NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 13
·6058-6065
·
IF 3.3
Xu Zhang,Jingxian Zhang,Shi Zeng,Haifan Wang,Yiling Bai,Huaming Hou,Ke Zhang,Bin Li,Guangjin Zhang
Iron–nitrogen-doped carbon (Fe–N–C) catalysts have been theoretically and experimentally demonstrated as one of the most promising materials to promote the oxygen reduction reaction (ORR), but they still have drawbacks in terms of stability and longevity. Herein, a novel strategy of loading Fe–N–C on cerium oxide cyanamide (Ce2O2CN2) is proposed to increase the density of active sites and improve the activity effectively. Ce2O2CN2 provides a Ce4+/Ce3+ redox pair to regulate the oxygen density on the catalyst surface, and the π–π interactions between Ce2O2CN2 and Fe–N–C are beneficial for interfacial charge transport. Consequently, Fe–N–C@Ce2O2CN2 shows excellent ORR activity with a half-wave potential (E1/2) of 0.89 V vs RHE and satisfactory long-term durability in an alkaline medium, and significantly outperforms commercial Pt/C. The Zn–air batteries made using the prepared catalyst exhibited a high peak power density of 119.35 mW cm−2. This study provides a new perspective for the application of platinum group-metal (PGM)-free catalysts in next-generation energy storage devices.
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ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Yingfang Yao,Yong You,Gaixia Zhang,Jianguo Liu,Haoran Sun,Zhigang Zou,Shuhui Sun
Tuna is one of the most rapid and distant swimmers. Its unique gill structure with the porous lamellae promotes fast oxygen exchange that guarantees tuna’s high metabolic and athletic demands. Inspired by this specific structure, we designed and fabricated microporous graphene nanoplatelets (GNPs)-based Fe/N/C electrocatalysts for oxygen reduction reaction (ORR). Careful control of GNP structure leads to the increment of microporosity, which influences the O2 adsorption positively and desorption oppositely, resulting in enhanced O2 diffusion, while experiencing reduced ORR kinetics. Working in the cathode of proton-exchange membrane fuel cells, the GNP catalysts require a compromise between adsorption/desorption for effective O2 exchange, and as a result, appropriate microporosity is needed. In this work, the highest power density, 521 mW·cm–2, at zero back pressure is achieved.
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Sustainable Energy & Fuels
·
2025
·
IF 4.1
Yongheng Xiong,Yang Yu,Huangang Shi,Jifa Qu,Wenyi Tan
Single atom Fe sites, doped in CN materials, exhibit outstanding electrochemical activity for CO2-to-CO conversion. The pyrolysis of ZIF8 is a controllable method for fabricating isolated single atom metal sites. In this study, we propose a new strategy to increase the ratio of Fe in ZIF8 precursors by synergistically replacing Zn2+ with Bi3+ and Fe3+. After precursor pyrolysis, the obtained Bi/Fe–N–C catalysts, consisting of Bi sites and pyrrole-type Fe–Nx sites, serve as efficient electrocatalysts for the CO2RR. The results show that the optimized catalyst loaded with 94.8 mg per kgCat Fe exhibits a high FECO of >90.1% over a wide potential range of −0.4 to −0.7 VRHE (98.2% at −0.5 VRHE). Insights into the electrochemical reaction mechanism show that this successful design of Bi/Fe–N–C catalysts can provide a stable catalytic site to form *COOH, thus achieving energy-efficient electrochemical CO2 reduction to CO.
