INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Fengxian Zhang,Ye Chen,Yang Liu,Xupo Liu,Shuyan Gao
Constructing highly efficient and durable non-noble metal modified carbon catalysts for oxygen reduction reaction (ORR) in the whole pH range is essential for energy conversion devices but still remains a challenge. Herein, the Fe/Fe 3 C nanoparticles and Fe-N X species anchored on the interconnected mesoporous carbon materials are fabricated through an economical and facile template-assisted polymerization-pyrolysis strategy. The catalyst exhibits unique features with the electronic interaction between Fe/Fe 3 C and Fe−N X , large specific surface area and high mesoporous structure as well as nitrogen doping in porous carbon skeletons, which can effectively catalyze ORR over the full pH range. In an alkaline electrolyte , the optimized catalyst displays favorable ORR performance with positive onset potential ( E onset = 0.91 V), half-wave potential ( E 1/2 = 0.83 V), long-term cycles stability and methanol tolerance, exceeding those for the commercial Pt/C. Furthermore, the prepared catalyst could be directly assembled into the alkaline Zn−air battery that exhibits the open-circuit voltage of 1.44 V, high power density of 96.0 mW cm −2 and long-term durability. Therefore, the template-assisted polymerization-pyrolysis strategy provides a promising route for designing high-performance non-noble metal decorated ORR electrocatalysts .
研究领域:
材料科学
·
电化学
·
能源转换技术
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Qin Wen,Dongxu Tian,Zequan Zeng,Fei Qi,Zhanggen Huang
Fe-N-C catalysts with magnetism were successfully synthesized through one-step heat treatment of ferrosoferric oxide and covalent organic frameworks composite (Fe 3 O 4 @COF) as heterogeneous catalysts for persulfate (PS) activation and 2,4-dichlorophenol (2,4-DCP) degradation. The morphologies, compositions and active sites were adjusted by changing the pyrolysis temperature. The catalyst prepared at 900 °C showed excellent activity with 2,4-DCP removal of 90% in 60 min, recycling convenience and regeneration stability. Large surface area (342 m 2 g −1 ) and hierarchical porous structure benefited PS activation. It was proved that the radical and non-radical mechanisms coexisted in Fe-N-C-900/PS system with the results of quenching and electrochemical experiments. Roles of graphitic N and Fe-N X were distinguished. Graphitic N and Fe-N X sites palyed an prominent part in the non-radical activation process , in which Fe-N X was closely related to the electron transfer activation mechanism. Density functional theory (DFT) calculation further verified that the Fe N 2 was the key site for PS activation. 2,4-DCP degradation was proved to be a toxicity-attenuation process according to the biotoxicity analysis. The effects of several operating parameters and degradation of different model pollutants were also systematically evaluated, and possible activation mechanism was proposed.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Yang Wang,Ye Chen,Ziwei Wang,Ping Li,Jianyun Zhao,Hongyang Zhao,Dan Li,Tianxi He,Yuantao Wei,Yaqiong Su,Chunhui Xiao
Developing non-precious metal-based catalysts as the substitution of precious catalysts (Pt/C) in oxygen reduction reaction (ORR) is crucial for energy devices. Herein, a template and organic solvent-free method was adopted to synthesize Fe, B, and N doped nanoflake-like carbon materials (Fe/B/N–C) by pyrolysis of monoclinic ZIF-8 coated with iron precursors and boric acid . Benefiting from introducing B into Fe–N–C, the regulated electron cloud density of Fe-N x sites enhance the charge transfer and promotes the ORR process. The as-synthesized Fe/B/N–C electrocatalyst shows excellent ORR activity of a half-wave potential (0.90 V vs 0.87 V of Pt/C), together with superior long-term stability (95.5% current density retention after 27 h) in alkaline media and is even comparable to the commercial Pt/C catalyst (with a half-wave potential of 0.74 V vs 0.82 V of Pt/C) in an acidic electrolyte. A Zn-air battery assembled with Fe/B/N–C as ORR catalyst delivers a higher open-circuit potential (1.47 V), specific capacity (759.9 mA h g −1 Zn at 10 mA cm −2 ), peak power density (62 mW cm −2 ), as well as excellent durability (5 mA cm −2 for more than 160 h) compared to those with commercial Pt/C. This work provides an effective strategy to construct B doped Fe–N–C materials as nonprecious ORR catalyst. Theoretical calculations indicate that introduction of B could induce Fe-N x species electronic configuration and is favorable for activation of OH∗ intermediates to promote ORR process.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
