CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Fenli Liu,Yujing Ren,Jianglin Duan,Pengcheng Deng,Jianyu Lu,Huibin Ge,Xin Liu,Qixing Xia,Haifeng Qi,Na Yang,Yong Qin
Activating hydrogen peroxide (H 2 O 2 ) to produce hydroxyl radical ( • OH) (Fenton-like process) is of great importance in heterogeneous catalytic oxidations. However, most of transition metal nano-catalysts as well as recently reported carbon supported Fe-N 4 single atom catalysts (SACs) suffer from unsatisfactory catalytic performance. Herein, a novel Fe 1 /C 3 N 4 SAC with Fe-N 5 active site was constructed. Using this SAC, the electron/structure-symmetry of Fe-N 4 site can be broken by axial nitrogen-coordination, which transforms less active Fe-N 4 species into highly active Fe-N 5 species in Fenton-like reaction. Specifically, Fe-N 5 site exhibits an unprecedented activity for 3,3′,5,5′-tetramethylbenzidine oxidation, which is at least one order of magnitude more active than reported Fe-N 4 /C SACs. Mechanism studies reveal that the unique role of axial nitrogen-coordination over Fe-N x sites is to change the adsorption behavior of H 2 O over Fe-N 5 site without influencing H 2 O 2 activation. This discovery provides a new approach for rationally designing efficient catalysts in Fenton-like reactions.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
Polymers
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2023
·Vol. 15
·期 19
·3879
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IF 5
Xiangyu Chen,Jiahua Ma,Xiaoshuai Sun,Chuanshan Zhao,Jiehua Li,Hui Li
This paper proposes a different strategy for deriving carbon materials from biomass, abandoning traditional strong corrosive activators and using a top−down approach with a mild green enzyme targeted to degrade the pectin matrix in the inner layer of pomelo peel cotton wool, inducing a large number of nanopores on its surface. Meanwhile, the additional hydrophilic groups produced via an enzymatic treatment can be used to effectively anchor the metallic iron atoms and prepare porous carbon with uniformly dispersed Fe−Nxstructures, in this case optimizing sample PPE−FeNPC−900’s specific surface area by up to 1435 m2g−1. PPE−FeNPC−900 is used as the electrode material in a 6 M KOH electrolyte; it manifests a decent specific capacitance of 400 F g−1. The assembled symmetrical supercapacitor exhibits a high energy density of 12.8 Wh kg−1at a 300 W kg−1power density and excellent cycle stability. As a catalyst, it also exhibits a half−wave potential of 0.850 V (vs. RHE) and a diffusion-limited current of 5.79 mA cm−2at 0.3 V (vs. RHE). It has a higher electron transfer number and a lower hydrogen peroxide yield compared to commercial Pt/C catalysts. The green, simple, and efficient strategy designed in this study converts abundant, low−cost waste biomass into high-value multifunctional carbon materials, which are critical for achieving multifunctional applications.Keywords:pomelo peel;enzymatic treatment;Fe−Nx;supercapacitors;ORR
研究领域:
材料科学
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能源科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Liuqun Fan,Zhiyan Hou,Tianbao Liu,Xiangjing Liang,Andrei Ivanets,Kongjun Ma,Xintai Su
Heteroatom-doped carbon materials derived from oil-bearing sludge exhibit excellent supercapacitor performance due to their unique electronic and chemical properties. However, the complex composition of heteroatoms in oil-bearing sludge makes it difficult to achieve sufficient and directional doping by direct pyrolysis . In this paper, an oleic acid pretreatment-roasting-secondary activation strategy was developed to make full use of hydrocarbons, iron- and nitrogen-containing compounds in oil-bearing sludge to prepare Fe-N X -C materials with excellent electrochemical properties. Characterization results such as transmission electron microscopy (TEM) and N 2 adsorption analysis showed that the best sample had a hierarchical pore structure and uniform Fe and N element loading. X-ray photoelectron spectroscopy (XPS) analysis found that the addition of oleic acid can promote the formation of Fe-Nx, and the dosage of oleic acid will affect the content of Fe-Nx in the carbon materials. Electrochemical characterization of this supercapacitor material was conducted. The best sample's specific capacitance was as high as 293.6 F g −1 at the current density of 0.5 A g −1 , and the capacitance retention rate could still reach 71.5% at the current density of 10 A g −1 . The assembled button-type symmetrical supercapacitors had an energy density of 8.68 Wh kg −1 and a power density of 137.53 W kg −1 , which is much higher than those of most other waste-based carbon materials. This work presents a new idea for the preparation of heteroatom doped carbon materials with excellent capacitive properties from oily sludge, which provides a new reference for the treatment and resource utilization of oily sludge.