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Chemistry-An Asian Journal
·
2025
·
IF 3.3
Boyu Jia,Li Ju,Fancang Meng,Huan Wu,Kexiang Li,Qingmin Ji
The chemical modification and self-assembly capability of fullerenes offer advantageous conditions for tailoring Fe/N-doped carbon-based catalysts. However, their strong π–π stacking tendency may partially restrict metal loading and the generation of active Fe species. Therefore, how to utilize the distinctive features of fullerenes to precisely regulate and optimize Fe–N active sites along with their local coordination environment remains challenging. In this work, water-soluble C 60 (wsC 60 ) was synthesized via a facile interfacial oxidation process. The presence of –OH on the C 60 cage may strengthen its binding affinity with Fe 3+ ion and effectively modulate the incorporation of Fe/N into the C 60 -derived carbon electrodes. By varying the wsC 60 /Fe 3+ mixing ratios followed by pyrolysis under NH 3 , we obtained Fe/N-doped carbons (FeN@wsC 60 -900) with distinct Fe/N-doping states, including FeN 4 , O–FeN 4 /Fe cluster, and FeN 4 /Fe cluster. The abundant –OH in wsC 60 also promoted the formation of a highly porous network, enhancing active site accessibility. The resultant FeN@wsC 60 -900 exhibited excellent oxygen reduction reaction (ORR) activity, outperforming both conventional C 60 -derived carbons and commercial Pt/C. Structural characterizations and density functional theory (DFT) simulations revealed that the O-coordinated Fe–N 4 with adjacent Fe cluster could optimize the coordinate geometry and adsorption energies of key ORR intermediates.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 5
·053505
·
IF 4.386
Yanfang Song,Jinxiong Wu,Jiliang Zheng,Yiwei Sun,Andrei Ivanets,Guangming Du,Xintai Su
The doping of multiple heteroatoms can improve the electrochemical properties of carbon substrates. However, in existing studies, carbon, iron and nitrogen sources are generally mixed directly and then pyrolyzed for secondary activation. This tends to form aggregates of metal particles or metal oxides and requires the consumption of large amounts of alkali and energy. Therefore, there is an urgent need to develop an environmentally friendly technology capable of uniformly doping iron and nitrogen into carbon materials. In this work, porous Fe–N–C composites were prepared at 600 °C using potassium humate (HA-K) obtained from cotton straw by low-temperature pyrolysis as the carbon source, and urea-iron complexes formed by the pre-coordination of urea and Fe as the iron and nitrogen sources. In the absence of secondary activation, the best sample Fe-NHPC-2 had a good mesoporous structure with high specific surface area (889. 01 m2 g−1). It had a high specific capacitance of 256.8 F g−1 at a current density of 0.5 A g−1. The capacitance retention was 92.6% after 10,000 cycles at a current density of 10 A g−1. In the symmetric supercapacitor application, the energy density reached 33.16 Wh kg−1 when the power density was 600.2 W kg−1.
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Industrial Chemistry & Materials
·
2024
·
IF 0
Jiayao Cui,Junyong Min,Hao Wang,Jianglan Shui,Lishan Peng,Zhenye Kang,Jieyuan Liu,Qingjun Chen,Shuo Bai,Yanrong Liu
Developing single-atom Fe–N4/C catalysts is crucial for the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). While Fe–N4/C catalysts are inherently active in accelerating the slow ORR process, their performance is still inferior to that of Pt/C. Herein, a trace Co-doped Fe single-atom catalyst (Fe(tCo)–N–C) containing more active Fe2N8 sites has been synthesized. Interestingly, compared with typical FeN4 sites in an Fe–N–C electrocatalyst, the Fe2N8 sites generate a larger Fe–N bond length due to Co-doping. The elongated Fe–N bond in Fe2N8 lowers the d-band center and charge density of iron sites, enhancing the ORR process by facilitating the formation of *OOH and generation and desorption of *OH. Fe(tCo)–N–C manifested excellent acidic and alkaline ORR activity, with a half-wave potential (E1/2) of 0.80 V in HClO4 solution and 0.89 V in KOH medium. More importantly, high peak power densities (Pmax) were realized by applying Fe(tCo)–N–C in PEMFCs, with the Pmax reaching 890 mW cm−2 in H2–O2 and 380 mW cm−2 in H2–air. Additionally, trace Co dopants in the catalyst improved carbon graphitization and provided high ORR catalytic stability. This research introduces an innovative approach to engineering highly active Fe2N8 sites, providing valuable insights for the sustainable progress of PEMFC technology.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lingfeng Li,Yandi Wen,Guokang Han,Yuxin Liu,Yajie Song,Wei Zhang,Jia Sun,Lei Du,Fanpeng Kong,Yulin Ma,Yunzhi Gao,Jiajun Wang,Chunyu Du,Geping Yin
