SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Youpu Zhao,Qing Sun,Jian Zhang,Jiawei Sheng
In this study, natural porous diatomite was utilized as a conciliatory carrier for the fabrication of Fe/N/C nano-clusters with assistance of binary molten salt of NaCl-ZnCl 2 under different annealing temperature and used to removal of norfloxacin (NFA). The sample Fe/D m900 (prepared at 900 °C) exhibited a high surface area and great catalytic performance for antibiotics in the presence of PMS. Over 97% NFA can be decomposed within 5 min and the final degradation rate reached 98%. Meaningfully, high-efficiency Fe/D m900 -PMS system was nearly impervious to pH values and inorganic cations in aqueous solution and could be a likely candidate for degradation of multiple contaminants in pharmaceutical outlet water. Furthermore, the other impacting variables such as catalyst dosage, PMS dosage, NFA concentration and initial pH were moreover explored towards debasement, and conceivable degradation pathways of NFA were presented through LC-MS. This work builds up a compelling procedure to synthesize super-dispersed Fe clusters, which may be amplified to other transition metal-based catalyst via molten salt.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 15
·9761-9770
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IF 12.732
Dan Wang,Hao Xu,Peixia Yang,Lihui Xiao,Lei Du,Xiangyu Lu,Ruopeng Li,Jinqiu Zhang,Maozhong An
Extensive efforts have been devoted to active site designing for non-precious metal electrocatalysts; however, the porous structure engineering has been less emphasized, particularly for catalysts for gas diffusion electrodes, e.g., the cathode (oxygen reduction reaction, ORR) of Zn–air batteries. The desired porous structure is not only important for exposing high-density active sites but also beneficial for boosting mass transfer. Here, a dual-template strategy is proposed for constructing hierarchically porous structural Fe–N–C catalysts with dense active Fe–Nx moieties for the cathode of Zn–air batteries. The dual ZnCl2 and MgO hard templates jointly promote the formation of hierarchically interconnected carbon networks. The experimental results indicated both significantly improved active site accessibility and mass transfer, reasonably leading to enhanced ORR activity in conventional three-electrode cells. Particularly, it is deduced that the microporous structure is beneficial for dense active Fe–Nx moieties, while the ultra-macroporous structure is conducive to mass transfer during the ORR process. We further applied this dual-template-mediated catalyst in a real-world liquid Zn–air battery, which presents a high open-circuit voltage of 1.48 V and a remarkable energy density of 952.8 W h kgZn−1. Such robust battery performance is among the best compared with reported Zn–air batteries using non-precious metal catalysts. Particularly, a peak power density of 116.8 mW cm−2 is achieved in an all-solid-state Zn–air battery.
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ANALYST
·
2021
·Vol. 146
·期 14
·4557-4565
·
IF 4.616
Xiangyu Ma,Kun Qian,Onome Ejeromedoghene,Martha Kandawa-Schulz,Wei Song,Yihong Wang
Taking a composite of a nanomaterial and a signal molecule as a substrate material can provide a label-free electrochemical platform. Besides, the nanomaterial with a high catalytic activity towards the signal molecule can improve the sensitivity of the platform. Herein, a thionine functionalized Fe–N–C nanocomposite was employed as the substrate. Firstly, the electrocatalytic activity of Fe–N–C towards the electroreduction of thionine was explored. Then, an immobilization-free and label-free electrochemical platform for the determination of microRNA-21 based on Fe–N–C–thionine/Fe3O4@AuNPs was constructed. A magnetic glassy carbon electrode (MGCE) was used to keep the magnetic Fe–N–C–thionine/Fe3O4@AuNPs modified onto the surface of the MGCE. Fe–N–C and Fe3O4 nanoparticles can co-catalyze the electroreduction of thionine and a strong electrochemical reduction signal of thionine could be realized in the differential pulse voltammetry (DPV) test. Also, a catalytic hairpin assembly (CHA) reaction was utilized to enhance the sensitivity of the developed electrochemical biosensor. Besides, the developed biosensor shows excellent specificity and reproducibility in the test of human serum samples, indicating its wide application prospects in the early-stage diagnosis of tumors.
