SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Xiaoling Ma,Wenlong Wang,Chenggong Sun,Hui Li,Jing Sun,Xin Liu
In light of the promising merits of large surface area, uniform pore size, and tunable functional groups, metal-organic frameworks (MOFs) have great potential to be utilized for adsorbing volatile organic compounds (VOCs). In this study, three Fe-based MOFs, MIL-100(Fe), MIL-101(Fe), and MIL-53(Fe), were synthesized systematically and used to adsorb a typical VOC, toluene. Static adsorption, dynamic breakthrough curves , and adsorption kinetics were conducted to assess the adsorption performance. Additionally, the surface functional groups, pore structure, and morphology were systematically characterized by means of XRD , SEM, XPS, FTIR and N 2 adsorption-desorption analyses to reveal the cause of the difference in adsorption of these Fe-based MOFs. The results revealed that the maximum equilibrium adsorption capacity of 663 mg/g was achieved by MIL-100(Fe) with the highest specific surface area and pore volume. The dynamic adsorption of toluene on MIL-100(Fe) was in accordance with the pseudo-first order kinetic model and the Langmuir isothermal model. The formed π-π stacking interaction between organic ligands and the benzene ring in the MIL-100(Fe) cluster is the primary adsorption mechanism based on XPS analysis. Moreover, MIL-100(Fe) was easily regenerated via microwave irradiation with a negligible adsorption capacity decrease after three cycles. This work highlights the feasibility of hierarchical porous Fe-based MOFs as toluene adsorbents and promotes the application of MOFs in the field of pollution control .
✓ 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.
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yi-Ran Li,Ying-Ming Li,Bing-Bing Chen,Wen-Juan Hu,De-Yi Wang
Ideal electromagnetic absorbing material should not only be light weight, broadband and high efficient, but also easily prepared and flame-retarding to satisfy the challenges from rapid development of electronic information technology. In present paper, a new type of electromagnetic absorbent (Fe-MOF-rGO) was prepared via a simple one-pot method to grow metal-organic framework (Fe-MOF) on the surface of in-situ reduced graphene oxide (rGO) by solvothermal method. When 25 wt% of Fe-MOF-rGO was incorporated into the paraffin matrix, the minimum reflection loss value (RL) reached to −43.6 dB at the thickness of 2 mm, and the effective absorption bandwidth (EAB) exceeded 5.0 GHz, which satisfied the goals of high efficiency, light weight and broadband. According the medium permittivity loss, magnetization loss and excellent resistance matching results, it was concluded that the conduction loss (excellent conductivity of rGO), magnetic loss (magnetic resonance of Fe nanoparticles) and interface polarization loss (heterostructure of two-dimensional rGO and three-dimensional Fe-MOF) of Fe-MOF-rGO jointly determined the electromagnetic absorbing performance. Moreover, the combustible behavior of Fe-MOF-rGO was also investigated. When 10 wt% of Fe-MOF-rGO was incorporated into the epoxy resin (EP), the heat release capacity (HRC) and peak heat release rate (PHRR) decreased by 42.1% and 42.3% respectively, which showed an excellent flame-retarding property.
✓ 已验证
DOI
高影响因子
Environmental Science-Nano
·
2024
·Vol. 11
·期 7
·3092-3103
·
IF 5.8
Manoj Kumar Panjwani,Feiyu Gao,Ting He,Pan Gao,Feng Xiao,Shaoxia Yang
M–Nx single-atom catalysts (SACs) with a high coordination number (x > 4) are effective catalysts for eliminating organic pollutants, while the origin of SACs with high activity still remains elusive. In this work, we successfully synthesized an Fe–N5 SAC with axial N coordination, which exhibited exceptional catalytic performance by peroxymonosulfate (PMS) activation for degrading 4-chlorophenol (4-CP) in a wide pH range (4.0–10.0). The rate constant of Fe–N5 (2.99 min−1) was 6.36 times higher than that of Fe–N4, and the turnover frequency (TOF) of Fe–N5 was found to be 4–149 times higher than those of state-of-the-art SACs and nanocatalysts reported in the literature for 4-CP degradation by PMS activation. Moreover, Fe–N5 was not significantly affected by coexisting substances (HA, HCO3−, SO42−, H2PO4−, NO3−, and Cl−) and had satisfactory degradation efficiency for various chlorophenols. Electron paramagnetic resonance (EPR), quenching experiments, and radical probe experiments demonstrated that 1O2 played a key role in the Fe–N5/PMS system for 4-CP degradation. Density functional theory calculations confirmed that a narrower gap between the Fe-3d band center and Fermi level enhanced the electron transfer in Fe–N5, which resulted in promoted PMS activation. In addition, the Fe–N5/PMS system showed good potential for application in real wastewater. The above findings offer important implications for the future of coordination chemistry in designing M–Nx–C SACs (x > 4), highlighting their practical applications in environmental remediation.
