APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 35
·期 8
·e6280
·
IF 4.105
Jinzhong Guo,Zhuming Guo,Zhiyin Xiao,Jing Jin,Xiuqin Yang,Yi He,Xiaoming Liu
Four new monoiron (II) tricarbonyl complexes with the amine bound, fac -[Fe(CO) 3 I 2 (NH 2 R)] (R = Et, 1 ; n Pr, 2 ; n Bu, 3 ; n Pent, 4 ), were reported using cis -[Fe(CO) 4 I 2 ] as the precursor. All the complexes 1 – 4 were structurally confirmed by various techniques such as ultraviolet–visible (UV–vis), Fourier transform infrared (FTIR), and nuclear magnetic resonance (NMR) spectra and elemental analysis of which complexes 1 and 2 are crystallographically determined. The reaction of the precursor with alkylamines proceeded in two main parallel pathways to form both aminium salts of fac -[Fe(CO) 3 I 3 ] − and the amine-bound complexes ( 1 – 4 ). Their dominances altered with the reaction time. These complexes in DMSO undergo quick decomposition with complex 1 as the relatively most stable one ( t 1/2 = 7.3 min) although they are stable in solid status. Unlike the triiodo anion and pyridinyl analogs showing severe cytotoxicity due to the generation of iodine radical during the decomposition, no iodine radicals were detected from the fac -[Fe(CO) 3 I 2 (NH 2 R)] complexes. Therefore, the cell viability of RT112 cells was not affected by the presence of the amine-bound iron complex ( 1 ) up to 100 μmol L −1 .
研究领域:
无机化学
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生物无机化学
·
医学化学
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DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Shipeng Wu,Rong Shang,Hao Zhang,Qinghu Tang,Qiue Cao,Bang Gu,Wenhao Fang
Low-temperature imine formation through oxidative coupling of alcohols with amines under base-free conditions is very important for fine-chemical synthesis. Supported-Au catalysts show superior performances toward selective oxidation reactions but are scarcely reported for the above application. In this work, the finely-dispersed Au nanoparticles (ca. 2.4 nm) loaded on magnetic Fe x Co 1 O y oxides were developed as novel, efficient and reusable heterogeneous catalyst. Varying the Fe/Co molar ratio allowed tuning the Au−Fe x Co 1 O y interface and further boosting the selective oxidation performance of Au. The optimum Au/Fe 0.25 Co 1 O y catalyst showed >99% yield of benzylideneaniline and 20.1 mol imine mol Au −1 h −1 productivity using the model reaction at 30 °C under air atmosphere without alkaline additives. This was the best result compared to benchmark Au-based catalysts in the literature. In addition, this catalyst exhibited superior performances towards gram-scaled synthesis and diverse substrates. XRD, N 2 -physisorption, TEM, H 2 -TPR, O 2 -TPD, EPR, pyridine-adsorbed FT-IR, and kinetic investigations were used to study this Au catalytic system. It was found that the synergy between Fe 2 O 3 and Co 3 O 4 can induce formation of abundantly mobile and reactive oxygen species (i.e., O 2 − and O − related to oxygen vacancies) and electron-rich metallic Au species on the surface of mesoporous Fe x Co 1 O y oxides. These interfacial features were disclosed to be vital to activating molecular O 2 and O H bond in an alcohol. Besides, it was demonstrated that the surface Lewis acidic sites associated with coordinatively unsaturated Co 3+ ions can help facilitate the tandem oxidation-condensation reactions.
研究领域:
催化化学
·
材料科学
·
有机合成
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DOI
高影响因子
Chemistry-An Asian Journal
·
2024
·
IF 3.5
Lijuan Ma,Han Wang,Jing Zang,Xinna Wang,Hao Li,Yanwei Li,Yanhui Li
The rational design of efficient, stable, low-cost non-precious metal-based electrocatalysts with enhanced oxygen reduction reaction (ORR) activity has attracted widespread attention. In this study, a novel electrocatalyst, Fe/Co-N-MWCNT, was prepared by in-situ growth of ZIF-8 and Fe/Co-Phen on multi-walled carbon nanotubes (MWCNTs), then pyrolysis under different temperature to obtain optimal one. During the pyrolysis process, the incorporation of Fe and Co facilitated the formation of metal active sites and Fe-Co alloy, thereby promoting electron transfer and enhancing the ORR activity. Compared to Pt/C (E1/2 = 0.854V, JL = 4.90 mA cm-2), Fe/Co-N-MWCNT demonstrated a comparable half-wave potential (E1/2 = 0.812V) and an enhanced limiting current density (JL = 5.37 mA cm-2). Furthermore, Fe/Co-N-MWCNT was stable and showed no significant change after 2000 cycles, with only a negative shift of 7 mV in E1/2. Ampere response testing revealed that the current decay of Fe/Co-N-MWCNT after 10000 s was only about 7.8%, while that of Pt/C was about 18.4%. Due to its excellent catalytic stability, Fe/Co-N-MWCNT was demonstrated to be an excellent candidate for rechargeable zinc-air batteries. The outstanding electrocatalytic performance of Fe/Co-N-MWCNT can be attributed to its high pyridinic nitrogen content, the unique structure and abundant metal active sites.