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高影响因子
CARBON
·
2020
·
IF 8.821
Shuqi Hu,Wenpeng Ni,Daihui Yang,Chao Ma,Jiaheng Zhang,Junfei Duan,Yang Gao,Shiguo Zhang
Atomically dispersed Fe–N–C catalysts with additional Fe-containing nanoparticles including metal, carbides or oxides have shown great potentials towards oxygen reduction reaction (ORR) catalysis. However, the formation of these synergistically active nanoparticles and the effect of the porous carbon structures remain unclear. In this work, a novel single-atom-involved electrochemical catalyst, i.e. , Fe 3 O 4 nanoparticles encapsulated in atomically dispersed Fe–N–C (Fe 3 O 4 @FeNC) was reported. The optimized Fe 3 O 4 @FeNC exhibits excellent ORR activity with a half-wave potential of 0.890 V and a Tafel slope of 58.8 mV dec −1 , comparable with recently reported ORR catalysts and superior to these of commercial Pt/C. More importantly, the porous architectures not only affect the mass transfer and active sites, but casts huge influence on the nucleation of Fe 3 O 4 nanoparticles, the graphitization degree of the carbon support, the chemical environments of the elements, and the ORR catalytic pathways. Density functional theory calculations show stronger O 2 adsorption on Fe–N–C when supported on Fe 3 O 4 moieties, which may increase the reactant concentration for ORR and promote the overall activity. These findings will provide important references for the future understanding and design of single-atom-involved catalysts with enhanced electrochemical properties .
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Xilong Wang,Qinghua Zhang,Hechun Jiang,Yadong Li,Hongwei Zhu,Lirong Zheng,Lin Gu,Han-Pu Liang
Pt-based intermetallic alloys with high activity and stability are promising for accelerating the cathodic oxygen reduction reaction (ORR) and large-scale application of proton exchange membrane fuel cells. So far, facile synthesis of Pt-based alloys in less time is desirable but still challenging. Herein, based on the traditional wet impregnation method, facile in situ reduction of H2PtCl6 and alloying with a hybrid nanostructure mainly doped with Fe single atoms as well as small amounts of Fe-based nanoparticles and oxides were developed to fabricate highly dispersed PtFe nanoparticles loaded on a mesoporous Fe–N–C support. Alloying of Pt derived from H2PtCl6 with various iron-based species existing in forms of single-atom, metallic, and oxide states was confirmed by systematic characterization, and the Fe content in the support is important for PtFe alloy formation, and the corresponding electrochemical performance promotion has been identified. The as-synthesized best-performance PtFe/Meso-PDA-5 catalyst delivered a high potential of 0.925 V at a current density of 3 mA cm–2 and achieved a high mass activity of 497.5 mA mgPt–1 at 0.9 V for the ORR in 0.1 M HClO4. More importantly, only 17.9% mass activity loss was observed after 10k potential cycles of the accelerated deterioration test. The present work provides a strategy for facile synthesis of Pt-based alloy nanomaterials for ORR catalysis and highlights the importance of supports in alloy formation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Qian Liu,Chenye Zhang,Meimei Ren,Jinyi Wang,Leixin Feng,Yixuan Wang,Chuang Liu,Ningru Xiao,Haiming Zhang
Development of low Pt-loading electrocatalyst with enhanced activity towards oxygen reduction reaction (ORR) is highly demanded for widespread penetration of clean energy technologies. Heterointerface regulation can effectively optimize the electronic structure and intrinsic activity of the carbon supported Pt-based electrocatalyst to reduce Pt consumption. Here, by judicious choice of a sulfur-doped Fe-N-C (Fe-NS-C) as support, we construct a novel Pt/Fe-N-C heterointerface with sulfur incorporation and develop a hybrid electrocatalyst (denoted as Pt@Fe-NS-C) with ultralow Pt-loading (1.51 wt%). The incorporation of sulfur triggers the charge redistribution at the heterointerface and reduces the electron transfer from Pt to Fe-NS-C, prompting the electron density around Pt sites and boosting the electrocatalytic performance towards ORR (half-wave potential: 0.903 V; mass activity of 1.28 A mg −1 Pt at 0.9 V). In comparison, Pt species dispersed onto Fe-N-C without sulfur doping (Pt@Fe-N-C) are electron-deficient, which is not conductive to activate O 2 and results in inferior ORR activity. Zinc-air battery fabricated with Pt@Fe-NS-C as the cathode catalysts shows a large peak power density and a specific capacity of 806.7 mAh g −1 Zn . This work offers an effective way to tailor the heterointerface of hybrid or supported electrocatalyst with optimized electronic structures towards advanced electrocatalysis .
