FOOD CHEMISTRY
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2024
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IF 8.5
Xinran Wang,Xufeng Zang,Hong Zhou,Na Wang,Yishan Fang,Bo Cui
Trichlorfon (TCF) has the possibility of contaminating agricultural crops and posing some health risks to humans. Herein, an electrochemiluminescence (ECL) sensor based on Fe, Cu dual-atom catalysts (Fe/Cu-N-C DACs) and Au@Luminol was developed for the ultrasensitive detection of TCF. Fe/Cu-N-C with diatomic sites has a very high catalytic activity and can be used as a co-reaction accelerator to activate H 2 O 2 to generate a large number of hydroxyl radicals which triggered a strong cathodic ECL signal of luminol. TCF molecularly imprinted polymer (MIP) was further introduced as a specific recognition element, and the interaction between the template molecule and the functional monomer was verified by molecular docking technique. The developed sensing platform was successfully applied to the ultrasensitive detection of TCF with a linear range from 1.0 pg/mL to 5.0 μg/mL with a low detection limit (0.39 pg/mL). This study broadens the application of DACs in ECL sensing.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yuzhen Zhang,Huajun Zhou,Peihua Zhao,Kai Yuan,Rui Zhou,Yongping Qu,Yanzhong Wang
The oxygen evolution reaction (OER) is a complex four-electron transfer process that poses a significant challenge to the efficient production of hydrogen through water splitting. However, developing non-noble metal electrocatalyst with excellent OER performance is still a big challenge. Herein, we propose a new strategy for the in-situ growth of two-dimensional amorphous/crystalline thiophene-based Ni-Fe metal–organic frameworks (MOFs) using Ni-Fe foam (NFF) as metal source and current collector, and thiophene-2,5-dicarboxylic acid (TDC) as corrosion agent and ligand. TDC was ionized at high temperature to produce H + ions that etch NFF to release Ni 2+ and Fe 2+ ions, which were coordinated with TDC to in situ synthesize two-dimensional Ni-Fe thiophenedicarboxylate coordination polymer (NiFe-TDC) nanobelts on NFF. The unique structure and synergistic effect of Ni and Fe ions of NiFe-TDC 0.05 result in the excellent OER performance with an overpotential of 224 and 256 mV at current densities of 10 and 100 mA cm −2 , respectively, and it can run stably for 100 h at a current density of 100 mA cm −2 , indicating the outstanding stability. Furthermore, NiFe-TDC 0.05 remains the excellent OER performance with an extremely low potential of 196 and 271 mV at current densities of 10 and 100 mA cm −2 in seawater with 1 mol L -1 (M) KOH, respectively. The assembled NiFe-TDC 0.05 || Pt/C water electrolysis cell achieves a current density of 100 mA cm −2 at a low voltage of 1.78 V. The work provides a new method to prepare two dimensional MOFs for efficient water oxidation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Qiang Zhong,Yan Xue,Zihao Qi,Yue Sun,Leliang Wu,Dunyu Sun,Chenmin Xu,Kwangchol Ri,Shaogui Yang,Jiandong Zhu,Qiuyi Ji,Yazi Liu,Shiyin Li,Huan He
Two-dimensional cage-in-cage carbon-coated FeSeS superlattices with varying degrees of sulfidation (FeSeS@C) are developed for activating peroxymonosulfate (PMS) to effectively degrade diatrizoic acid (DTZ), and the intrinsic origin that govern the activity of FeSeS@C are deeply elucidated. Experimental and theoretical analyses manifested that proper sulfidation led to increased surface acidity of FeSeS@C. The high surface acidity can optimize the exposure and spin state of Fe sites for FeSeS@C-4, a high spin state of Fe (6.27 μ B ) not only regulating PMS adsorption for enhancing the charge density, but also expediting interfacial charge deliver to trigger the efficient PMS activation. Therefore, among FeSeS@C, FeSeS@C-4 exhibited the best degradation performance for DTZ, with first-order kinetic rate constants (k obs ) of 0.232 min −1 and degradation rate of 100 %. This study demonstrates a novel application of cage-in-cage superlattices in environmental remediation and offers new insights into the mechanism of PMS activation by sulfur modification Fe-based catalysts.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Bolong Liang,Xiaoyu Huang,Xi Zhu,Hongbin He,Shu-xuan Liang