研究领域:
环境科学
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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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2022
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IF 6.371
Yang Yuan,Youzhen Liu,Chenhui Li,Shi Feng,Qingquan Liu,Jia Huo
The electrocatalytic oxygen reduction reaction (ORR) plays an important role in renewable energy storage and conversion systems such as polymer electrolyte membrane fuel cells. However, design of high-performance cathode electrocatalysts is still required to speed up the sluggish kinetics of ORR. In this work, we develop a facile strategy to synthesize hierarchically porous N-doped carbon nanosheet networks with ultrafine encapsulated Fe 3 C and Fe-N x for ORR by consideration of thermodynamic (intrinsic and support effect) and kinetic (diffusion effect) parameters. The synthetic process is straightforward and sustainable and the hierarchically porous materials can be synthesized directly starting from raw materials and without any additional template. The as-designed catalyst exhibits excellent ORR catalytic performance in both acidic and basic media with much positive half-wave potential and good stability, which is comparable to commercial Pt/C. The excellent ORR performance may result from highly active Fe-N x sites and ultrafine encapsulated Fe 3 C, and the hierarchically porous nanosheet structure for accelerating mass diffusion and increasing exposure of the active site. This work provides a facile strategy for rational design and synthesis of highly active, hierarchically porous non-precious metal electrocatalysts.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
RSC Advances
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2019
·Vol. 9
·期 72
·42236-42244
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IF 3.049
Limeng Yang,Zhigang Shao
The development of low-cost, efficient and stable electrocatalysts for the oxygen reduction reaction (ORR) is desirable but remains a great challenge. We report a convenient and efficient synthesis approach of highly dispersed Fe–Nx catalysts for ORR. Typically, Fe–Zn-ZIF (zeolitic imidazolate frameworks) nanocrystals cast as precursor and graphene as supports, highly dispersed Fe–Nx species were fabricated with PVP (polyvinyl pyrrolidone) as surfactant via pyrolysis. With the help of graphene and surfactant, the agglomeration of iron particles has been avoided during pyrolysis, and the size and morphology of ZIF particles intercalating into the graphene layers can be regulated precisely as well. The amount of Fe–Nx active sites in C-rGO-ZIF catalyst arrived 4.29%, which is obviously higher than most monodispersed non-precious metal catalysts reported. The obtained C-rGO-ZIF catalyst exhibits a high onset potential of 0.89 V and a half-wave potential of 0.77 V, which is only 30 mV away from Pt/C in acidic media. The active sites of the catalyst was characterized and found to be the highly dispersed Fe–Nx species, large and accessible specific surface area of graphene and abundant active nitrogen atoms. When the C-rGO-ZIF catalyst was applied in the cathode of fuel cell, the power density can reach up to 301 mW cm−2, which highlights a practical application potential on small power supplies.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Junjie Cheng,Xinman Tu,Pengxuan Wu,Rentao zhou,Shaohua Luo,Li Zhang,Jianping Zou,Yanhong Li,Hannah M. Johnson,Qiang Zhang
In the reaction systems involving peroxymonosulfate (PMS) activation, the degradation of organic pollutants is influenced by the distinct roles played by the oxidation of free radicals and non-free radicals. The synergistic effect resulting from both oxidation pathways is often more efficient compared to a single oxidation pathway, as it allows for the optimal utilization of oxidation capacity and adaptation to complex reaction environments. Nitrogen-doped carbon substrates hosting single-atom catalysts (SACs) are anticipated to serve as an optimal platform for managing the dual oxidation pathways in the PMS activation reaction. This is attributed to the availability of numerous reaction sites that meet the activation requirements. However, there's a lack of substantial reports on this subject. Herein, we synthesized a series of single-atoms Fe nitrogen-doped carbon catalysts with different coordination structures by adjusting the coordination numbers between Fe and N atoms. It is used to investigate the reaction pattern of PMS over SACs, so as to enhance the catalytic efficacy of SACs through distinct coordination structures. The experimental and theoretical results indicate that PMS functions as both an electron receiver and provider on FeN x /C catalysts. Moreover, the specific arrangement of the Fe-N-C structure influences the exchange of electrons between the catalysts and PMS. Hence, the co-oxidation pathway of free radicals ( OH, SO 4 − and O 2 − ) and non-free radicals ( 1 O 2 ) can be modulated by altering the coordination number of Fe and N atoms during PMS activation. The elimination efficiency of tetracycline hydrochloride was significantly enhanced due to the abundance of both free radical and non-free radical species generated in the FeN 3 /C/PMS reaction system, exhibiting a degradation kinetic constant of 0.564 min −1 . In addition, it showed promising potential for application in practical wastewater degradation, exhibiting high anti-interference to general environmental disturbances (such as humic acid, chloride ions, bicarbonate ions and nitrate ions).