Developing advanced non-precious metal catalysts towards acidic oxygen reduction reaction (ORR) is critical for electrochemical energy conversion devices. Fe-N-C catalysts are demonstrated to be the most promising alternatives to platinum-based catalysts for ORR. Herein, Fe single atoms (SAs) coordinated by pyridinic nitrogen catalysts (denoted as Fe-pyridinic N-C) are synthesized through pyrolysis of ZIF-8 encapsulating ferrocene. Owing to the synergistic effects between Fe SAs and pyridinic N, Fe-pyridinic N-C exhibits remarkable ORR activity and outstanding stability in acid media, evidenced by golden kinetic current density of 9.71 mA cm −2 at 0.8 V, along with only 21 mV decrease in half-wave potential after 20,000 cycles. Theoretical calculations demonstrate that pyridine-type N possesses stronger binding energy with Fe SAs compared with pyrrole-type N, in other words, high pyridinic N content will help stabilize the catalyst. This study will be of great significance for the development of non-noble metal catalysts towards ORR with enhanced stability in acidic media.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2026
·
IF 5.9
Xiaofei Guo,Zhongyao Guo,Chen Wang,Candong Liu,Honghui Cheng,Kuikui Wang
The highly active and stable oxygen reduction reaction (ORR) process is essential for driving the development of zinc-air batteries (ZABs). Therefore, by integrating the precise regulation of precursors, the tannic acid (TA) etching and nitrogen coordination strategy, a nitrogen-rich hierarchical porous Fe-N-C catalyst was successfully constructed. The uniform dispersion of particles was achieved by controlling the formation of the Fe-ZIF-8 precursor. Subsequent TA etching formed a rich mesoporous/microporous structure to improve active-site exposure. During the high-temperature pyrolysis process with melamine as the nitrogen source, a highly dispersed Fe-N X coordination structure was formed. Based on this rational design, the obtained catalyst presents a hierarchical porous structure, high nitrogen content and superior ORR activity, with a half-wave potential of 0.91 V in 0.1 M KOH solution. When applied to liquid and flexible ZABs, the catalyst delivers peak power densities of 186 mW cm −2 and 75 mW cm −2 , respectively, and cycling stability of over 1486 h is maintained in the liquid system-surpassing the performance of commercial Pt/C + RuO 2 . This research offers a fresh perspective on the design and synthesis of efficient ND-FeNC-TA catalysts and promotes the practical application of ZABs.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Wan Xin,Liu Qingtao,Liu Jieyuan,Liu Shiyuan,Liu Xiaofang,Zheng Lirong,Shang Jiaxiang,Yu Ronghai,Shui Jianglan
Simultaneously increasing the activity and stability of the single-atom active sites of M–N–C catalysts is critical but remains a great challenge. Here, we report an Fe–N–C catalyst with nitrogen-coordinated iron clusters and closely surrounding Fe–N 4 active sites for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction is built between iron clusters and satellite Fe–N 4 due to unblocked electron transfer pathways and very short interacting distances. The iron clusters optimize the adsorption strength of oxygen reduction intermediates on Fe–N 4 and also shorten the bond amplitude of Fe–N 4 with incoherent vibrations. As a result, both the activity and stability of Fe–N 4 sites are increased by about 60% in terms of turnover frequency and demetalation resistance. This work shows the great potential of strong electronic interactions between multiphase metal species for improvements of single-atom catalysts.