✓ 已验证
DOI
高影响因子
Nano Energy
·
2018
·
IF 13.12
Li An,Jianrui Feng,Yu Zhang,Yong-Qing Zhao,Rui Si,Gui-Chang Wang,Fangyi Cheng,Pinxian Xi,Shouheng Sun
Transition-metal nitrides (TMNs), especially iron-based TMNs, have high electrical conductivity , superior chemical stability and unique oxygen-reaction ability, and have emerged as a new form of noble metal-free electrocatalysts . In this paper, we demonstrate that the ORR-active/OER-inert single function catalyst Fe-N can be made as the OER/ORR-active bifunctional catalyst Co-Fe-N by controlled substitution of Fe with Co. To obtain atomic insights of the Co-enhanced OER catalysis, we develop a new exfoliation method to prepare atomically thin (1.1 nm) nanosheets (NSs) of Co x Fe 1-x N 0.5 (x = 0, 0.05, 0.1, 0.15 and 0.2). Our studies show that both electronic structure and local binding environment of Fe are modified by Co substitution and the Co-Fe-N NSs show a volcano−like OER catalysis with Co 0.15 Fe 0.85 N 0.5 NSs being the most efficient OER catalyst, showing the lowest overpotential of 266 mV at 10 mA cm −2 , a Tafel slope of ∼30 mV dec −1 , and excellent stability in the 1.0 M KOH OER condition. Density functional theory (DFT) calculations suggest that the Co-Fe sites in the Co 0.15 Fe 0.85 N 0.5 structure are optimized to promote OH* to O* conversion, O*-O* coupling and O 2 formation. The Co 0.15 Fe 0.85 N 0.5 NSs are a class of new noble-metal-free catalyst for OER.
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Mengyang Xu,Bingqing Chang,Jinze Li,Huiqin Wang,Pengwei Huo
The assembly of different Metal organic framework (MOFs) into hybrid heterostructures has proven to be a promising strategy that can effectively break through the limited regulatory capacity of single metal sites. Here, an S-scheme heterostructure (Fe 3 Ni-MOF) based on homologous ligands (1,4-phthalic acid) of ultra-thin Ni-MOF and Fe-MOF nanoparticles with directional electron transport channels, was developed and used it for photoreduction of CO 2 . Under the S-scheme electric field mechanism, the photogenerated carrier can achieve efficient directional separation through Fe–O–Ni atomic bond, which significantly reduces the energy barrier of the rate-determining step. Results show that the performance of Fe 3 Ni-MOF (63.5 μmol g –1 ) was 20 and 3.2 times higher than that of Ni-MOF and Fe-MOF, respectively, and exhibits excellent CO selectivity (96.4%) and stability. Transmission electron microscopy and atomic force microscopy revealed the two-molecular-layers structure of Ni-MOF and the micro-assembly structure of Fe 3 Ni-MOF, which can shorten the electron transport distance and increase the molecular mass transfer rate. X-ray photoelectron spectroscopy, electron spin resonance and electron density difference calculations reveal that interfacial electric fields and atomic bonds work together to promote directional carrier separation, resulting in the accumulation of holes on Ni-MOF and electrons on Fe-MOF. The Gibbs free energy calculation and in-situ Fourier transformed infrared spectroscopy validate that the micro-assembled S-scheme heterostructures with directional electron transport channels can significantly reduce the activation energy barrier of the reaction. This study not only proves the feasibility of constructing MOFs S-scheme heterostructures using homologous ligands, but also provides a new way to overcome the limitations of monometallic MOFs. This strategy is expected to open up a new avenue to design efficient photocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Junpu An,Hongchen Liu,Fan Yang,Kexin Wei,Chunhui Yu,Siyuan Sun,Yang Sun,Qing Guo,Jianfeng Wang,Chenlin Wang,Jiahui Liu,Kuobo Wang,Yongfeng Li