Materials
·
2020
·Vol. 13
·期 21
·4779
·
IF 3.057
Yuzhe Wu,Yuntong Li,Conghui Yuan,Lizong Dai
Introduction of both nitrogen and transition metal elements into the carbon materials has demonstrated to be a promising strategy to construct highly active electrode materials for energy shortage. In this work, through the coordination reaction between Fe3+and 1,3,5–tris(4–aminophenyl)benzene, metallosupramolecular polymer precursors are designed for the preparation of carbon flakes co-doped with both Fe and N elements. The as-prepared carbon flakes display wrinkled edges and comprise Fe3C nanoparticle and active site of Fe–Nx. These carbon materials exhibit excellent electrocatalytic performance. Towards oxygen reduction reaction (ORR), the optimized sample has Eonsetand Ehalf-waveof 0.93 V and 0.83 V in alkaline system, respectively, which are very close to that of Pt/C. This approach may offer a new way to high performance and low-cost electrochemical catalysts.Keywords:coordination;metallosupramolecular polymer;active site;carbon materials;oxygen reduction reaction
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Hao Han,Xiaomei Wang,Xu Zhang
Doping Fe N C catalysts with heteroatoms has been widely recognized as a most promising way to improve the electrocatalytic activity to achieve the replacement of Pt-based electrocatalysts for efficient oxygen reduction reaction (ORR). However, it is still a challenge to combine delicate control of the catalyst structure with heteroatom-doping to achieve optimal electrocatalytic efficiency. Herein, a strategy of combining chemical vapor deposition (CVD) with dual-template cooperative pyrolysis was rationally designed to synthesize the novel electrocatalyst with densely isolated single Fe atoms scattered on hierarchically ordered porous N and S codoped carbon (ISA-Fe/HOPNSC). The three-dimensional hierarchically ordered interconnected macro/mesoporous structure and uniform sulfur-doping make ISA-Fe/HOPNSC exhibit superb ORR performance in both alkaline and acidic electrolytes with a positive half-wave potential (0.920 V in 0.1 M KOH and 0.795 V in 0.5 M H 2 SO 4 ) as well as outstanding methanol tolerance and long-time stability. As cathode catalyst in Zn-air battery, ISA-Fe/HOPNSC also provides much better maximum power density (210.7 mW cm −2 ) and specific capacity (796.7 mAh g Zn −1 ) than those of Pt/C (112.6 mW cm −2 and 712.6 mAh g Zn −1 ). Remarkably, the synthesis strategy in this work proposes myriad opportunities for combining delicate control of the catalyst structure with heteroatom doping to synthesize high-performance ORR catalysts.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
ChemElectroChem
·
2021
·Vol. 8
·期 24
·4804-4809
·
IF 4.59
Ke Qin,Zhenye Zhu,Mingjie Yi,Shunyou Hu,Fei-Xiang Ma,Jiaheng Zhang
Graphical In a tangle : Benefiting from the unique hierarchical porous structures and abundant Fe−Nx active sites, the tangled Fe−N−C nanosheets prepared through a facile dopamine-coordination strategy can be utilized as high-performance oxygen reduction reaction electrocatalysts. Developing efficient, economical, and durable transition metal atom-dispersed catalysts to boost the sluggish oxygen reduction reactions (ORRs) is crucial for the practical metal-air batteries. Herein, a facile dopamine-coordination strategy was developed to obtain tangled Fe, N co-doped ultrathin carbon nanosheets (donated as tangled Fe−N−C nanosheets), which can be utilized as high-performance ORR electrocatalysts. Benefited from the unique hierarchical porous structures and abundant Fe−N x active sites, the tangled Fe−N−C nanosheets exhibited excellent ORR activity in alkaline medium with more positive half-wave potential (0.88 V vs. RHE) than 20 wt % Pt/C (0.84 V vs. RHE). Meanwhile, the tangled Fe−N−C nanosheets exhibit excellent long-term stability and good tolerance to methanol crossover. When applying the Fe−N−C nanosheets as the cathode catalyst for primary zinc-air batteries (ZABs), the assembled cells exhibit high open circuit voltage (∼1.43 V), high peak power density (∼89 mW cm −2 ) and large specific capacity of 801 mA h g −1 .