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Journal of Energy Storage
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2023
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IF 9.4
Tao Xie,Guancheng Xu,Yong Yao,Peiyan Li,Wene Du,Hui Ding,Jiahui Jiang,Li Zhang
Metal-nitrogen doped carbon materials (M/NCs) exhibit considerable potential as electrocatalysts for oxygen reduction reaction (ORR) in novel energy conversion and storage devices. Herein, the Fe–N x doped porous carbon catalysts (FeN x PCs) with three-dimensional (3D) pore structure are synthesized by in situ pyrolyzation of polypyrrole-coated Fe 2 O 3 (Fe 2 O 3 @PPy). Fe 2 O 3 derived from the iron-formate framework (Fe-FF) is partially dissolved to generate Fe 3+ for driving polymerization and served as template to form the 3D structure during polymerization. FeN x PCs exhibit satisfactory long-term durability and superior ORR activity ( E 1/2 = 0.89 V) compared to commercial Pt/C. The Zn-air battery (ZAB) assembled with FeN x PCs reveals excellent battery performance, including a high open circuit voltage of 1.50 V, peak power density of 155.4 mW cm −2 , and cycling stability with 500 cycles. The excellent ORR activity of FeN x PCs could be ascribed to the porous structure , Fe–N x active sites, and high defect level of FeN x PCs. This strategy can modulate 3D porous structure via self-template synthesis, which provides a novel insight for development of high-performance air cathode catalyst.
研究领域:
能源材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Lei Cao,Maliang Zhang,Kunmei Su,Feng Gu,Zhenhuan Li
Decorating porous carbon nanomaterials with rich homodispersed metal cluster and heteroatoms can effectively shorten the diffusion pathway of oxygen and expose more active sites, thereby promoting oxygen reduction reaction (ORR). Herein, hierarchical porous carbon nanorods with homodispersed Fe–N x –C active sites are obtained by calcination , etching and ammonia activation of Fe-nitrogenous acid (NTA) coordination polymer nanowires. The obtained Fe-PCNRs-700 as ORR catalysts show the excellent activity with half wave potential (E 1/2 ) of 0.71 V vs. reversible hydrogen electrode (RHE) in 0.5 M H 2 SO 4 and 0.87 V vs. RHE in 0.1 M KOH electrolyte, which owe to its huge specific surface area (1652 m 2 g −1 ), hierarchical pore structure , homodispersed Fe–N x –C active sites and structural defects. Furthermore, using Fe-PCNRs-700 as a cathode catalyst in both liquid and flexible solid Zn-air batteries, and the assembled liquid batteries display the high power density of 161 mW cm −2 and robust charge/discharge stability of 116 h.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
CHINESE CHEMICAL LETTERS
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2023
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IF 9.1
Fengxian Zhang,Xupo Liu,Ye Chen,Miao Tian,Tianfang Yang,Jing Zhang,Shuyan Gao
Fe-N X /C electrocatalysts have aroused extensive interest in accelerating sluggish oxygen reduction reaction (ORR) kinetics as potential alternatives to platinum catalysts in rechargeable Zn-air batteries (ZABs). However, the low density and poor accessibility of Fe-N X sites have severely restricted the electrocatalytic performance of Fe-N X /C. Herein, Fe, N co-doped ordered mesoporous carbon fiber bundles are prepared through a ligand-assisted strategy with nitrogen-rich 1,10-phenanthroline as space isolation agent. 1,10-Phenanthroline reveals a six-membered heterocyclic structure containing abundant nitrogen species to tightly coordinate with Fe ions , which is conducive to achieving high-density Fe-N X sites. Meanwhile, the adoption of SBA-15 as hard-templates enables the catalysts with highly ordered channels and large specific surface areas, improving the accessibility of Fe-N X sites. The optimal catalyst (PDA-Fe-900) demonstrates a positive half-wave potential of 0.84 V ( vs. RHE) in alkaline solution, outperforming the commercial Pt/C (0.83 V). In addition, PDA-Fe-900 delivers comparable ORR performance to commercial Pt/C in acidic electrolyte. Impressively, when PDA-Fe-900 is employed as an air cathode, it achieves large power densities of 163.0 mW/cm 2 in liquid-state ZAB and 116.6 mW/cm 2 in the flexible solid-state ZAB. This work provides an efficient ligand-assisted pathway for fabricating catalysts with dense and accessible Fe-N X sites as high-performance ORR electrocatalysts for ZABs.
