NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 25
·10300-10308
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IF 3.288
Xiuqin Yang,Jing Jin,Zhuming Guo,Zhiyin Xiao,Naiwen Chen,Xiujuan Jiang,Yi He,Xiaoming Liu
In this study, five salts containing the same anion fac-[FeII(CO)3I3]− were prepared through the reaction of cis-[Fe(CO)4I2] with organic amines whose protonated forms, i.e., (EtNH3+), (PrNH3+), (BuNH3+), (PentNH3+), and (Et2NH2+), become the cations of the salts 1, 2, 3, 4, and 5, respectively. These aminium salts, which are soluble in water and polar organic solvents such as DMSO and methanol, were characterized by various techniques including X-ray single-crystal diffraction. These salts underwent solvolysis in both water and DMSO to release CO, following first-order kinetics. In DMSO, the decomposition of these salts proceeded via a significantly simpler mechanism without the involvement of radicals than that in water, and the CO-release rate of these salts was almost linearly related to the hydrophobicity (the logarithm of the oil/water partition coefficient P) of the amines. The CO-release rate was substantially faster in water and in addition to undergoing solvolysis, the anions generated an iodine radical, I˙. Due to the complicated decomposition of these salts in water, the CO-release proceeded in a two-stage manner. The iodine radical was found to be at least partly responsible for the cytotoxicity of these salts in water; this indicates that the proposed anion has potential for applications in cancer therapy.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Limeng Yang,Wendou Chen,Cuihong Sheng,Hailiang Wu,Ningtao Mao,Hui Zhang
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are encouraging methods for wastewater treatments, but the recycling of used PMS activators in powder form from the wastewater treatment system is still problematic. In this paper, we designed a novel and highly effective carbocatalyst for PMS activation, which was achieved by pyrolyzing the hybrids of metal–organic framework MIL-101(Fe) and dicyandiamide immobilized on the surface of carbon cloth (CC), and a facile route for the preparation of fibrous catalysts was developed. The resultant CC loaded with Fe/N-codoped carbocatalyst exhibited desirable reusability and good stability for the degradation of organic dyes. The mechanism of the novel Fe/N-codoped carbocatalyst for PMS activation including the specific roles of N species and Fe-N binding was investigated. It was demonstrated in electrochemical impedance spectroscopy (EIS) results that the CC facilitated the electron transport of the carbocatalyst in AOPs. It was shown in the radical quenching and electron paramagnetic resonance (EPR) experiments that both the radical and non-radical pathways were accountable for the degradation of contaminants, and the non-radical path was principal. It was also evident in the X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) results that pyridinic N and graphitic N were the main active species for PMS activation.
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NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Fang Wu,Yuhong Jiao,Jinlong Ge,Yujun Zhu,chao feng,Zhong Wu,Chang-Peng Lv
Exploring highly active, low-cost electrocatalysts for oxygen evolution reaction (OER) is of great significance but still a major challenge. Here, we synthesized Ni(OH)2@Ni(Fe)OOH with a sea urchin structure on nickel foam via a simple hydrothermal and subsequent soaking process. Experimental results indicate that incorporation of Fe into Ni(OH)2 is favorable for modulate the electronic structure, faster electron transfer and improved intrinsic activity, thereby leading to excellent OER activity. The optimized Ni(OH)2@Ni(Fe)OOH exhibits superior OER activity with overpotentials of 245 and 310 mV at 10 and 100 mA cm-2, respectively, and a small Tafel slope of 40.7 mV dec-1, and along with high stability over 100 h, which is more active than benchmark RuO2 and sever control samples without introduction of Fe. More importantly, the overall water splitting system by using Ni(OH)2@Ni(Fe)OOH-100 as anode and Pt/C as the cathode only requires a cell voltage of 1.54 V to afford 10 mA cm-2. This work not only demonstrate the key factor of Fe doping, but also offers a new path for the development of NiFe-based OER catalysts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Chenyu Song,Jishuang Yang,Chinnadurai Ayappan,Shree Kesavan Kannan,Haitang Yang,Ruimin Xing,Hongxun Yang,Shanhu Liu
The large-scale application of water electrolysis technology is limited by the slow kinetics of the oxygen evolution reaction (OER) that cause vast energy loss. Rational design and construction of hierarchical heterostructures are helpful for developing efficient OER electrocatalysts due to their interesting morphological features and electrochemical properties. Herein, we prepared hierarchical CoS 2 @(Fe,Ni)S 2 heterostructures on carbon fiber paper (CoS 2 @(Fe,Ni)S 2 /CFP) with particle-on-wire morphology using prussian blue analogue as template and precursor. The unique hierarchical heterostructure maximizes accessible active sites and the synergistic effect between different components significantly improves electrocatalytic activity. Impressively, CoS 2 @(Fe,Ni)S 2 /CFP electrocatalyst requires a small overpotential of 237 mV to achieve a current density of 20 mA cm −2 with a low Tafel slope of 54 mV dec −1 and the corresponding voltage has no obvious change after 60 h stability test under a constant current density of 50 mA cm −2 in 1 M KOH solution. This work provides a new idea for the design of efficient and stable non-noble metal-based OER electrocatalysts.
