EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2024
·Vol. 27
·期 24
·e202400196
·
IF 2.2
Wenkang Mao,Jinjing Ju,Dan Li,Daishe Wu,Feigao Xu
Graphical Synopsis: A pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) framework is synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. M/PN-g-C 3 N 4 are constructed for peroxodisulfate activation. The synergy between photocatalysis and Fe/PN-g-C 3 N 4 catalyst results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe 3+ /Fe 2+ couple. Photocatalysis is an efficient technology for the degradation of pollutants. However, there is still much room for improvement in its degradation efficiency. In this study, a pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) framework was synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. Then, a series of single atomic metals M anchored to PN-g-C 3 N 4 (M/PN-g-C 3 N 4 ) are constructed for peroxodisulfate activation. Their order of catalytic activity follows Fe>Cr>Ni>Cu≈Co>Mn, in particular the degradation rates of the TCH for Fe-PN-g-C 3 N 4 are 3.74 times higher than that of undoped PN-g-C 3 N 4 . These carefully regulated pyrrolic N-rich Fe sites demonstrate outstanding performance in degrading organic pollutant. As an exemplary model, the Fe/PN-g-C 3 N 4 catalyst efficiently drives the catalytic oxidation of TCH through Fenton-like reaction under visible light, showcasing exceptional cycle stability and a broad effective pH range of 3.0–11.0. The synergy between photocatalysis and Fe doped catalysis results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe 3+ /Fe 2+ couple. This combination significantly enhances the Fenton-like performance, making it a highly effective process for pollutant degradation.
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Science Advances
·
2022
·Vol. 8
·期 40
·
IF 14.957
Jingzhong Qin,Bo Han,Xixi Liu,Wen Dai,Yanxin Wang,Huihui Luo,Xiaomei Lu,Jiabao Nie,Chensheng Xian,Zehui Zhang
The cleavage and functionalization of recalcitrant carbon─carbon bonds is highly challenging but represents a very powerful tool for value-added transformation of feedstock chemicals. Here, an enzyme-mimic iron single-atom catalyst (SAC) bearing iron (III) nitride (FeN 3 ) motifs was prepared and found to be robust for cleavage and cyanation of carbon–carbon bonds in secondary alcohols and ketones. High nitrile yields are obtained with a wide variety of functional groups. The prepared FeN 3 -SAC exhibits high enzyme-like activity and is capable of generating a dioxygen-to-superoxide radical at room temperature, while the commonly reported FeN 4 -SAC bearing FeN 4 motifs was inactive. Density functional theory (DFT) calculation reveals that the activation energy of dioxygen activation and the activation energy of the rate-determining step of nitrile formation are lower over FeN 3 -SAC than FeN 4 -SAC. In addition, DFT calculation also explains the catalyst’s high selectivity for nitriles.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2023
·Vol. 34
·期 4
·1751-1764
·
IF 4
Zhou Zhuyou,Zou Congyang,Wang Yong,Liu Menghe,Ji Yufeng
A one-step solvothermal synthesis technique was employed to fabricate C 60 /MIL-101(Fe) composites. The C 60 /MIL-101(Fe) composites showed a better performance in the degradation of methylene blue (MB) and tetracycline hydrochloride (TCH) when compared to MIL-101(Fe) in the photo-Fenton system, which can be credited to the charge transfer and separation facilitated by the addition of C 60 . Results showed that C 60 /MIL-101(Fe) had the capacity to nearly completely eliminate TCH and MB over a broad pH range. The catalysts demonstrated remarkable catalytic degradation on various organic pollutants and water samples. Through active substance quenching experiments and EPR, it was determined that hydroxyl radical (·OH) is the main factor in the photocatalytic reaction process.
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ANALYST
·
2013
·Vol. 138
·期 16
·4526-4531
·
IF 3.969
Ya Li Liu,Xi Juan Zhao,Xiao Xi Yang,Yuan Fang Li
In this paper, a nanosized porous metal–organic framework, Fe-MIL-88NH2, was facilely prepared with a uniform octahedral shape by the addition of acetic acid, and for the first time was demonstrated to possess intrinsic peroxidase-like activity. Kinetic analysis and electron spin resonance measurements indicated that the catalytic behavior was consistent with typical Michaelis–Menten kinetics and follows a ping-pong mechanism. As a novel peroxidase mimic material, Fe-MIL-88NH2 shows the advantages of high catalytic efficiency, ultrahigh stability and high biocompatibility in aqueous medium compared with natural enzymes and other peroxidase nanomimetics. Here, Fe-MIL-88NH2 was used to quickly catalyze oxidation of the peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 to produce a colored product, which provided a simple, sensitive and selective method for the colorimetric detection of glucose. Glucose could be linearly detected in the range from 2.0 × 10−6 to 3.0 × 10−4 M with a detection limit of 4.8 × 10−7 M, and the color variation for glucose response was also obvious by visual observation at concentrations as low as 2.0 × 10−6 M. More importantly, the colorimetric method could be successfully applied to the determination of glucose in diluted serum samples.