Nickel-based catalysts show great potential as promising candidates for the electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF). However, the limited adsorption capacity of nickel-based catalysts for OH – and HMF limits their further development. In this study, amorphous Fe/NiOOH-SO x was generated from nanosheets (Fe/NiOOH-Ni 3 S 2 ), which was pre-fabricated on nickel foam via pre-reconstruction and anionic regulation strategy. The optimized catalyst Fe/NiOOH-Ni 3 S 2 demonstrated exceptional activity in the HMF oxidation reaction (HMFOR) with a current density of 10 mA cm −2 at 1.32 V vs RHE, accompanying with the 98.9 % HMF conversion, 97.8 % 2,5-Furandicarboxylic acid (FDCA) selectivity, 96.8 % Faraday efficiency, and stability for ten cycles. The incorporating amorphous FeOOH reduces the electron density around Ni, promoting the formation of high-valent Ni spices. Meanwhile, the SO x combined with amorphous hydroxy nickel oxide provides unsaturated sites, which enhances the adsorption capacity of HMF. Density functional theory (DFT) computations reveal that the designed amorphous Fe/NiOOH and surface-adsorbed SO x collectively modulate the electronic structure of the catalyst, causing an upwards shift of the NiOOH d-band center and enhancing adsorption capacities for both HMF and OH – . This study proposes the adsorption enhancement mechanism of regulating electronic structure and offers a rational strategy for HMFOR electrocatalysts.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Ruoyi Chen,Fuding Tan,Xiang Wang,Yuxin Hou,Ming Ouyang,Xingyun Guan,Peng Liu,Zuliang Wu,Shuiliang Yao,Steven L. Suib,Daiqi Ye
The transportation and transformation of biogenic isoprene are vital for the organic carbon cycle in the troposphere. As a typical mineral with high oxidation potential, Fe-substituted cryptomelane oxidizes the surface monolayer of isoprene into formic and acetic acids, and simultaneously, the Mn4+ ions in the structure are reduced to Mn3+ and Mn2+. The flow of H2O in isoprene decreases the adsorption and oxidation of isoprene significantly, even at low relative humidity (10%). As physisorbed H2O retains Fe-substituted cryptomelane’s crystal structure and oxidation ability, the adsorption and oxidation capacity recovers when H2O is absent in the isoprene flow. Theoretical calculations on (001) surfaces show that isoprene prefers to be adsorbed by the Fe3+ site and H2O tends to form hydrogen bonds. Due to the decrease in total adsorption energy of H2O and isoprene, Fe-substituted cryptomelane favors the adsorption of H2O in the flow of humid isoprene. The low oxidation performance at ambient relative humidity suggests that direct oxidation by aerosols of mineral dust might not be the transformation pathway of biogenic isoprene at night.