Ciprofloxacin accumulates in aqueous environment due to its non-degradability. Photocatalysis, as an economical and efficient treatment technology for organic matter, is mostly used to remove antibiotics from water environment. However, the photocatalytic performance is limited by photocatalysts, which suffer from wide band gap and severe recombination of photogenerated electrons and holes. Therefore, we developed a Z-scheme heterojunction photocatalyst Fe-ZIF-8@AgCl, which was synthesized by combining pre-prepared Fe-ZIF-8 with AgCl. Meanwhile, the X-ray diffractometer, scanning electron microscopy, transmission electron microscopy, Brunauer-Emmett-Teller analysis and X-ray photoelectron spectroscopy were employed to characterize the structure of Fe-ZIF-8@AgCl, and a series of photoelectric tests were conducted to demonstrate the photocatalytic properties of Fe-ZIF-8@AgCl. The results revealed that Fe-ZIF-8@AgCl had a remarkable 71.9 % removal efficiency of ciprofloxacin by photodegradation in 120 min. Fe-ZIF-8@AgCl could help reduce band gap energy, inhibit the recombination of photoelectrons and holes, lower the charge transfer resistance, and enhance the photocurrent response. Furthermore, Fe-ZIF-8@AgCl still maintained a high photocatalytic performance after 4 cycles, and ·O 2 - was detected and identified as the main photocatalytic active factor. Subsequently, the charge transfer mechanism of direct Z-scheme heterojunction was proposed, and the photocatalytic degradation pathways of ciprofloxacin were analyzed. In this study, Z-scheme heterojunction photocatalyst was prepared and showed great potential for efficient photodegradation of ciprofloxacin.
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Regenerative Biomaterials
·
2024
·
IF 5.6
Yang Shuaikang,Wang Weiqiang,Xu Yanan,Yuan Yonghui,Hao Shengzhi
Fe-based biodegradable materials have attracted significant attention due to their exceptional mechanical properties and favorable biocompatibility. Currently, research on Fe-based materials mainly focuses on regulating the degradation rate. However, excessive release of Fe ions during material degradation will induce the generation of reactive oxygen species (ROS), leading to oxidative stress and ferroptosis. Therefore, the control of ROS release and the improvement of biocompatibility for Fe-based materials are very important. In this study, new Fe–Zn alloys were prepared by electrodeposition with the intention of using Zn as an antioxidant to reduce oxidative damage during alloy degradation. Initially, the impact of three potential degradation ions (Fe2+, Fe3+, Zn2+) from the Fe–Zn alloy on human endothelial cell (EC) activity and migration ability was investigated. Subsequently, cell adhesion, cell activity, ROS production and DNA damage were assessed at various locations surrounding the alloy. Finally, the influence of different concentrations of Zn2+ in the medium on cell viability and ROS production was evaluated. High levels of ROS exhibited evident toxic effects on ECs and promoted DNA damage. As an antioxidant, Zn2+ effectively reduced ROS production around Fe and improved the cell viability on its surface at a concentration of 0.04 mmol/l. These findings demonstrate that Fe–Zn alloy can attenuate the ROS generated from Fe degradation thereby enhancing cytocompatibility.
