understanding of reaction mechanisms. The electrocatalytic nitrate reduction reaction (NO3RR) offers a sustainable route to ammonia (NH3) synthesis and nitrate mitigation. However, it suffers from poor nitrate adsorption, low NH3 selectivity and sluggish reaction kinetics. Herein, N-doped carbon nanosheets supported Fe3C nanoflakes featuring large surface areas (860.024 m2 g−1) were prepared. Their NO3RR performances showed volcano-like relationships with the Fe3+/Fe2+ ratios and d-band centers. At −0.5 V, the NH3 yield, faradaic efficiency, selectivity and current density reached 1.19 mmol h−1 mg−1, 96.7%, 79.0% and 85.6 mA cm−2, respectively, exceeding most reported results. Such exceptional performances mainly originated from the optimized electronic structures that boosted nitrate adsorption and reaction kinetics (Tafel slope: 56.7 mV dec−1). Mechanistic investigations revealed a NO3− → NO2− → NH3 reaction pathway with the chemical process following the fast electron transfer process as the rate-determining step.
研究领域:
电催化
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2016
·
IF 0
Ruizhong Zhang,Wei Chen
Fe 3 C-functionalized three-dimensional (3D) porous nitrogen-doped graphite carbon composites (Fe 3 C/NG) were synthesized via a facile solution-based impregnation and pyrolysis strategy using the commercially available melamine foam and FeCl 3 as precursors. The structural characterizations confirmed that Fe 3 C nanoparticles with an average core size about 122 nm were assembled on the surface of the carbonized melamine foam (CMF) skeletons. The electrochemical measurements demonstrated the superior electrocatalytic activity of the advanced Fe 3 C/NG composite for hydrogen peroxide reduction reaction in 0.1 mol/L PBS electrolyte and the limit of detection of H 2 O 2 is estimated to be 0.035 mmol/L at a signal-to-noise ratio of 3 with a wide linear detection range from 50 μmol/L to 15 mmol/L ( R 2 = 0.999). Compared with the pure CMF, the Fe 3 C/NG exhibited higher catalytic activity , more stable response, lower detection limit, higher selectivity and a wider detection range, which could be attributed to the synergic effect between the two types of active sites from the iron carbide species and the nitrogen-doped graphite carbon. Meanwhile, the large surface area, high conductivity and the improved mass transport from the 3D porous material can also promote the electrochemical sensing performance. Moreover, the Fe 3 C/NG-based electrochemical sensor showed high anti-interference ability and stability for H 2 O 2 detection. Thus, the novel and low-cost Fe 3 C/NG composite may be a promising alternative to noble metals and offer potential applications in various types of electrochemical sensors, bioelectronic devices and catalysts.
研究领域:
材料科学
·
分析化学
·
生物医学工程
✓ 已验证
产品关联
DOI
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 14
·7218-7223
·
IF 3.43
Mengyao Lv,Haichuan Guo,Hangjia Shen,Jun Wang,Jiacheng Wang,Yuichi Shimakawa,Minghui Yang
A key challenge in carrying out an efficient oxygen reduction reaction (ORR) is the design of a highly efficient electrocatalyst that must have fast kinetics, low cost and high stability for use in an energy-conversion device (e.g. metal–air batteries). Herein, we developed a platinum-free ORR electrocatalyst with a high surface area and pore volume via a molten salt method along with subsequent KOH activation. The activation treatment not only increases the surface area to 940.8 m2 g−1 by generating lots of pores, but also promotes the formation of uniform Fe3C nanoclusters within the atomic dispersed Fe–Nx carbon matrix in the final material (A-FeNC). A-FeNC displays excellent activity and long-term stability for the ORR in alkaline media, and shows a greater half-wave potential (0.85 V) and faster kinetics toward four-electron ORR as compared to those of 20 wt% Pt/C (0.83 V). As a cathode catalyst for the Zn–air battery, A-FeNC presents a peak power density of 102.2 mW cm−2, higher than that of the Pt/C constructed Zn–air battery (57.2 mW cm−2). The superior ORR catalytic performance of A-FeNC is ascribed to the increased exposure of active sites, active single-atom Fe–N–C centers, and enhancement by Fe3C nanoclusters.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子