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ANALYST
·
2020
·Vol. 146
·期 1
·207-212
·
IF 3.978
Wenjie Jing,Xiangkun Cui,Fanbo Kong,Wei Wei,Yunchao Li,Louzhen Fan,Xiaohong Li
Identifying the species and concentrations of antioxidants is really important because antioxidants play important roles in various biological processes and numerous diseases. Compared with an individual sensor detecting a single antioxidant with limited specificity, a sensor array could simultaneously identify various antioxidants, in which 3–5 types of nanomaterials with peroxidase-like activity are absolutely necessary. Herein, as a single-atom nanozyme, Fe–N/C with oxidase-mimicking activity was applied to construct a triple-channel colorimetric sensor array: (1) Fe–N/C catalytically oxidized three substrates 3,3′,5,5′-tetramethylbenzidine (TMB), 2,2′-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) (ABTS) and o-phenylenediamine (OPD) to produce blue oxidized TMB (oxTMB), green oxidized ABTS (oxABTS) and yellow oxidized OPD (oxOPD), respectively; (2) with oxTMB, oxABTS and oxOPD as three sensing channels, a colorimetric sensor array was constructed for simultaneously discriminating glutathione (GSH), L-cysteine (L-Cys), ascorbic acid (AA), uric acid (UA), and melatonin (MT), even quantifying concentrations (with GSH as a model analyst). The performance of the sensor array was validated through accurately identifying 15 blind samples containing GSH, L-Cys, AA, UA and MT in buffer solution and human serum samples, and also in binary and ternary mixtures. This work proved that fabricating a single nanozyme-based sensor array was a simplified and reliable strategy for simultaneously probing multiple antioxidants.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Xiaobin Zhou,Mengke Wang,Junyang Chen,Xiaolei Xie,Xingguang Su
Single atom nanozymes are the artificial enzymes with enzyme-like activity, which have attracted a great deal attention in recent years due to their unique merits such as remarkable stability, excellent atom utilization and low cost. Herein, a convenient and sensitive colorimetric strategy was developed for the sensing of galactose based on Fe–N–C single-atom nanozyme (Fe-SAzyme). The Fe-SAzyme was prepared through “isolation-pyrolysis” method that exhibited intrinsic peroxidase mimicking activity, which can quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to produce blue-colored oxTMB in the presence of hydrogen peroxide (H 2 O 2 ). Galactose can be oxidized by galactose oxidase (Gal Ox) to generate H 2 O 2 , and Fe-SAzyme can be utilized for quantitative colorimetric detection of galactose. A good linearity between absorbance and the galactose concentration in the range of 50–500 μM was obtained with a detection limit of (LOD) 10 μM. The Fe-SAzyme based colorimetric strategy offered a rapid, convenient and economic way for galactose quantification detection, which could be used as an alternative method for galactosemia diagnosis.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2023
·
IF 4.3
Qi Guo,Xiaorong Huang,Yajuan Huang,Zhaowei Zhang,Peiwu Li,Li Yu
Aflatoxin B 1 (AFB 1 ) is a prominent food contaminant known for its high toxicity. Rapid, low-cost, and sensitive detection of AFB 1 is an urgent demand for food safety risk control. In the traditional enzyme-linked immunosorbent assay (ELISA) method for AFB 1 detection, horseradish peroxide (HRP) is high-cost and possesses poor environmental stability. In this study, a direct competitive single-atom nanozymes (SAzymes) -linked immunosorbent assay was developed based on Fe-N-C SAzymes. The proposed methods exhibited excellent sensitivity, rapid detection, fabrication, and low cost. Under the optimal conditions, the limit of detection of the new assay was 3.3 pg mL −1 , with a quantitative relationship between 0.0084 and 0.358 ng mL −1 . In addition, the developed method presented good recoveries in spiked samples, ranging from 84.50% and 103.75%, with coefficients of variation below 10%. Furthermore, the developed detection method showed good consistency (R 2 = 0.9852) with the reference method, liquid chromatography/mass spectrometry (LC-MS/MS). To our knowledge, this is the first report about single-atom nanozymes-based ELISA for AFB 1 determination. This work provides a feasible strategy for the rapid and sensitive detection of food contaminants using SAzymes.
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