SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Mingyu Li,Chaoqun Li,Zhao Chunrui,Tianren Li,Jingjing Jiang,Zhonghui Han,Chongjun Zhang,Haoran Sun,Shuangshi Dong
Fe-based metal organic framework with high active site exposure, wide light absorption and fast H 2 O 2 activation are pivotal for photo-Fenton degradation of contaminants. However, insufficient active site exposure, weak visible light adsorption and low charge transfer efficiency in iron-oxo clusters usually lead to the slow Fe(II)/Fe(III) cycle. In this study, we develop a novel citric acid (CA)-modified MIL-88A(Fe) strategy to boost photo-Fenton efficiency by accelerating Fe(II)/Fe(III) cycle for emerging contaminants removal. Relationship between CA coordination mode and photo-Fenton performance was studied by using methylene blue (MB) and carbamazepine (CBZ) as model contaminants. It was found that the degradation rate constants of MIL-88A(Fe)-CA-3 were 6.5 and 2.6 times higher than those in the pristine MIL-88A(Fe) for MB and CBZ degradation, respectively. The optimized MIL-88A(Fe)-CA-3 also exhibited good recyclability, enabling multiple cycles in photo-Fenton reaction. The results of experimental characterizations and density functional theory calculations demonstrated that ligand substitution was conductive to active site exposure, visible light absorption, charge carrier transfer and Fe 2+ /Fe 3+ redox cycle, which are responsible for an improved photo-Fenton performance.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Science China-Chemistry
·
2020
·Vol. 63
·期 6
·810-817
·
IF 6.356
He Qian,Meng Yuying,Zhang Hao,Zhang Ying,Sun Qingdi,Gan Tao,Xiao Huajian,He Xiaohui,Ji Hongbing
Recently, nitrogen-doped porous carbon supported single atom catalysts (SACs) have become one of the most promising alternatives to precious metal catalysts in oxygen reduction reaction (ORR) due to their outstanding performance, especially those derived from porphyrin-based materials. However, most of them involve other metal residuals, which would cause the tedious pre- and/or post-treatment, even mislead the mechanistic investigations and active-site identification. Herein, we report a precursor-dilution strategy to synthesize Fe SACs through the Schiff-based reaction via co-polycondensation of amino-metalloporphyrin, followed by pyrolysis at high temperature. Systematic characterization results provide the compelling evidence of the dominant presence of atomically dispersed Fe-N x species. Our catalyst shows superior ORR performance with positive half-wave potential ( E 1/2 =0.85 V vs. RHE) in alkaline condition and moderate activity ( E 1/2 =0.68 V vs. RHE) under the acidic condition, excellent methanol tolerance and good long-term stability. All the results indicate Fe SACs would be a promising candidate for replacing the precious Pt in metal-air batteries and fuel cells.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yapeng Li,Qinghong Pan,Huiting Shi,Youyou Du,Ailing Yang,Da-Peng Yang
The quantitative determination of cholesterol in foods, drugs, and biological fluids holds significant importance due to its potential health risks. Herein, a self-powered photoelectrochemical (PEC) sensor was developed for cholesterol detection. The photoelectrochemical system was constructed by modifying fluorine-doped tin oxide (FTO) electrodes with ZnO/C (serving as the photoanode) and iron-modified CuBi 2 O 4 (denoted as CBFO, functioning as the photocathode) through a controlled deposition process. To enhance detection selectivity, molecularly imprinted polymers (MIPs) were electrodeposited on the photocathode surface. The optimized sensor exhibited a linear detection range of 1–1000 nmol L −1 and a detection limit of 0.26 nmol L −1 (S/N = 3). Practical application of the sensor for cholesterol detection in milk samples demonstrated satisfactory recovery rates (98.6 %–107 %) with relative standard deviations (RSD) ranging from 2.38 % to 4.25 %. These results underscore the potential of this self-powered PEC sensor as a robust platform for rapid and accurate cholesterol determination in food products, pharmaceuticals, and environmental samples.