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
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Zhenrui Li,Zhihui Wang,Linxin Dai,Jianfeng Ma,Xing’e Liu
A lignin-based Fe/N co-doped carbonaceous catalyst was synthesized via freeze-drying followed by pyrolysis to activate peroxymonosulfate (PMS) for efficient degradation of bisphenol A (BPA). The Fe/N co-doped biochar exhibited a high specific surface area (364.84 m 2 /g), hierarchical porous structures, and abundant oxygen-containing functional groups (hydroxyl and carboxyl groups), which enhancing the dispersion of Fe 3 O 4 nanoparticle and exposure of catalytic site. The Fe 8 -N 10 -C/PMS system achieved 100 % BPA degradation within 20 min with a corresponding first-order reaction rate constant ( k obs ) of 0.4056 min −1 , which outperformed most reported catalysts in efficiency. Quenching and EPR analyses revealed that both free radicals ( • OH, SO 4 •− , and O 2 •− ) and non-radical ( 1 O 2 ) were rate-limiting steps, while graphitic N and Fe-N x structures facilitated direct electron transfer from BPA to PMS in electrochemical tests. XPS results confirmed that pyrrolic N, rather than pyridinic N, played a crucial role in forming the Fe-N x structure. Moreover, the catalyst showed excellent stability, regeneration capability, and adaptability under diverse conditions, highlighting the potential of the Fe-N-C/PMS system for practical wastewater treatment applications.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Guang Li,Juan Yang,Yulian Chen,Min Liu,Xiaowei Guo,Gairong Chen,Baobao Chang,Tianjing Wu,Xianyou Wang
Looking for a high-efficiency, durabile, and low-cost dual-functional oxygen electrocatalyst as the air electrode catalyst in rechargeable zinc-air batteries (ZABs) is urgently desirable but faces many challenges. Herein, we propose the preparation strategy of effectively using a bifunctional electrocatalyst (Fe–Nx/C) based on the zeolite imidazole organic framework-8 (ZIF-8) as the template agent, with surface modification coated by ferrocene (Fc) molecules followed by pyrolysis at high temperature under inert atmosphere. Benefiting from the surface modification of ZIF-8 with Fc molecules, more abundant multiple catalytic Fe/Fe–Nx/FeCx sites with high intrinsic activity are derived, the resultant Fe–Nx/C exhibits excellent potential gap (ΔE = 0.63 V) and durability, which is obviously superior to the Pt/C + IrO2 benchmark (ΔE = 0.77 V) and other state-of-the-art electrocatalysts. Furthermore, the assembled rechargeable ZABs employing the Fe–Nx/C as an air-electrode show a reduced charging–discharging potential difference of 0.603 V, high power density of 214.8 mW cm–2, and long-term cycling stability of more than 290 h at 2.0 mA cm–2. Therefore, this work presents a feasible strategy to prepare a high-efficiency and durability ORR/OER bifunctional electrocatalyst toward high performance ZABs and next-generation energy storage devices.
研究领域:
材料科学
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电化学能存储与转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Miao,Ying Liu,Dandan Wang,Ningjie Du,Ziwei Ye,Yang Hou,Shun Mao,Kostya (Ken) Ostrikov
Transition-metal and nitrogen co-doped carbon-based catalysts receive much attention in peroxymonosulfate (PMS) activation. However, the contribution of doped metal and the kinetic mechanisms of the emerging nonradical pathways especially enabled by reactive singlet oxygen species remain unclear. Herein, we report Fe-N-co-doped carbon-based catalysts (FeCNx) for peroxymonosulfate activation. The catalysts achieve fast removal of a broad spectrum of organic pollutants in a wide pH range without the common Fe leaching. Both catalyst surface-activated PMS complex (catalyst-PMS*), surface-bound radicals, and singlet oxygen are identified. The new mechanism is enabled by the Fe-Nx single-atomic-site that enhances the adsorption of PMS and facilitates the formation of catalyst-PMS*. The formation route of singlet oxygen species is elucidated for the first time for Fe, N-co-doped carbon-based catalysts with density functional theory simulation. This study reveals the intrinsic role of Fe-Nx site in catalysts and provides new insights into the origin and kinetics of non-radical pathways for peroxymonosulfate activation.
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
危险品化学品经营许可证（带存储）