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Small
·
2024
·
IF 13
Jinghan Zhang,Qiming Chen,Pengwei Zhao,An Cai,Xiaobin Fan,Wenchao Peng,Yang Li
NiFe-based materials, especially NiFe layered double hydroxides (LDHs), are recognized as the most promising non-precious metal electrocatalysts for alkaline oxygen evolution reaction (OER). However, the precisely designed distribution of active sites for enhancing activities is still significantly restricted due to the lack of reasonable modulation strategies. Herein, sulfur doped Ni/Fe gradient-distributed LDH (GD-NiFe LDH/S) is fabricated by facile air-induced strategy at room temperature. This strategy accelerates the growth process with abundant CO 2 and O 2 in air, which promotes the inward migration of Fe species, resulting in gradient distribution with Ni/Fe-rich edge/planar. This allows significant enhancement of Ni/Fe synergistic effect, which plays a vital role in OER. Moreover, the sharp pine-like morphology of GD-NiFe LDH/S endows superhydrophilicity/aerophobicity characteristics, facilitating electrolyte penetrating and oxygen releasing. The optimized GD-NiFe LDH/S delivers superior OER performance with low overpotentials of 234 and 270 mV at 10 and 100 mA cm −2 . The assembled anion exchange membrane water electrolyzer only requires 1.90 V at 1.0 A cm −2 and 2.10 V at 1.5 A cm −2 with robust stability for at least 130 h. This work introduces a facile air-induced strategy under room temperature to controllably design active site distributions of LDH for enhanced OER performance.
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PubMed
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Miao Li,Chenxu Guo,Xingzhong Yuan,Zhiyan Feng,Chencheng Qin,Aoqiang Shu,Edison Huixiang Ang,Yan Wu,Hou Wang
A novel Fe-N 2 O 1 S 1 single-atom catalyst (Fe SA -NS-Ti 3 C 2 T x ) was developed for dual activation of ultra-low concentration peroxymonosulfate (PMS) and dissolved oxygen in wastewater treatment. The catalyst was synthesized via a multivariate heteroatom doping strategy using transition metal salt solution and thiourea on Ti 3 C 2 T x . Under 0.1 mM PMS, the Fe SA -NS-Ti 3 C 2 T x achieved 100 % acetaminophen (20 μM) removal within 6 min, with a K c mp of 889.77 min −1 g −2 L 2 and a turnover frequency over two orders of magnitude higher than homogeneous Fe 2+ /Fe 3+ and iron oxides. Mechanistic analysis and theoretical calculations showed that the asymmetric Fe-N 2 O 1 S 1 site optimizes the generation of ·O 2 − and 1 O 2 , efficiently removing ACE through deacetylation and electrophilic attack on the benzene ring. In the long-term tests, the iron leaching of the high-density catalytic bed is negligible, ensuring environmental safety. This study highlights a cost-effective and scalable strategy to advance PMS-based advanced oxidation technologies in wastewater treatment.