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Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 17
·6630-6638
·
IF 8.262
Fei He,Xinghua Chen,Yanfei Shen,Ying Li,Anran Liu,Songqin Liu,Toshiyuki Mori,Yuanjian Zhang
The development of efficient and low-cost non-precious-metal electrocatalysts such as Fe–N/C for the oxygen reduction reaction (ORR) is crucial for fuel cells and metal–air batteries. Here, we report a class of highly efficient Fe–N/C electrocatalysts derived from versatile imidazolium-based ionic liquids (ILs) with a halogen-coordinated iron anion. Without any supports, templates, or multi-step pyrolysis, the as-prepared Fe–N/C catalysts exhibited superior activity in the ORR to the state-of-the-art Pt/C in alkaline electrolytes by 44 mV in half-wave potential. More interestingly, owing to the versatile configuration of the imidazolium-based IL precursors, a diverse range of catalyst structures was successfully modulated. Based on this, it was clearly revealed that the electrical conductivity, type/amount of N dopants, and “effective porosity” (not the conventional total surface area) jointly determined the electrocatalytic activity. A pivotal radar chart is further proposed to successfully predict activity in the ORR merely from the structures of Fe–N/C catalysts. The proposed ILs platform would provide a valuable toolbox for the molecular design of precursors to tune the structures of Fe–N/C electrocatalysts towards excellent activity in the ORR in a highly flexible manner, and facilitate the long-term challenging study of relationships between processing, structure and activity.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Junhao Chen,Shutian Lin,Sisi Xiang,Yuanhong Zhong,Yingxia Zhao,Ming Sun,Lin Yu
A ZIF-8-derived Fe–N–C single-atom catalyst is developed for HMF-to-FFCA oxidation. • The catalyst obtained 99.4% HMF conversion and 94.2% FFCA yield under mild conditions. • O 2 • and 1 O 2 are identified as the key reactive species governing selective oxidation. • Fe–N x moieties are confirmed as the active centers for O₂ activation and selectivity. The catalytic valorization of 5-hydroxymethylfurfural (HMF) to high-value chemicals is critical for sustainable chemistry. However, 5-formyl-2-furancarboxylic acid (FFCA), a key oxidation intermediate, remains a significant challenge. Herein, a Fe N C single-atom catalyst derived from zeolitic imidazolate framework-8 (ZIF-8) is developed for efficient HMF-to-FFCA conversion under mild conditions (90 °C, 0.1 MPa O 2 ). It has been revealed that the isolated Fe–N x sites are dispersed on a nitrogen-doped carbon matrix. The optimized catalyst delivers 99.4% HMF conversion with 94.2% FFCA yield within one hour, and exhibits excellent catalytic and structural stability over consecutive reaction cycles. Mechanistic studies combining Electron paramagnetic resonance (EPR) spectroscopy and radical trapping experiments demonstrate that superoxide radicals (O 2 • ) and singlet oxygen ( 1 O 2 ) govern the selective oxidation pathway. Active-site poisoning with thiocyanate confirms the essential role of Fe–N x moieties in oxygen activation. This work presents a robust non-noble metal catalyst platform for HMF valorization and advances the fundamental understanding of single-atom catalyst design for biomass oxidation reactions. Download: Download high-res image (189KB) Download: Download full-size image
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CATALYSIS LETTERS
·
2023
·Vol. 153
·期 12
·3569-3580
·
IF 2.8
Lin Shanshan,Liu Jianguo,Ma Longlong
Aniline is a group of important platform molecules that has been widely used in the synthesis of other high-value chemicals and pharmaceutical products. How to produce high-value anilines as the high-value chemical intermediates more efficiently and environmentally has always been a research topic in the industry. Catalytic hydrogenation is an environmentally friendly method for preparing halogenated anilines. Traditional noble metal catalysts face the problems of cost and noble metals residue. To improve the purity of the product as well as the activity and recyclability of the catalyst, we prepared a Pd/Fe magnetic bimetallic catalyst supported on N-doped carbon materials to reduce nitrobenzene to aniline under mild conditions. The catalyst has a low Pd loading of 2.35%. And the prepared bimetallic Pd/Fe@N/C catalyst showed excellent catalytic reactivity with the nitrobenzene conversion rate of 99%, and the aniline selectivity of 99% under mild reaction conditions of 0.8 MPa H 2 and 40 °C. A variety of halogenated and aliphatic nitro compounds were well tolerated and had been transformed to the corresponding target amine products with excellent selectivity. In addition, the novel N-doped graphene-encapsulated bimetallic magnetic Pd/Fe@N/C catalyst not only had magnetic physical properties, which was easy to separate, recover, and used for the recycling of the catalyst without metal leaching but also catalyzed highly selective reductive amination of aromatics was a green, economical and environmentally friendly reaction with the only by-product of H 2 O. Graphical Abstract