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npj Clean Water
·
2025
·Vol. 8
·期 1
·1-17
·
IF 11.4
Xu Dan,Cao Xiaolin,Zhou Jie,Lin Zhihao,Wang Jing,Han Jiatong,Chen Ge,Liu Guangyang,Xu Xiaomin,Zhang Yanguo,Xu Donghui
To address the environmental threats posed by dye pollution, it is crucial to develop adsorbents with high selectivity and adsorption capacity for the removal of chemical dye pollutants. In this study, five types of Ni/Fe-MOFs were synthesized via a one-pot solvothermal method by varying the Ni/Fe molar ratio. Their physicochemical structures, surface morphologies, and compositions were characterized through a series of techniques, and their adsorption performances for different dyes were preliminarily investigated. The results demonstrated that the Ni/Fe ratio significantly affects the microstructure and adsorption performance of the MOFs. As the molar ratio of Ni/Fe increased, the structures of the five materials transformed from nanoflowers (Fe-MOFs) to nanospheres (Ni/Fe(3:1)MOFs) , and eventually to rhombic blocks (Ni-MOFs) . The specific surface area decreased from 281.3 m²/g (Fe-MOFs) to 67.11 m²/g (Ni/Fe(1:1)MOFs) and further to 0.5369 m²/g (Ni-MOFs) . XPS analysis confirmed the synergistic coordination between Ni and Fe, and FT-IR spectra revealed characteristic peaks for hydroxyl groups on the MOF surface and carboxylate ligands. XRD analysis indicated that materials with higher Ni content were more prone to ligand decomposition, which is consistent with the weight loss observed in the TG-DSC between 230 and 350 °C. The materials exhibited selective adsorption for different dyes. Under optimal conditions, the maximum adsorption capacities for Eosin Y (EY), Neutral Red (NR), and Acid Fuchsin (AF) were 54.92 mg/g (Fe-MOFs) , 636.31 mg/g (Ni-MOFs) , and 79.30 mg/g (Ni/Fe(1:1)MOFs) , respectively. The adsorption kinetics followed a pseudo-second-order model, and the adsorption isotherms conformed to the Langmuir model, while Fe-MOFs and Ni/Fe(1:1) MOFs also exhibited compatibility with the Freundlich model. The adsorption mechanism primarily involved monolayer adsorption as the dominant process, with localized multilayer adsorption, as well as chemisorption, hydrogen bonding, hydroxyl interactions, and electrostatic interactions. These MOFs demonstrated high dye removal efficiency in actual water samples and fruit and vegetable juices, exhibiting excellent reusability and anti-interference capabilities. Importantly, compared with the single system, Fe-MOFs and Ni/Fe(1:1)MOFs exhibit competitive adsorption, and Ni-MOFs exhibit synergistic adsorption in the binary system. This study confirms that by adjusting the Ni/Fe molar ratio, MOFs with high selectivity and adsorption performance for different dyes can be designed, providing new theoretical insights and technical support for environmental remediation and food safety applications.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Sleshi Fentie Tadesse,Worku Lakew Kebede,Dong-Hau Kuo
Visible-light-driven photocatalysis is an efficient and environmentally benign approach to mitigate organic pollutants from waste effluents. A facile one-step precipitation method was used to synthesize Fe–Mo3(O,S)4−x/La4Mo2O11 (FeLaMoOS) nanocomposites. The as-prepared materials were characterized by XRD, SEM, HR-TEM, XPS, PL, EIS, photocurrent, and UV-visible spectroscopy. The type I heterojunction formed between Fe–Mo3(O,S)4−x and La4Mo2O11 exhibited a maximum light absorption response in the visible spectrum. The FeLaMoOS composite (13% Fe and 20% La) demonstrated the highest degradation efficiency, degrading 97.5% MO and 99.2% RhB in 90 min. The removal efficiency of MB was 99.6% after 45 min of magnetic stirring in the dark. The enhanced catalytic efficiency can be attributed to the effective charge separation of photoinduced e−–h+ pairs due to doping and heterojunction formation. Superoxide radicals (O2˙−) played a dominant role, while hydroxyl radicals (˙OH) played only a minor role, in the photocatalytic degradation process. Possible photocatalytic degradation mechanisms of organic dye molecules were proposed, based on the active radical species involved and the band potentials of the photocatalysts. This study can be used to establish a simple and efficient strategy for designing reusable composite photocatalysts for the degradation of organic dyes.