研究领域:
材料科学
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电化学
·
能源存储与转换
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Jie Di,Junxia Guo,Nannan Wang,Guiping Ma
In this work, unique sugar-coated haws stick-like core–shell ZIF-67@PAN-HCCP-MIM-FeCl3 nanofibers were successfully prepared by electrospinning and an in situ nanocrystal growth process. After carbonization of the as-synthesized nanofibers at various temperatures, the resulting sample Fe/Co-N/P-9 (carbonized at 900 °C) retained the presented a sugar-coated haws stick-like structure. The internal carbon nanofiber acts like a “stick” as a support, the “haws” composed of Co2P and Fe5C2 nanoparticles act as catalytic active sites, and the graphite carbon acts as “sugar” to protect particles from detachment. The channel gap between inner core and outer layer can improve the mass transfer process. Owing to these special structure and unique composition features, Fe/Co-N/P-9 exhibited excellent oxygen reduction reaction (ORR) performance with an onset potential of 0.96 V (vs RHE) and a half wave potential of 0.85 V (vs RHE) in 0.1 M KOH solution. Fe/Co-N/P-9 also showed good catalytic stability and methanol tolerance. In addition, the rechargeable Zn–air battery fabricated by Fe/Co-N/P-9 exhibited a galvanostatic discharge voltage of 1.25 V, a higher specific capacity of 565 mAh/gZn, and a better cycle stability than Pt/C+RuO2.
研究领域:
材料科学
·
能源化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Zhe Li,Shudi Mao,Ying Yang,Zhuo Sun,Ran Zhao
Capacitive deionization (CDI) is considered one of the most promising desalination technologies for obtaining fresh water from saline water. In this work, we synthesized a hollow core–shell Co-MOF@Fe/Co-LDH (Co-Fe-LDH) material by developing a strategy to simultaneously grow Co/Fe-LDH on the surface of a Co-MOF precursor in situ. Owing to the increase in the specific surface area of the hollow structure and the Faradaic process of a layered double hydroxide (LDH), the Co-Fe-LDH material exhibits high electrical double layer (EDL) capacitance and pseudocapacitance, which significantly improves the salt adsorption of the material during CDI (34.2 mg/g in a 600 mg/L NaCl solution at 1.2 V). The adsorption for NaCl in this work is approximately 2.5 times the maximum salt adsorption capacity (SAC) of LDH materials applied in nonmembrane CDI (NMCDI). This work may provide a promising model for the application of hollow LDH materials that exhibit pseudocapacitance in CDI.
研究领域:
材料科学
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环境工程
·
海水淡化技术
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Hongyue Li,Jun Yao,Zhiqiang Peng,Mengyun Yang,Taotao Zhao,Peng Wang,Yupei Zhao
As is well known that, transition metal sulfides often face challenges such as excessive intermediate adsorption and poor electrical conductivity, which greatly limits their use in large-scale water electrolysis. Herein, we prepare a Fe-Co bimetallic synergistic catalyst based on solvothermal method. This catalyst ((FeCo) 9 S 8 /C-1) exhibits excellent oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performance due to multiple synergistic effects. For instance, low overpotentials of 284.7 mV for OER and 310 mV for HER at 10 mA·cm −2 could be reached in 1 M KOH, while the electrochemical active surface area reaches 40.25 m 2 ·g −1 , which is twofold compared to bare Co 9 S 8 . Density Functional Theory (DFT) calculations further reveal the strong charge transfer between Fe and Co would reduce the energy barriers for the rate-determining steps, enhancing the desorption of *OOH and *H intermediates, as well as improving the electrocatalytic efficiency. This study opens new avenue for designing other dual-transition metal sulfides for water splitting with high-performance.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
Nature Sustainability
·
2022
·Vol. 6
·期 2
·169-179
·
IF 27.157
Zhang Shengbo,Han Miaomiao,Shi Tongfei,Zhang Haimin,Lin Yue,Zheng Xusheng,Zheng Li Rong,Zhou Hongjian,Chen Chun,Zhang Yunxia,Wang Guozhong,Yin Huajie,Zhao Huijun