研究领域:
分析化学
·
生物医学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH PART A-TOXIC/HAZARDOUS SUBSTANCES & ENVIRONMENTAL ENGINEERING
·
2021
·
IF 2.269
Peng Zhou
A new material, polyacrylic acid-b-polyptyrene (PAA-b-PS) covered Ni/Fe nanoparticles (PAA-b-PS-nZVI-Ni), was developed and evaluated for the selective dechlorination of 1,1,1-trichloroethane (1,1,1-TCA) in the presence of potential interferents. The average size of the PAA-b-PS coated Fe/Ni bimetallic nanoparticles was approximately 50 nm, which resulted from agglomeration prevention by PAA-b-PS. The removal efficiency of 1,1,1-TCA by an optimal dose with a 1.0 g/L Fe/Ni (Ni/Fe = 2 wt%) and 0.5 g/L PAA-b-PS-coated concentration was higher (87.5%) than that of bare Fe/Ni (60%). The pseudo-first-order rate constant (Kobs) of 1,1,1-TCA removal by PAA-b-PS-nZVI-Ni was 0.0142 min−1 within 240 min. Comparatively, the Kobs values of 1,1,1-TCA removal by other materials (Fe, pure bimetallic Fe/Ni, PAA-b-PS-Fe) were only 0.003, 0.0052 and 0.0103 min−1, respectively. The 1,1,1-TCA removal efficacy by PAA-b-PS-nZVI-Ni showed no obvious gap regardless of pH or various common inorganic anions (NO3−, HCO3− and SO42−) at different concentrations. However, humic acid (HA) had great influence on the degradation of 1,1,1-TCA. In conclusion, PAA-b-PS-covered Ni/Fe nanoparticles with its selectivity high effectiveness could be used as one remedial agent for the degradation of 1,1,1-TCA in water.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 21
·8952-8959
·
IF 3.288
Hehe Qin,Jinhong Fan,Shun Mao
The Fenton method is an important water treatment process. However, the mechanism of the Fenton reaction is still not widely recognized. In this article, the autocatalysis process responsible for the degradation of 4-chlorophenol (4-CP) as well as the generation of Fe(II) and the decomposition of H2O2 is elaborated using a Fe(III)/H2O2 system. It was found that the one electron reduction of Fe(III) to Fe(II) via oxidization of H2O2 to ˙HO2 is not spontaneous according to the standard electrode potential rather than being limited by the rate constant of 0.0027 M−1 s−1 in view of the Haber–Weiss circulation. However, the reaction of Fe(III) and 4-CP is spontaneous with a second-order kinetic rate constant of >0.12 M−1 s−1 and a conversion rate of 0.56%, which triggers the switch of the Fenton-like reaction as a real rate-determining step. The circulation of Fe(III) to Fe(II) in the proposed Fenton-like reaction mechanism depends on the organic species and various intermediates, which indicates its reaction selectivity, preferable for organics with a stronger thermodynamic and kinetic activity. Besides, a slight pH decline with time-scale and the stoichiometric ratio of ˙OH to H2O2 and H2O2 to 4-CP being 1 and 2, respectively, pointed to the new proposed reaction mechanism. The discovery of the new reaction mechanism might promote the theoretical and technical advancement of the Fenton-like process.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Yibo Tang,Ying Lei,Kang Tong,Tong Yang,Tiantian Fu,Yang Xiang,Shulin Zhang,Yujun Si,Chaozhong Guo
Fe, N-doped graphene-like carbon layers-wrapped carbon black composite (L-Fe-AD+C) was developed by pyrolyzing the mixture of Fe-adenine precursors and conductive carbon black as an efficient catalyst to oxygen reduction reaction (ORR). Graphitic N sites with more ORR activity are preferentially formed due to the facilitation of metallic Fe. Furthermore, graphene-like ultra-thin networks wrapped around nanoparticles of carbon black greatly increase the exposure of active sites and construct continuous diffusion channels favorable for the transfer of substances. As a result, the as-prepared L-Fe-AD+C exhibits an excellent ORR activity in alkaline electrolyte with a high half wave potential (0.88 V), and superior selectivity together with admirable stability, which are comparable to those of the benchmark Pt/C catalyst. More encouragingly, the L-Fe-AD+C can serve as an efficient cathode catalyst in a zinc-air battery, which reaches a peak power density of 221 mW cm −2 approximating to that of Pt/C catalyst (236 mW cm −2 ). The battery also shows a steady discharge voltage plateau of 1.26 V and specific capacity of 799 mAh g −1 at a discharge current density of 10 mA cm −2 . The results suggest the considerable potential of the L-Fe-AD+C catalyst to replace precious metal catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nano Research
·
2020
·Vol. 13
·期 8
·2079-2084
·
IF 8.183