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ACS Applied Nano Materials
·
2025
·
IF 5.5
Xudong Zhao,Shuibo Wang,Hua Li,Yushi Wei,Yiming Li,Haocheng Li,Hongbo Yu,Kaijie Li,Haotian Li,Hongfeng Yin
Preventing nanoparticle migration and agglomeration on the surface of supported heterogeneous catalysts, especially at tailored bimetallic sites, poses a significant challenge. The reverse water–gas shift (RWGS) reaction is considered a promising route for converting CO2 into CO, an essential feedstock for industrial chemical production. Herein, a core–shell nanostructure anchoring on the surface was developed, which consists of a PtFe bicomponent core (∼2.6 nm) and a nitrogen-doped carbon nanoshell (∼1.3 nm). This structural design enhances the CO2 adsorption saturation, weakens the CO adsorption strength, and promotes hydrogen spillover. This PtFe core–shell material (Pt/Fe = 1:1) demonstrates an elevated reaction rate of 12.58 molCO2 gPt–1 h–1, with nearly 100% CO selectivity at 450 °C and atmosphere pressure. The activity is 5.1-fold higher than that of the Pt nanoparticle, attributed to the tuned geometric and electronic properties. The nitrogen-doped carbon nanoshell preserves the core–shell morphology at a high temperature. Moreover, the in situ experiments reveal the H-assisted dissociation/activation of the CO2 pathway for RWGS. The integration of the bimetallic synergy and core–shell structure is a potent strategy for thermal catalytic processes.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wenxuan Zhou,Xiaoyong Mo,Cham Wah Cheung,Edmund C.M. Tse
At present, over 95 % of H 2 O 2 is produced via the anthraquinone process that requires large infrastructure, generates organic pollution, and poses safety issues. Electrochemical H 2 O 2 generation through oxygen reduction can serve as an alternative, reliable, and decentralized production method if affordable and high-performance electrocatalysts can be developed. Herein, a two-step process is used to prepare an Fe-based complex as a non-precious metal electrocatalyst to facilitate oxygen reduction reaction (ORR) and produce an alkaline H 2 O 2 solution. The Fe complex of benzene-1,3,5-tricarboxylate (FeBTC) is first synthesized using a hydrothermal method and then activated via a pulsed laser treatment process that is optimized via the Taguchi method. The pulse-laser-treated FeBTC (PL-FeBTC) lowers the H 2 O 2 electrosynthesis overpotential by 50 mV at −0.1 mA/cm 2 and exhibits a 25 % increase in H 2 O 2 product selectivity at 0.4 V vs. RHE. The experimental results indicate that the O 2 -to-H 2 O 2 turnover frequency and electrocatalytic yield of the Fe-based metal–organic framework are enhanced simultaneously through solid-to-solid pulsed laser conversion. Through a series of X-ray photoelectron spectroscopy, elemental analysis, Raman spectroscopy, X-ray absorption spectroscopy, and control atmospheric experiments, the origin of the improvement in catalytic performance is rationalized through the formation of an oxo-bridge across the di–Fe active site via an oxygen-doping mechanism, thus providing a systematic laser methodology for precise structure-performance tuning. Beyond H 2 O 2 generation, this study further lays the foundation for the development of cost-effective and scalable electrocatalysts that are central to other commodity manufacturing and sustainable resourcification processes.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Juan Huang,Xiaomin Lang,Mochou Zhang,ZiTao Liu,Yongbin Yang,Jianrong Liu,Hua Lin
The high cost of precious metals limits their use as effective catalysts for water electrolysis, while non-precious metal catalysts are more affordable but often underperform. A promising strategy to improve electrocatalytic performance and reduec costs is to incorporate noble metals onto non-precious substrates. This study successfully synthesized a trace Ru-doped FeNi 2 Ru 0.01 metal aerogel catalyst utilizing a one-step reduction method, resulting in a distinctive core-shell structure. The aerogel exhibits an overpotential of only 228 mV at a current density of 50 mA cm −2 and a stable operation time of up to 70 hours. Analysis reveals that the high specific surface area and porous architecture of the FeNi 2 Ru 0.01 aerogel facilitate the dispersion and exposure of trace Ru. In this configuration, Ru can serve as an active site following oxidation and aid in transforming Ni into the active species NiOOH, significantly boosting OER activity. This research provides a novel approach to optimizing metal aerogel catalysts through precious metal doping and lays a strong foundation for sustainable energy conversion and storage technologies.
