JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Dawei Liu,Bin Wang,Katam Srinivas,Bo Yu,Xin Chen,Fei Ma,Xinqiang Wang,Xiaojuan Zhang,Dongxu Yang,Yuanfu Chen
It is still challenging but essential to synthesize non-noble catalysts with rich and uncovered catalytic active sites towards oxygen reduction reaction (ORR). And the limited research of the ORR properties of FeN x atom clusters also hinders their practical implementations. Here, we report a two-dimensional (2D) non-precious ORR catalyst constructed by abundant and fully exposed FeN x atom clusters anchored on nitrogen-doped graphene nanosheets (Fe-N-C/NG), which derives from three-dimensional (3D) ZIF-8, 2D graphene oxide nanosheet, and ferrocene. The optimized Fe-N-C/NG delivers outstanding ORR activities ( E onset = 0.97 V, E 1/2 = 0.84 V, J d = 5.48 mA cm −2 ), excellent Tafel slope (57.7 mV dec −1 ), remarkable long-term durability, and strong methanol tolerance in an alkaline electrolyte . Its superior catalytic activity is possibly attributed to its unique conversion of nanoarchitecture and the synergistic effects: the change of morphology effectively utilizes the advantages of 2D graphene oxide and 3D ZIF-8, which guarantees sufficient and reachable active sites; the 2D porous nanoarchitecture of Fe-N-C/NG promotes the ion diffusion and mechanical stability; both the FeN x atom clusters and N-doped graphene nanosheets facilitate the catalytic activity. This work introduces an innovative strategy to rationally design the nanoarchitecture and facilely synthesize nonprecious ORR catalysts with sufficient and uncovered active sites for high efficiency and durability.
研究领域:
材料科学
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电化学
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催化
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2026
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IF 7.8
Zhenzhen Wu,Xiaoyu Wu,Wenting Liu,Songfeng Liang,Jiaming Luo,Mengyang Li,Yang Wang
Zinc-air batteries, widely regarded as a frontrunner in sustainable energy storage solutions, struggle with performance constraints stemming from the insufficient activity and durability of bifunctional oxygen electrocatalysts. This research presents a composite catalyst (FeCo@Fe-N-CNTs) synthesized through a straightforward in situ growth method, effectively integrating FeCo alloys with Fe single atoms incorporated in nitrogen-doped carbon nanotubes (N-CNTs). Theoretical and experimental studies show that FeNx atoms weaken the interaction between active iron sites and reactants, enhancing the reaction energy optimization. The optimization improves the characteristics of the intermediates’ adsorption and desorption, enabling the catalyst to exhibit remarkable bifunctional activity under alkaline conditions, achieving an overall overpotential as low as 0.67 V, with overpotential of merely 290 mV for the oxygen evolution process. The performance boost stems from a 38% larger electrochemical surface area (ECSA) combined with an 18% lower charge transfer resistance (Rct), pointing to gains in both active site numbers and intrinsic catalytic efficiency. We also employed X-ray absorption spectroscopy (XAS) and in situ Raman measurements to probe the Fe–Nx bonding configuration and track how the surface changes under the working conditions. Notably, zinc-air batteries using dual-function catalyst reached a peak energy density of 894 mAh g–1, maintained stable cycling for over 3000 h, and exhibited consistent charge–discharge capabilities in flexible quasi-solid-state devices (with voltage fluctuation remaining under 5% during bending strain), highlighting its immense potential for practical use in creating compact, high-capacity rechargeable batteries that can be worn or carried around. It is like giving us the keys to unlock a world where we can seamlessly incorporate portable energy solutions for renewable energy projects.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Jingjing He,Yu Wan,Wenjun Zhou
Developing high-efficient hybrids carbon catalysts for PMS-based advanced oxidation process (AOPs) are crucial in the field of environmental remediation. In this work, novel carbon nanocubes (xFe‒N‒C) with three-dimensional porous structure and abundant well-dispersed FeN x sites were obtained via a skillful cage-encapsulated-precursor pyrolysis strategy. The as-synthesized xFe‒N‒C exhibited superb activity for phenol degradation by activating peroxymonosulfate (PMS). Besides, the catalytic system not only possessed good recycling performance, wide pH adaptation and relatively low activation energy, but also had high resistance to environmental interference. Singlet oxygen ( 1 O 2 ) dominated non-radical process was responsible for phenol degradation rather than traditional radical pathways. Impressively, the doping level of Fe could regulate FeN x contents in catalysts, and the catalytic activity of xFe‒N‒C was greatly enhanced with increasing FeN x contents. Based on density functional theory calculations (DFT), the introduction of FeN x sites regulated the electronic structure of catalysts. Such electron-deficient Fe center acted as electron acceptor to receive electrons transmitted by the adsorbed PMS , thus generating highly reactive 1 O 2 for rapid phenol oxidation. This work provides a new insight into the innovation in transition metal-nitrogen hybrid carbon catalysts and highlights the pivotal roles of FeN x sites in 1 O 2 generation during PMS activation process.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Shengzhi He,Jingyu Wang,Chunwen Sun
Oxygen reduction reaction (ORR) serves as the foundation for various electrochemical energy storage devices. Fe/N C catalysts are expected to replace commercial Pt/C as oxygen electrode catalysts based on the structural tunability at the atomic level, abundant iron ore reserves and excellent activity. Nevertheless, the lack of durability and low active site density impede its advancement. In this work, a durable catalyst, Cu Fe/N C, for ORR was prepared by modulating the interfacial composition and electronic structure. The introduction of Cu nanoclusters partially eliminates the Fenton effect from Fe and optimizes the electron structure of Fe N x , thereby effectively enhancing the long-term durability and activity. The prepared Cu Fe/N C exhibits a half-wave potential ( E 1/2 ) of 0.90 V and superior stability with a decrease in E 1/2 of only 20 mV after 10,000 cycles. The assembled alkaline Zinc-Air batteries (ZABs) with Cu Fe/N C exhibit an open-circuit potential of 1.458 V. At a current density of 5 mA cm −2 , the batteries are capable of operation for 600 h with a stable polarization. This Cu Fe/N C may promote the practical application of novel and renewable electrochemical energy storage devices.
研究领域:
电化学
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催化
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能量存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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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
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