Wang Hong-Hui,Lv Li-Bing,Zhang Shi-Nan,Su Hui,Zhai Guang-Yao,Lei Wei-Wei,Li Xin-Hao,Chen Jie-Sheng
The rational design of highly active and stable atomically dispersed M-X 4 (M = Fe, Co, Ni, etc., X = C, N) -based catalysts holds promises for wide application in almost all realms of catalysis. Despite great effort in the construction of specific M-X 4 centers, the possible effect of non-coordinated heteroatoms on the catalytic activity of metal centers has been rarely explored. Herein, we develop a new type of M-X 4 catalyst composed of Fe-N 4 centers and non-coordinated B heteroatoms (FeNC+B) and find the key role of non-coordinated B adjacent to Fe-N 4 centers in tailoring their electron density and final catalytic selectivity. The experimental and theoretical results demonstrated that non-coordinated boron atoms could decrease the electron density of Fe-N 4 centers to a suitable level and thus boost the selective production of nitriles from amine oxidation by depressing the formation of imines due to the flattened energy barrier of the reversible conversion of imines back to amines. As a reusable heterocatalyst, the state-of-the-art FeNC+B catalyst provides a turn-over frequency (TOF) value of 21.6 mol benzonitrile ·mol Fe −1 ·h −1 (100 °C), outpacing that of bench-marked nonnoble-metal-based homogeneous catalyst by a factor of 3.4.
研究领域:
催化化学
·
材料科学
·
理论化学
✓ 已验证
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·
IF 4.3
Ruosong He,Yang Wang,Meng Li,Jianxin Liu,Yongqiang Gu,Wenhang Wang,Qiang Liu,Noritatsu Tsubaki,Mingbo Wu
Graphical Core-shell structured Fe-based catalyst Na−Fe 3 O 4 @C with confinement effect delivered higher productivity of light olefins compared with the naked Na−Fe 2 O 3 counterpart. Multiple characterization and DFT calculation verified that the timely carbon chain-growth termination, as well as unique CO 2 /H 2 ratio and electronic property on the catalytic interface played vital roles in boosting light olefins synthesis. Even though Fe-based catalysts have been widely employed for CO 2 hydrogenation into hydrocarbons, oxygenates, liquid fuels, etc., the precise regulation of their physicochemical properties is needed to enhance the catalytic performance. Herein, under the guidance of the traditional concept in heterogeneous catalysis-confinement effect, a core-shell structured catalyst Na−Fe 3 O 4 @C is constructed to boost the CO 2 hydrogenation performance. Benefiting from the carbon-chain growth limitation, tailorable H 2 /CO 2 ratio on the catalytic interface, and unique electronic property that all endowed by the confinement effect, the selectivity and space-time yield of light olefins (C 2 = −C 4 = ) are as high as 47.4 % and 15.9 g mol Fe −1 h −1 , respectively, which are all notably higher than that from the shell-less counterpart. The function mechanism of the confinement effect in Fe-based catalysts are clarified in detail by multiple characterization and density functional theory (DFT). This work may offer a new prospect for the rational design of CO 2 hydrogenation catalyst.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
PubMed
高影响因子
Desalination and Water Treatment
·
2024
·
IF 1
Jianqing Ma,Ziheng Huang,Hao Xi,Yuezhong Wen
ABSTRACT Metal-doping graphitic carbon nitride (g-C 3 N 4 ) is a potential catalyst for the Fenton-like reaction. Selecting an appropriate supporter for this material is essential to improve its catalytic ability and lower the costs. Three common supporters, graphite, activated carbon, and SBA-15, were employed to investigate their effects on the catalyst structure and performances. Results show that graphite could increase the active Fe–N centers due to geometric effects and promote the electron transfer by π–π stacking, and therefore, the Fe-doping g-C 3 N 4 /graphite (FegN/G) composite displayed excellent catalytic ability for the bisphenol A (BPA) removal. In addition, magnetic catalyst was further fabricated through a simple coprecipitation method using Fe 3 O 4 and chitosan-Fe hydrogel. The magnetic catalyst kept in dozens of micrometer size range as well as high activity for the Fenton reaction. Hydroxyl radicals were generated during the reaction process, and 99.9% of the original BPA was therefore degraded and mineralized in 1 h. More importantly, it also exhibits a good reusability and stability, as well as a quick separation performance from the solution when using a magnet, indicating that this magnetic FegN/G composite would be a promising Fenton-like catalyst in practical applications.