The dominant Haber–Bosch process to produce ammonia, arguably the most important chemical in support of global food supply, is both energy and carbon intensive, resulting in substantial environmental impacts. Electrocatalytic nitrogen reduction reaction (NRR) powered by renewable electricity provides a green synthetic route for ammonia, but still suffers from insufficient yield rate and Faradaic efficiency. Single-atom electrocatalysts (SACs) have the potential to transform this catalytic process; however, controllable synthesis of SACs with high loading of active sites remains a big challenge. Here we utilize bacterial cellulose with rich oxygen functional groups to anchor iron (Fe) and cobalt (Co), realizing high density, atomically dispersed, bimetallic Fe–Co active sites. For electrocatalytic NRR, our catalyst design delivers a remarkable ammonia yield rate of 579.2 ± 27.8 μg h −1 mg cat. −1 and an exceptional Faradaic efficiency of 79.0 ± 3.8%. The combined theoretical and experimental investigations reveal that the operando change in coordination configuration from [(O-C 2 ) 3 Fe–Co(O-C 2 ) 3 ] to [(O-C 2 ) 3 Fe–Co(O-C)C 2 ] is the enabling chemistry. Our findings suggest a general approach to engineer SACs that can drive critical reactions of relevance for sustainability.
研究领域:
材料科学
·
催化化学
·
环境科学
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产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Mei Luo,Xiangmin Fu,Shuo Geng,Ziwei Li,Min Li
CO 2 electrocatalysis reduction (CO 2 RR) is considered to be one of the most efficient methods to achieve carbon neutralization and realize renewable energy conversion. Unfortunately, at present, CO 2 electrocatalysts confront the challenges of high overpotential, low selectivity, and poor stability. Ag based electrocatalysts are considered to be the most promising catalysts for CO production via CO 2 RR on a large scale, due to their relatively higher catalytic performance and more abundant reserves compared with other noble metals. Whereas, they still suffer from high cost. In this paper, we design bimetallic CuAg/CeO 2 -6 catalysts by the simple impregnation method for CO 2 RR, exhibiting the highest FE CO of 84% at –1.1 V vs. RHE compared with other bimetallic catalysts with different Cu/Ag ratio and monometal catalysts. XPS results demonstrate the electron delocalization effect not only between Cu and Ag bimetals but also among CeO 2 support. This effect results in the electronic structure change and the formation of the highest concentration of oxygen vacancies, promoting the CO 2 adsorption and activation as well as facilitating the formation of COOH* intermediates as evidenced by the in situ ATR-SEIRAS measurements. Additionally, the highest active surface for CO 2 RR and the smallest charge resistance of CuAg/CeO 2 -6 also contributes to its good CO 2 RR performance. This work sheds light on the design of other efficient CO 2 RR catalysts through electronic structure tuning by bimetallic strategy.
研究领域:
电化学
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催化
·
材料科学
·
可再生能源
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产品关联
DOI
高影响因子
MOLECULES
·
2025
·Vol. 31
·期 1
·
IF 4.6
Mingyu Liu,Bowen Pei,Hongyu Ba,Wei Ni,Huaheng Zhao,Shuang Chen,Jiamin Zhao,Jinsheng Zhao
The oxygen evolution reaction (OER) in water splitting involves complex multi-electron–proton transfer processes and represents the rate-determining step limiting overall electrolysis efficiency. Developing non-noble-metal catalysts with high activity and stability is therefore essential. Herein, a heterogeneous synthesis strategy was employed to in situ construct an iron-rich layered sulfate precursor (Fe0.42Co0.58-SO4/NF) on nickel foam, which underwent deep self-reconstruction in alkaline electrolyte to form nanoflower-like Fe0.42Co0.58OOH/NF. The optimized catalyst maintained its iron-rich composition and hierarchical structure, delivering outstanding OER performance with an overpotential of 220 mV at 10 mA·cm−2, a Tafel slope of 31.9 mV·dec−1, and stability exceeding 12 h at 600 mA·cm−2. Synchrotron analyses revealed dynamic transitions between mono-μ-O and di-μ-O Fe–M (M = Fe, Co) oxygen bridges during reconstruction, which enhanced both structural robustness and active-site density. The Fe-rich environment promoted the formation of Fe3+–O–Fe3+units that synergized with Co4+species to activate the lattice oxygen mechanism (LOM), thereby accelerating OER kinetics. This work elucidates the key role of oxygen-bridge geometry in optimizing catalytic activity and durability, providing valuable insights into the rational design of Fe–Co-based non-noble-metal catalysts with high iron content for efficient water oxidation.