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ChemCatChem
·
2024
·
IF 3.8
Chengzhuo Yu,Jin Xu,Yarui Wang,Silong Wang,Li Xiong,Fanglan Geng,Zesen Shang,Huasheng Wu,Jitao Lv,Lixia Zhao,Yawei Wang
Graphical Untill now, reactive oxygen species (ROS) are difficult to generate in the natural light conditions, since most photocatalysts require external strong stimuli. We surprisingly found the ROS generation on MIL-100(Fe)/TiO 2 driven by mild natural light. The ROS generation patterns and mechanism of MIL-100(Fe)/TiO 2 was revealed by chemiluminescence (CL) and density functional theory (DFT). Reactive oxygen species (ROS), as one kind of the most highly oxidizing oxidants, are difficult to generate and utilize in the natural light conditions, since many materials require external strong stimuli for ROS release to be effective as pollutant degradation or biocide. In this work, we surprisingly found the ROS generation on MIL-100(Fe)/TiO 2 driven by mild natural light. Then ROS generation patterns and mechanism was revealed by chemiluminescence (CL) and density functional theory (DFT). Meanwhile, rhodamine B (RhB) can also be removed by MIL-100(Fe)/TiO 2 under natural light, which further evidence the ROS generation under the natural light. This work provides a new direction for spontaneously generating ROS releasing without external strong stimuli and has the broad potential applications in the field of pollutant degradation or antimicrobials under natural conditions.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Ping Zhang,Dan Zou,Chunhua Dong,Feiping Zhao,Weichun Yang,Mengying Si,Zhihui Yang
Heavy metal polluted soil remediation is a global concern. Therefore, it is urgently needed to develop new ways for soil remediation . Although the electrochemical method is a simple, efficient, and promising process, the reaction mechanism of arsenic (As) in contaminated soil treated by the electrochemical method is rarely noticed. Herein, electrochemical techniques were developed for As removal from contaminated soil, which can be effectively achieved by using a Fe sacrificial anode to form Fe 3+ species and by combining manganese oxide in soils for remediation. The results showed that the As was changed from an unstable to a stable state, and As pollutions were effectively removed by this electrochemical method. Further, the dissolution kinetics of Fe and Mn oxides , arsenic reaction kinetics and the phase transformation process during the remediation process were investigated by cyclic voltammetry (CV) methods. From the simulation experiments, it was found that As(III) should be oxidized by Mn 4+ and Fe 3+ to form As(V), and As(V) was the main reactant with Fe and Mn oxides for As removal. Consequently, the current work may provide a new insight into solve As contamination in soil, and provide some new insights into the interaction mechanism between multiple components.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Hao Wang,Renting Huang,Wei Mao,Hao Xu,Chutong Ling,Junru Zhao,Fan Yi,Yongxin Zhou,Jinghong Zhou
Iron-based metal-organic frameworks (MOFs) represent a potentially important tool for controlling organic pollutants . However, the structural stability of most iron-based MOFs in the aqueous environment is limited. Therefore, this study sought to improve the aqueous stability and photocatalytic activity of MIL-101(Fe) using an in-situ modification strategy. A novel and highly water-stable MIL-101(Fe)@IPA 4 was prepared using ligand regulation. Owing to the in-situ modification effect, MIL-101(Fe)@IPA 4 exhibited remarkable hydrophobicity with a water contact angle at 102.4° while maintaining minimal leaching of iron ions (0.46 mg/L), even after five cycles of photocatalysis . Under MIL-101(Fe)@IPA 4 /UV/H 2 O 2 conditions, the removal rates of ciprofloxacin and total organic carbon reached 100% and 49.16%, respectively, within 60 min. These researches suggest that introducing IPA improves the light absorption properties of MIL-101(Fe)@IPA 4 and facilitates electron-hole separation, thereby promoting the generation of active species. The ecotoxicity assessment of major degradation intermediates of ciprofloxacin was conducted using the ECOSAR system. Our findings provide novel insights for enhancing the water stability of iron-based MOFs through an in-situ modification strategy, which is crucial for pollution control efforts.
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MOLECULES
·
2025
·Vol. 30
·期 1
·177
·
IF 4.6
Zhi Lu,Yifan Guo,Shilin Li,Jiaqi Ding,Yingzi Ren,Kun Tang,Jiefeng Wang,Chengxin Li,Zishuo Shi,Ziqi Sun,Hongbo Meng,Guangxin Wang