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Materials Today Bio
·
2025
·
IF 10.2
Xinying Liu,Baohui Liu,Conglong Chen,Chaowei Hong,Jia Xu,Yixuan Ruan,Ling Huang,Shanni Hong,Wei Chen,Ye Kuang
A significant challenge in modern radiotherapy (RT) is to minimize the detrimental effects on adjacent healthy tissues while concurrently increasing the susceptibility of tumor tissue to radiation. Investigating nanoradiosensitizers with multifunctional properties has a lot of potential as a highly effective strategy for augmenting the efficacy of RT. A novel Janus Ag/Fe-HfO 2 nanoparticle was synthesized in a single-step process. This versatile nanoradiosensitizer combines photothermal capabilities, enzyme-like activities, and the capacity for magnetic resonance imaging (MRI). The surfaces have been meticulously engineered with PEG to boost biocompatibility and adorned with RGD-targeting peptides that selectively target tumor cells (Ag/Fe-HfO 2 -PEG-RGD). The characterization results have demonstrated the successful preparation of Janus Ag/Fe-HfO 2 nanoparticles with a diameter of roughly 10 nm. Furthermore, the photothermal properties, MRI ability, and enzymatic catalytic activities (generate O 2 , produce hydroxyl radical, and consume GSH) of Ag/Fe-HfO 2 -PEG-RGD were verified in vitro experiments. In vivo experiments, by integrating T 1 -weighted MRI-guided RT with the enzymatic activities of these nanoparticles, along with the application of photothermal heating, we have achieved a synergistic enhancement in the therapeutic efficacy of RT. Moreover, it stimulates tumor-specific immune responses, leading to an increased presence of tumor-infiltrating CD8 + T cells. This integrated multimodal nanotherapeutic platform, which capitalizes on the potent enhancement of RT effects, offers a promising new strategy in the ongoing battle against cancer.
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PubMed
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INDUSTRIAL CROPS AND PRODUCTS
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2025
·
IF 6.2
Honghui Yan,Xiangyu Wang,Yi Zhu,Yuding Zhu,Ruiqi Xin,Shunze Zhang,Meiling Chen,Song Li,Jeonghun Kim,Wenkai Zhu
Free formaldehyde poses significant health risks as a prevalent indoor organic pollutant, driving demand for efficient and renewable adsorption solutions. While Fe-CoPBA bimetallic metal-organic frameworks show potential for formaldehyde removal, their powdered crystalline form presents practical limitations including poor recyclability and secondary contamination. Herein, we developed a novel Fe-CoPBA@bamboo composite (Fe-Co@B) through solution blending, leveraging bamboo's inherent micro-nano hierarchical pores for Fe-CoPBA encapsulation. The Fe-CoPBA nanoparticles (NPs) successfully integrated into delignified bamboo conduits through hydroxyl-mediated ligand bonding and van der Waals interactions. Formaldehyde removal tests demonstrated Fe-Co@B's dual adsorption-catalysis mechanism effectively eliminates indoor free formaldehyde. The Fe-Co@B maintained stable removal efficiency for formaldehyde through 10 regeneration cycles while preserving structural integrity. Furthermore, the Fe-Co@B exhibits high reusability along with moisture and deformation resistance. Therefore, this work contributes to solving the current problem of indoor free formaldehyde pollution and provides research ideas for the development of new functional bamboo-based products.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huimin Li,Zhe Sun,Chenlong Dong,Xueli Zhang,Chengkun Lei,Baobao Jin,Qianqian Shen,Husheng Jia,Jinbo Xue
Photocatalytic non-oxidative coupling of methane is an attractive strategy for CH 4 to C 2 conversion, how to facilitate the photogenerated charge separation and accelerate the C–C coupling to promote the reaction kinetics remains a great challenge. Herein, a symbiotic r-Fe 2 O 3 /NiO heterostructure with robust interfaces is constructed in situ. The coherent interface not only provides unique Ni–O–Fe asymmetric sites, but also achieves the separation and transport of photogenerated charge. The unbalanced charge density distribution of two adjacent methyl or methylene at the Ni–O–Fe asymmetric site alleviates the dipole repulsion of the C–C coupling, and promotes C–C coupling to form C 2 hydrocarbons. Under visible light irradiation, the optimal r-Fe 2 O 3 /NiO performs a brilliant C 2 activity up to 71.00 μmol g −1 h −1 , and the C 2 H 4 yield can reach a high value of 40.46 μmol g −1 h −1 and the selectivity of 56.98 %. This work provides new insights into the coupling of C–C to generate C 2 hydrocarbons.