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·Vol. 108
·期 7
·e20447
·
IF 3.8
Mingyang Zhao,Xiao Chen,Huiping Zhu,Songqin Xia,Yan Ma,Kyle S. Brinkman,Zhenfeng Tong
This study systematically explored the crystal chemistry of Fe-substituted hollandite (Fe-hollandite) solid solutions (Ba x Cs y )(Fe 2 x + y Ti 8−2 x − y )O 16 ( x + y = 1.33) yielding reliable results through meticulous Rietveld analysis of XRD data. Continuous Cs substitution triggered a monoclinic-tetragonal (M-T) phase transition, enhancing structural stability, as evidenced by increased tolerance factor ( t H ). The transition boundary, controlled by t H = .985, determines the symmetry of the hollandite phase. Unit cell parameters and the local bonding environment were refined, indicating enlarged tunnel sizes/cavities with higher Cs content, attributed to a larger ionic radius (Cs + vs. Ba 2+ ). Comparison between Cs/Ba-O bond distances and tunnel cross-section sizes confirmed effective A-site cation immobilization, hindered by oxygen bottlenecks. Additionally, a refined model was proposed and validated to predict lattice constants of Fe-hollandite precisely. Beyond crystal chemistry evolution with Cs substitution, leaching resistance in the same sample suites was assessed. As Cs content increased, normalized elemental release of A-site cations initially decreased until reaching a minimum at intermediate Cs substitution, then rose again. Ba 0.33 Cs 1.0 Fe 1.66 Ti 6.34 O 16 (i.e., HF5) displayed optimal leaching resistance. Variations in leaching resistance might be influenced by the distortion in [BO 6 ] octahedra and the bonding environment of tunnel cations. This comprehensive analysis highlights intricate correlations between crystal chemistry and leaching resistance, offering insights to guide the design of advanced crystalline nuclear waste forms with enhanced corrosion resistance.
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2025
·
IF 15.6
Jun Mao,Huan Liu,Yanan Li,Meng Gao,Yunlong Zhang,Yao Song,Mo Zhang,Guilan Xu,Wu Zhou,Liang Yu,Xiaoju Cui,Dehui Deng
The oriented conversion of CH4 to CH3COOH at low temperature, even room temperature, is both scientifically significant and industrially applicable for CH4 utilization, yet it is extremely challenging due to the difficulties associated with efficient CH4 activation and controllable C–C coupling. In this study, we for the first time achieve the room-temperature conversion of CH4 to CH3COOH using molecular O2 and CO over MoS2-confined Rh–Fe sites, which delivers an unprecedented CH3COOH selectivity of 90.3% and a productivity of 26.2 μmol gcat.–1 h–1 at 25 °C. Furthermore, the productivity of CH3COOH can be enhanced to 105.6 μmol gcat.–1 h–1 at 80 °C, while maintaining a high selectivity of 95.6%. Comprehensive experimental and theoretical investigation reveal the critical role of Rh–Fe synergy in the selective formation of CH3COOH. The confined Fe sites in MoS2 enable the activation of O2 to generate highly reactive Fe═O center for CH4 dissociation to CH3 species at room temperature, which then readily couple with adsorbed CO on adjacent Rh sites to form the key CH3CO intermediate for CH3COOH production. The unique structure of Rh–Fe sites offers synergistic catalytic properties that effectively balance C–H activation and C–C coupling, successfully addressing the trade-off between activity and selectivity in the carbonylation of CH4 to CH3COOH under mild conditions.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CARBON
·
2025
·
IF 11.6
Lianzhong Shen,Lin Wang,Zhouwei Li,Yu Ye,Qizhou Dai
Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts are one of the more popular materials for electrochemical reduction of CO 2 to fuels and chemicals. Still, their Faraday efficiency and current density are generally low due to the single coordination environment and defect sites. Heteroatom doping has been demonstrated to increase the degree of defects in the material, improve the electron distribution at the single atomic sites, and enhance the catalytic performance. In this study, we prepared an S-doped single-atom catalyst called FeS@PC by a simple high-temperature pyrolysis method for efficient electroreduction of CO 2 to CO, with a maximum CO Faraday efficiency of 97.0% at -0.6 V vs. RHE potential. S atoms doped in the second-shell can change the electron distribution on the Fe-N 4 sites and accelerate the electron transfer during the electrochemical CO 2 reduction reaction (CO 2 RR). Through in situ ATR-FTIR characterization and kinetic experiments, it is found that the doped S can also promote the dissociation of H 2 O, provide sufficient protons for the conversion of CO 2 to *COOH, and promote the rate of CO conversion.
✓ 已验证
产品关联
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.
✓ 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）