研究领域:
电催化
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材料科学
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能量转换
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水分解
·
无机化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Chao Wang,Qing Zhang,Cong Liu,Haishun Jiang,Wan Zhou,Muhammad Nadeem,Qiaoliang Bao,Yoshio Bando,Ding Yuan,Yuhai Dou
The slow kinetics of the anodic oxygen evolution reaction (OER) impose a major limitation on overall water electrolysis, creating a demand for highly active catalysts. Transition metal selenides (TMSs) offer favorable electrical conductivity, inexpensive constituents, and adjustable electronic configurations; however, their inherent catalytic activity is still insufficient. In this study, nanorod-like Fe/Co co-doped NiSe (Fe,Co-NiSe) was prepared by hydrothermally forming NiSe and subsequently introducing Fe and Co through a simple soaking treatment. The simultaneous incorporation of Fe and Co effectively tunes the electronic structure of NiSe. Raman measurements performed in situ show that introducing Fe/Co favors the generation of NiOOH-type oxyhydroxide species, thereby enhancing OER activity. 18O-labeling differential electrochemical mass spectrometry confirms that Fe,Co-NiSe follows the conventional adsorbate evolution mechanism. Density functional theory (DFT) analysis further indicates that Fe-induced electronic redistribution at Co sites raises the Co d-band position and reduces the Gibbs energy required for the kinetically limiting *O → *OOH conversion. Consequently, under alkaline conditions, Fe,Co-NiSe reaches 10 mA cm-2 at an overpotential of 229 mV and sustains 50 mA cm-2 for 300 h. When employed as the anodic electrode in an anion exchange membrane (AEM) water electrolyzer coupled with Pt/C, this electrolyzer delivers 1 A cm-2 while registering a cell voltage of 1.84 V.
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Ming Yan,Jiangtao Huang,Mengliu Yang,Hao Zhang,Yu Zhu,Nengyu Zhou,Juan Wang
MAX phases are layered ternary carbides and nitrides with unique properties, doping transition metals in it is attracting significant attentions for the processing of this relatively new class of materials. In this paper, a magnetic solid solution MAX phase V 2 (Sn 1− x A x )C ( A = Mn, Fe, Co) was synthesized by doping Mn/Fe/Co atoms into V 2 SnC by pressure-less sintering. The XRD results show that when x = 0.4, the characteristic peak shifts to the right, and the substitution reaches saturation. SEM and TEM show that doping does not change the original layered morphology and hexagonal crystal form, but only the lattice constants decrease slightly. Magnetic test results indicate that V 2 (Sn 1− x A x )C is a typical low-temperature magnetic material with a Curie temperature around 60 K, and the magnetization increases with the increase of doping amount. Moreover, we explained the reasons of V 2 SnC doping A-site instead of M-site and the changing trend of the magnetic moments by first-principles calculations, which are consistent with the experimental results.
研究领域:
材料科学
·
物理学
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产品关联
DOI
高影响因子
International Journal of Environmental Research and Public Health
·
2023
·Vol. 20
·期 6
·4902
·
IF 4.614
Ruiqi Wu,Ning Liu,Chengna Dai,Ruinian Xu,Ning Wang,Gangqiang Yu,Biaohua Chen
N2O is a greenhouse gas and a candidate oxidant. Volatile organic pollutants (VOCs) have caused great harm to the atmospheric ecological environment. Developing the technique utilizing N2O as the oxidant to oxidize VOCs to realize the collaborative purification has significant importance and practical value for N2O emission control and VOC abatement. Therefore, the study of N2O catalytic oxidation of tert-butanol based on zeolite catalysts was carried out. A series of molecular sieves, including FER, MOR, ZSM-5, Y, and BEA, were selected as the catalyst objects, and the 1.5% wt Fe and Co were, respectively, loaded on the zeolite catalysts via the impregnation method. It was found that the catalytic performance of BEA was the best among the molecular sieves. Comparing the catalytic performance of Fe-BEA under different load gradients (0.25~2%), it was found that 1.5% Fe-BEA possessed the best catalytic activity. A series of characterization methods showed that Fe3+content in 1.5% Fe-BEA was the highest, and more active sites formed to promote the catalytic reaction. The α-O in the reaction eventually oxidized tert-butanol to CO2over the active site. The Co mainly existed in the form of Co2+cations over Co-BEA samples; the 2% Co-BEA possessing higher amounts of Co2+exhibited the highest activity among the prepared Co-BEA samples.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子