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THERMOCHIMICA ACTA
·
2024
·
IF 3.1
Guangyan Chen,Zai-Yin Hu,Zhijun Guo,Yi Xie
Transition metal nanomaterials are widely applied as flame retardants in materials. Herein, an oxidation-mediated strategy was developed for temporally controlling the in situ growth of Fe(OH) 3 nanoparticles on wool/nylon (W/N) fabrics. The formed particles exhibit homogeneous dispersion on the surface of W/N fabrics, with an average particle diameter of about 60 nm. These Fe(OH) 3 nanoparticles can simultaneously enhance both the flame retardancy (the limiting oxygen index increased by 18.8 % and passed the UL-94 burning test of V-0 rating) and mechanical performance (the tensile strength increased by 9.13 %) of the W/N fabrics. Meanwhile, the obtained W/N fabrics exhibit remarkable smoke-suppressant properties, demonstrating a reduction of 76.4 % and 65.5 % in smoke production rate and total smoke production, respectively, compared to the pure W/N fabrics. Furthermore, the prepared W/N fabrics exhibit good durability. This innovative strategy may be also extended for synthesizing other nanomaterials and pave a new path to develop high-performance flame-retardant materials.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Huihua Wang,Jinhong Wu,Siwei Guo,Haosen Chen,Ruiqi Guo,Ding Huan,Deyong Wang,Wenchang Li,Xianglong Li,Dong Hou
Engineering interface, regulating morphology, and doping heteroatoms are regarded as effective strategies for boosting the electrocatalytic performances of transition-metal phosphides (TMPs), while still encounter some challenges to obtain desirable stability and sustaining catalytic activity. Herein, the Fe-CoP/Ni 2 P@NC/CC-350 self-supported electrode was successfully synthesized via pyrolysis of FeNi/ZIF-67/CC precursors followed by phosphating. In this structure, Fe-doped CoP and Ni 2 P composite nanoparticles are uniformly confined in the porous carbon matrix and anchored firmly on the surface of carbon cloth (CC). Moreover, the flocculent-like Fe-CoP/Ni 2 P@NC/CC-350 demonstrates superhydrophilicity to significantly facilitate mass transfer, while the unique morphology originates from a facile strategy of soaking ZIF-67/CC in the mixed solution composed of FeSO 4 and NiSO 4 . The synthesized Fe-CoP/Ni 2 P@NC/CC-350 integrates the advantages of abundant active sites, confinement effect, interface regulation and superhydrophilicity, thereby demonstrating superior HER and OER activities and stabilities in an alkaline medium (1.0 M KOH). Remarkably, Fe-CoP/Ni 2 P@NC/CC-350 electrodes used both as anode and cathode require a cell voltage of only 1.49 V at 10 mA cm −2 , much lower than that of the well-established 20 % Pt-C/CC and RuO 2 /CC couple (1.612 V). Besides, Fe-CoP/Ni 2 P@NC/CC-350 Fe-CoP/Ni 2 P@NC/CC-350 system exhibits an outstanding stability for monitoring water splitting up to 100 h at 10 mA cm −2 . DFT results further confirm that the heterointerface and Fe doping in Fe-CoP/Ni 2 P@NC/CC-350 lead to a upshift d-band center of active sites and decreased reaction Gibbs energy barrier for the rate-determining step during catalysis, thereby contributing to the superior HER and OER activities. The work provides a novel strategy to construct a superhydrophilic microstructure, and the synergistic effect of electrons originating from the heterointerface and doping paves the way for designing electrocatalysts with high activities toward water splitting.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuhang Ren,Yu Tian,Yating Lu,Dongyu Nie,Huayi Zhu,Xia Yang
Malathion (MA) is a widely used organophosphorus pesticide globally. Developing efficient photocatalysts is crucial for eliminating MA pollution in water by photocatalytic technology. This study focuses on preparing a series of H-PDI supermolecule/NH 2 -MIL-101(Fe) (PM) materials by amidating NH 2 -MIL-101(Fe) with the more stable H-PDI supermolecule, forming a covalent O C–NH bond. Among these materials, 40 %PM (indicating a mass percentage content of 40 % H-PDI supermolecule in PM) exhibited the best performance for degradation of MA. Under simulated sunlight irradiation of a 10 mg·L 1 MA solution for 180 min, the reaction rate constants of 40 %PM were 5.95 times and 3.13 times higher than those of NH 2 -MIL-101(Fe) and H-PDI supermolecule, respectively. The enhanced performance is attributed to the formation of Z-scheme heterojunctions in the 40 %PM composite lead to fast separation of photogenerated e − and h + . Combining the results of HPLC-MS with Fukui Function, the HOMO, LUMO, and pathway of degradation of MA attracted by 1 O 2 , •OH, and h + were speculated. The pathway involves oxidation, demethylation, P-S bond breakage, decarboxylation, and final conversion to some inorganic molecules. The toxicity of the degradation byproducts were lower than that of MA estimated by Toxicity Estimation Software Tool.
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