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RARE METALS
·
2025
·
IF 11
Ma Jingwen,Li Junbin,Tian Ying,Liu Jinhao,Wang Ruiting
Fe–N–C single-atom catalysts are considered among the most promising non-precious metal-based catalysts for oxygen reduction reaction (ORR), but issues such as low utilization of active sites and the easy aggregation of single atoms severely hinder their application in fuel cells and metal–air batteries. Herein, a single-atom Fe-embedded hierarchical porous hollow carbon fiber catalyst (Fe SAC/HCNF) is reported for ORR. The hollow channels and the porous structure of the fibers facilitate the exposure of single-atom active sites, and offer multidimensional mass transfer pathways to promote the transport of reactants, thus significantly enhancing catalytic performance. Additionally, the abundant micropores exert spatial confinement, which is beneficial for preventing the aggregation of single atoms. Leveraging its unique structural advantages, the Fe SAC/HCNF catalyst demonstrates outstanding ORR activity with low metal loading, boasting a high half-wave potential of 0.905 V, a substantial double-layer capacitance ( C dl ) of 41.1 mF cm −2 , and a notable kinetic current density of 45.2 mA cm −2 in alkaline media. Furthermore, the liquid Zn–air battery (ZAB) using Fe SAC/HCNF catalyst as the air cathode exhibits excellent battery performance and long-term cycling durability nearly 600 h. And the flexible quasi-solid-state ZAB can be stably cycled in various flat/bent states, which is promising for applications in flexible electronic devices. Graphical
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Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 35
·29590-29597
·
IF 9.5
Pengyu Wei,Peng Fu,Liuzhen Bian,Changyang Liu,jianquan Gao,Lei Xing,Chaoyi Wang,Lilin Yang,Yong Li,Shengli An
The development of high-performance perovskite cathodes is critical for advancing carbon-neutral energy technologies through efficient CO2-to-fuel conversion in solid oxide electrolysis cells (SOECs). In this work, we present a groundbreaking dual-functional engineering strategy that simultaneously achieves in situ exsolution of Fe nanoparticles and oxygen vacancy formation in Sr2−xFe1.5Mo0.5O6−δ perovskites. By correlating A-site deficiency with tailored reduction protocols, we demonstrate precise control over Fe nanoparticle density and the oxygen vacancy concentration, synergistically addressing the dual bottlenecks of CO2 activation kinetics and ionic transport limitations. The engineered cathode delivers record-breaking performance: −0.92 A cm−2 (H2O electrolysis@800 °C/1.3 V) and −1.58 A cm−2 (co-electrolysis@800 °C/1.5 V), surpassing that of benchmark perovskites. The dual-modified architecture demonstrates unprecedented durability with 120 h of steam electrolysis and 80 h of co-electrolysis operation at 750 °C/0.5 A cm−2. This work establishes a materials design paradigm that directly bridges atomic-scale defect engineering with macroscale energy conversion efficiency, offering a scalable pathway for transforming industrial CO2 emissions into renewable fuels.
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ENERGY AND BUILDINGS
·
2025
·
IF 7.1
Gonghui Gu,Xinchi Xu,Jinsheng Han,Lin Wan-Wendner,Zhiji Gao,Rongze Fu,Chuanqing Fu,Tao Ma
In this study, a soft magnetic geopolymer (SMG) co-modified with nanomagnetic fluid and spherical micron-sized Fe powders was developed for enhancing the energy conversion in airport pavement induction heating. The effects of Fe particle size on the microstructure, electromagnetic behavior, and mechanical performance of SMG were systematically investigated, with a focus on the size-dependent coupling mechanisms. Results show that Fe powder with a particle size no less than 150 μm provides pore-filling and skeletal reinforcement, leading to improved compressive strength and stable magnetic permeability. In contrast, finer particles significantly increase the specific surface area, which intensifies internal demagnetizing fields and magnetic flux pinning, thereby reducing saturation magnetization and coercivity. Simultaneously, excessive water demand caused by fine particles suppresses geopolymer gel formation, resulting in increased porosity and decreased mechanical strength. COMSOL simulations confirm the development of localized demagnetizing fields around smaller Fe particles. Indoor induction heating tests further reveal that the incorporation of SMG improved the energy conversion efficiency during induction heating by 19.4 % when the Fe powder particle size was not less than 150 μm, demonstrating its potential for energy-responsive, structure-integrated infrastructure.
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