研究领域:
环境科学
·
催化材料
·
化学工程
✓ 已验证
DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2020
·
IF 7.182
Lumin Chen,Houyong Yu,Christopher Deutschman,Ting Yang,Kam Chiu Tam
We report a facile method to prepare a novel composite based on Fe-Cu alloy decorated cellulose nanocrystals (Fe-Cu@CNC) via simple oxidation-reduction reaction. Spherical zero-valent iron nanoparticles (NZVI) and sheet-like copper nanoparticles were serially anchored on the CNC surface, and the generated composite exhibited excellent antibacterial activities and highly efficient Pb 2+ removal. The composites had high antibacterial ratios of 95.9 %–99.9 %, because superoxide radicals can cause irreversible damage to the bacteria, eventually leading to apoptosis and bacterial death. Meanwhile, the Fe-Cu@CNC composite showed quick Pb 2+ ion removal, reaching a 70.76 % removal within 5 min, a total removal of 93.98 % after 1 h, and excellent reusability (retaining removal efficiency of 80.41 % after six cycles). The adsorption kinetics demonstrated that the adsorption behavior can be described by pseudo-second-order kinetic model (R 2 >0.99). This study offers a new strategy to prepare a promising composite with advanced antibacterial and heavy metal removal properties for wastewater treatment.
研究领域:
材料科学
·
环境科学
·
生物学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Mang Ma,Anuj Kumar,Danni Wang,Yiyan Wang,Yin Jia,Ying Zhang,Guoxin Zhang,Zifeng Yan,Xiaoming Sun
Atomically dispersed metal-nitrogen-carbon complexes on carbon supports have drawn tremendous attention in the electrocatalysis fields. Herein, we managed the synthesis of atomically dispersed binary Ni x Fe 100-x -NC (x = 0–100) materials with tunable Ni/Fe ratios and investigated their underneath synergy effects for the enhancement of oxygen reduction (ORR) and oxygen evolution reactions (OER). EXAFS revealed the abundant presence of Ni(N 3 )-Fe(N 3 )-C n moieties in Ni 66 Fe 34 -NC sample. XPS fine scans indicated deep synergy of dual-site Ni/Fe that favored more charge localized over Ni/Fe sites. Electrochemical measurments showed that the Ni 66 Fe 34 -NC delivered a very high ORR half-wave potential ( E 1/2 ) of 0.85 V and a low OER overpotential of 467 mV at ∼10 mA cm −2 ( E j=10). The Fe site with Ni neighboring, as suggested by DFT simulations and in-situ Raman, was the responsible site for both ORR and OER. Furthermore, the Ni 66 Fe 34 -NC-assembled Zn-air battery afforded large specific power density and extraordinary cycling stability.
研究领域:
电催化
·
材料科学
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Shijiang Feng,Rong Qiang,Yulong Shao,Lei Rong,Fangjie Ren,Na Xiao,Siyuan Zhang,Zheng Guo,Caihong Chen,Qing Miao
The construction of hollow structures and the incorporation of metal nanoparticles have been shown to be two potential approaches to achieving high-performance microwave absorption. In this study, a hollow polyhedron material featuring an FeN/Fe-doped carbon matrix was synthesized by an acidification corrosion and pyrolysis strategy. The formation of heterojunctions, coupled with the design of hollow structures, significantly improved the dielectric loss capacity of the material. Furthermore, the incorporation of magnetic metal nanoparticles not only increased the magnetic loss but also enriched the loss mechanisms of the material, leading to an overall improvement in the magnetic loss. Under the synergistic effects of these factors, the material exhibited exceptional microwave absorption properties. In particular, at a material thickness of only 2.3 mm, the minimum reflection loss value of the FeN/Fe@HC nanocomposite reached −64.5 dB with an effective absorption bandwidth of 5.1 GHz. These results further highlight the importance of a hollow structure design and metal atom doping in improving microwave absorption performance.
研究领域:
材料科学
·
电磁学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）