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Cheng Hou,Jiang Zhao,Libin Yang,Jiabin Chen,Xuefen Xia,Xuefei Zhou,Yalei Zhang
A single-atom Fe-N-C catalysts (Fe-N-C) was successfully prepared through a facile synthesis route using microalgae to drive hydrogen peroxide (H 2 O 2 )-based Fenton-like reactions. The detailed characterization analyses confirmed the simultaneous presence of Fe/Fe compounds and Fe-N x coordination sites in the optimal catalyst (Fe-N @ MBC) obtained through the pyrolysis of FeCl 3 ·6 H 2 O and Chlorella vulgaris . Surprisingly, when applied in H 2 O 2 -based advanced oxidation processes (AOPs), Fe-N @ MBC demonstrated excellent proficiency for both H 2 O 2 and O 2 activation, with the contribution of the original dissolved oxygen for sulfamethoxazole removal reaching up to 47.59%. The experiment and density functional theory (DFT) calculation results indicated that the Fe/Fe compounds significantly boosted the activity of Fe-N x by lowering the energy barrier of the reactive oxygen species formation and promoting the electron transfer between Fe-N x and the oxidants (H 2 O 2 and O 2 ). These findings provide new insights into the facile synthesis, rational design, and catalytic mechanisms of Fe-N-C used in H 2 O 2 -based AOPs.
研究领域:
环境科学
·
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 15
·7145-7157
·
IF 11.301
Jinling Xue,Yinshi Li,Jue Hu
It remains a major challenge to develop a facile method to prepare non-noble metal electrocatalysts with high activity and durability to drive the sluggish oxygen reduction reaction (ORR) for proton exchange membrane fuel cells (PEMFCs). Herein, a highly efficient bimetallic Zn/Fe@N-doped hierarchical porous carbon (Zn/Fe–N–C) catalyst derived from ZIF-8 and hemin (host–guest) was firstly reported by one-step thermal treatment. Fe2+ spatially separated by using the hemin guest in the ZIF-8 framework and hydrocarbon-branched chains form rich Fe–Nx active sites, and the evaporation of Zn2+ generates a highly porous structure in the Zn/Fe–N–C catalysts. Benefitting from this unique structure and composition, the resulting Zn/Fe2–N–C catalyst exhibits excellent ORR activities in both 0.1 M KOH (onset potential, Eonset = 1.08 V, and half-wave potential, E1/2 = 0.86 V vs. RHE) and 0.5 M H2SO4 media (Eonset = 1.04 V and E1/2 = 0.81 V), which are even comparable to those of the commercial Pt/C catalyst, and ranks among the top reported electrocatalysts. In addition, it also has outstanding long-term durability and good methanol resistance, much better than those of Pt/C in both acidic and alkaline media, which makes it one of the best non-noble alternatives of Pt-based catalysts for ORR electrocatalysis. This work highlights the potential to rationally design and fabricate high-performance ORR catalysts for fuel cell applications.
研究领域:
材料科学
·
电化学
·
催化
·
能源材料
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Mengxi Yin,Boya Fu,Tengfei Ren,Mingwei Wang,Xiaoxin Cao,Xia Huang,Xiaoyuan Zhang
Bioelectrochemical systems (BESs) are promising for future wastewater treatment towards carbon neutrality. Hemes, as the active center of outer-membrane c-type cytochromes, play an important role in anodic electron transfer. In this work, a biomimetic Fe–N x incorporated carbon membrane (Fe-NCM) mimicking the heme active center was proposed based on a nanocage confinement-electrospinning strategy and applied as the anode in BESs. The aligned carbon fibers with high electrical conductivity could serve as the electron “expressway” for swift electron transfer while the Fe–N x nexus served as the “gas station” and endowed the membrane anode with boosted redox activity. The Fe-NCM anode featuring great biocompatibility and electrochemical activity was conducive to microbe adhesion and biotic-abiotic interfacial interaction. The power output and chemical oxygen demand (COD) removal rate constant in the BES with this Fe-NCM anode reached 1406 ± 44 mW m −2 and 0.42 ± 0.01 h −1 under filtration operation mode, which were 156 % and 191 % those of the pristine carbon membrane. The introduction of Fe–N x species exerted a significant influence on the anodic biofilm property, composition and function, which were of importance to bolstering wastewater energy conversion. Metagenomics unveiled that simultaneous intensification of intracellular electron production and extracellular electron transfer processes was achieved in the Fe-NCM BES. The Fe-NCM anode with electroactive Fe–N x sites facilitated the biotic-abiotic interfacial interaction in BESs and highlighted the rational design of anodes for efficient wastewater treatment and energy conversion.
研究领域:
环境科学
·
生物技术
·
电化学
·
废水处理
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）