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PubMed
高影响因子
NANOTECHNOLOGY
·
2021
·Vol. 32
·期 30
·305402
·
IF 3.874
Yaqi Cui,Jiaoxing Xu,Yi Zhao,Lunhui Guan
The utilization of earth abundant iron and nitrogen doped carbon as a precious-metal-free electrocatalyst for oxygen reduction reaction (ORR) significantly depends on the rational design and construction of desired Fe−Nx moieties on carbon substrates, which however remains an enormous challenge. Herein a typical nanoporous nitrogen-rich single atom Fe−N/C electrocatalyst on carbon nanotube (NR-CNT@FeN-PC) was successfully prepared by using CNT as carbon substrate, polyaniline (PANI) and dicyandiamine (DCD) as binary nitrogen sources and silica-confinement-assisted pyrolysis, which not only facilitate rich N-doping for the inhibition of the Fe agglomeration and the formation of single atom Fe−Nx sites in carbon matrix, but also generate more micropores for enlarging BET specific surface area (up to 1500 m2·g−1). Benefiting from the advanced composition, nanoporous structure and surface hydrophilicity to guarantee the sufficient accessible active sites for ORR, the NR-CNT@FeN-PC catalyst under optimized conditions delivers prominent ORR performance with a half-wave potential (0.88 V versus RHE) surpass commercial Pt/C catalyst by 20 mV in alkaline electrolyte. When assembled in a home-made Zn−air battery device as cathodic catalyst, it achieved a maximum output power density of 246 mW·cm−2 and a specific capacity of 719 mA·h·g−1Zn outperformed commercial Pt/C catalyst, holding encouraging promise for the application in metal-air batteries.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Zhiyan Huang,Pingxiao Wu,Chenhui Liu,Meiqing Chen,Shanshan Yang,Zhi Dang,Nengwu Zhu
Understanding the origin of high activity of graphene layers encapsulated Fe-N-C catalysts in Fenton-like reaction is critical, but still challenging for developing catalysts with high activity and durability. Therefore, we prepared a highly active Fe-N-C catalyst (Fe x Mn y -Fe@NCs) containing FeN 4 coordination to activate peroxymonosulfate (PMS) toward 4-aminobenzoic acid ethyl ester (ABEE) degradation, and revealed the multiple catalytic reaction sites by investigating the composition and the structure of the catalyst. The relationship between the catalytic degradation performance and multiple catalytic reaction sites was performed on the basis of both experiments and density functional theory (DFT) calculations. The catalytic performance of Fe 2 Mn 1 -Fe@NCs was found to show optimal catalytic degradation performance. Pyrrolic N served as adsorption site as well as singlet oxygen generation site to promote the catalytic degradation. Fe-pyridinic N-C acted as hydroxyl radical and sulfate radical generation site. Both singlet oxygen and superoxide radical were dominated the catalytic reaction. The insight achieved from this study may be further applied to other Fe-N-C catalysts design and further efficient organic pollution remediation.
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Materials Today Energy
·
2020
·
IF 5.604
Kuofeng Xu,Huayuan Bao,Chaoyun Tang,Kristina Maliutina,Fengjiao Li,Liangdong Fan
The development of non-platinum electrocatalysts for the quick oxygen reduction reaction (ORR) is highly desirable in electrochemical energy conversion technologies such as fuel cells and metal-air batteries. In this work, we synthesize Fe 3 O 4 /Fe–N–C-CNT (FeNC) using Fe 3+ adsorbed ZIF-8 as a chemical precursor that is obtained with a green and sustainable procedure. FeNC possesses impressive ORR activities, stability and selectivity over that of the commercial Pt/C electrocatalyst in alkaline media, and demonstrates a better peak power density of 118.05 mW cm −2 over that with Pt/C cathode and quicker reaction kinetics when integrated as air electrode catalyst into a primary zinc-air battery. In-depth investigation confirms that the presence of Fe 3 O 4 increases the wettability of carbon-based composite that promotes the adsorption of the dissolved O 2 in the electrolyte solution and extends the triple-phase boundary for ORR, and also protect the active site of Fe–N–C from poisoning. This work sheds light on a sustainable method to synthesize highly efficient non-precious metal-based electrocatalyst from metal-organic-framework precursors and understanding the reaction mechanism of the ORR process for efficient chemical energy to electricity conversion.
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