Water electrolysis is a promising path to the industrialization development of hydrogen energy. The exploitation of high-efficiency and inexpensive catalysts become important to the mass use of water decomposition. Ni-based nanomaterials have exhibited great potential for the catalysis of water splitting, which have attracted the attention of researchers around the world. Here, we prepared a novel Mo-doped NiFe-based layered double hydroxide (LDH) with a nanoarray microstructure on Ni foam. The doping amount of Mo can significantly change the microstructure of the electrocatalysis, which will further affect the oxygen evolution reaction (OER) performance of water splitting. This novel nanomaterial required only an overpotential of 227 mV for 10 mA cm−2and a Tafel slope of 54.8 mV/dec in 1 M KOH. Meanwhile, there was no Mo, and the NiFe-LDH needed 233 mV to attain to 10 mA cm−2. Compared to the NiFe-LDH without Mo, the NiFeMo-LDH nanosheet arrays exhibited enhanced activities with 17.1 mV/dec less Tafel in OER. The good performance of the electrocatalyst is ascribed to the special nanosheet arrays and the heterostructure of the Ni-Fe-Mo system. These features help to increase the active surface, enhancing the efficient charge transfer and the reactive activity in OER.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Chongyang Wei,Xiaoxue Han,Shouying Huang,Haoting Liang,Yidan Wang,Ting Li,Yong Wang,Yue Wang,Xinbin Ma
In the Fischer–Tropsch synthesis (FTS) reaction, the intricate reaction conditions are prone to induce phase transitions in iron carbides, which markedly affect catalytic performance. Manipulating and stabilizing the active phase is paramount for ensuring the catalyst efficiency. In this study, we regulated the Fe-Zn interaction to investigate the influence of iron carbides and the characteristics of surface carbon species. The strong interaction significantly enhanced the adsorption and dissociation of CO on the catalyst surface, thereby facilitating the formation of carbon-rich Fe 2(.2) C. Consequently, the FeZn-s catalyst exhibited the highest iron time yield (FTY) of 959 μmol CO ·g Fe - 1 ·s - 1 . But meanwhile, the stronger Fe-Zn interaction also accelerated the carbon deposition rate and elevated the graphitization degree of the surface carbon, expediting the catalyst deactivation. These results provide an insight into the modulation and stabilization of iron carbides by adjusting the interaction between the Fe and supports, which inspires the further development of Fe-based catalysts for FTS applications.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2025
·
IF 4.9
Yu Qinyuan,Li Jiahui,Wang Yufen,Wei Xuedong
Transition metal sulfides (TMS) have drawn increasing research interest owing to their unique electronic structure. They hold broad prospects in accelerating the sluggish oxygen evolution reaction (OER) during water electrolysis. Metal-organic frameworks (MOFs) feature controllable electronic structures and specific surface areas, which facilitate the adsorption of reactants and expedite interfacial electron transfer. Leveraging the above-mentioned advantages of the two materials, a kind of composite electrocatalyst, CuCo 2 S 4 @MIL-53(Fe)/NF, was synthesized by growing MIL-53(Fe) in-situ onto CuCo 2 S 4 nanowires supported on nickel foam. This composite electrocatalyst can accelerate charge transfer, significantly increase the number of active sites, and enhance both electrocatalytic activity and stability. The electrocatalyst CuCo 2 S 4 @MIL-53(Fe)/NF can drive the OER with an overpotential of 390 mV at a current density of 100 mA·cm −2 . Moreover, it still demonstrates excellent catalytic activity after 75 h of testing. This study not only broadens the avenues for sulfide composites but also provides an experimental basis and support for the direct combination of metal chalcogenides and Fe-based MOFs as electrocatalysts.
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LANGMUIR
·
2024
·
IF 3.7
Zhuangzhi Sun,Jiawei Lin,Suwei Lu,Yuhang Li,Tingting Qi,Xiaobo Peng,Shijing Liang,Lilong Jiang
The electrochemical nitrogen reduction reaction (eNRR) has emerged as a promising strategy for green ammonia synthesis. However, it suffers unsatisfactory reaction performance owing to the low aqueous solubility of N2 in aqueous solution, the high dissociation energy of N≡N, and the unavoidable competing hydrogen evolution reaction (HER). Herein, a MIL-53(Fe)@TiO2 catalyst is designed and synthesized for highly efficient eNRR. Relative to simple MIL-53(Fe), MIL-53(Fe)@TiO2 achieves a 2-fold enhancement in the Faradaic efficiency (FE) with an improved ammonia yield rate by 76.5% at −0.1 V versus reversible hydrogen electrode (RHE). After four cycles of electrocatalysis, MIL-53(Fe)@TiO2 can maintain a good catalytic activity, while MIL-53(Fe) exhibits a significant decrease in the NH3 yield rate and FE by 79.8 and 82.3%, respectively. Benefiting from the synergetic effect between TiO2 and MIL-53(Fe) in the composites, Fe3+ ions can be greatly stabilized in MIL-53(Fe) during the eNRR process, which greatly hinders the catalyst deactivation caused by the electrochemical reduction of Fe3+ ions. Further, the charge transfer ability in the interface of composites can be improved, and thus, the eNRR activity is significantly boosted. These findings provide a promising insight into the preparation of efficient composite electrocatalysts.
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