DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 46
·17787-17794
·
IF 4.569
Pengjun Li,Zili Li,Xirui Miao,Haoting Hou,Mao Wang,Xudong Yang
It has become a significant problem to develop and improve carbonized polymer dot (CPD)-based fluorescence sensors with environmental detection features. In this study, fluorescent “turn on” sensors of CPDs were prepared by a one-step hydrothermal method using o-phenylenediamine (o-PD) and ferric chloride (FeCl3) as raw materials. Fe-doped CPDs exhibited excellent fluorescence properties, stability, and the sensitive and selective “turn on” detection of hydrazine hydrate (N2H4·H2O). In this detection system, Fe3+ acts as an effective fluorescence inhibitor that inhibits the yellow fluorescence emission from CPDs, while Fe3+ is reduced upon the addition of the N2H4·H2O reducing agent. The fluorescence intensity of CPDs gradually increased with the increasing concentration of N2H4·H2O, while the limit of detection (LOD) could reach 0.168 μM. In addition, CPD-based polyvinyl alcohol (CPDs@PVA) films were also prepared, which still maintained excellent sensitivity to N2H4·H2O. The results show that CPDs and their composite films can detect N2H4·H2O with good detection performance.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·125180
·
IF 7.5
Lin Xu,Lifen Liu,Yan Li
An aeration-driven piezocatalytic fuel cell (PzFC) was tested for sulfide removal. • Single-atom Fe-doped MoS 2 piezoanode enhanced the oxidation of sulfide. • The PzFC achieved sulfide removal of 2.53 kg/(m 3 ·d) with 83% selectivity of S 0 /S n 2- . Sulfide (S 2- , HS - , and H 2 S) can be directly oxidized by air, but the reaction kinetics are sluggish, and the resulting sulfate product is stable but of low value. To accelerate sulfide oxidation to recoverable value-added products, we constructed an aeration-driven piezocatalytic fuel cell (PzFC) with single-atom Fe 1 @MoS 2 catalysts, in which mechanical strain was induced by continuous air bubbling. Herein, the sulfide was oxidized and selectively converted to low-toxicity products: about 83% elemental sulfur/polysulfides (S 0 /S n 2- ), with minor soluble sulfate (SO 4 2- ) and thiosulfate (S 2 O 3 2- ). S 0 /S n 2- can be used to enhance biological denitrification in wastewater treatment. Notably, the PzFC achieved 93% sulfide removal (initial concentration: 170 mg/L) within 90 min and exhibited stability over six consecutive cycles. Key operational parameters (temperature, pH, initial sulfide concentration, and aeration rate) were systematically evaluated, achieving a maximum desulfurization capacity of 20.68 g/(m 2 ·h) (i.e., 4.96 kg/(m 3 ·d) at an initial concentration of 470 mg/L). Furthermore, the influences of self-bias and single-atom Fe loading on PzFC performance were systematically clarified, and the underlying catalytic mechanism was proposed. This work establishes a low-carbon, efficient strategy for wastewater desulfurization by integrating single-atom piezocatalysts Fe 1 @MoS 2 and PzFC. Download: Download high-res image (240KB) Download: Download full-size image
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Mingyue Zhou,Ziwei Yang,Tianpeng Yin,Yunfeng Zhao,Cai-yun Wang,Guo-yuan Zhu,Li-ping Bai,Zhi-hong Jiang,Wei Zhang
Nonapoptotic ferroptosis is a promising cancer treatment which offers a solution to the multidrug resistance of conventional apoptosis-induced programmed cancer cell death therapies. Reducing intracellular glutathione (GSH) is essential for inducing excess ROS and has been considered a crucial process to trigger ferroptosis. However, treatments reducing GSH alone have not produced satisfactory effects due to their restricted target. In this regard, FeCDs (Fe3+-modified l-histidine -sourced carbon dots) with dual GSH-consumption capabilities were constructed to engineer ferroptosis by self-amplifying intratumoral oxidative stress. Carbon dots have the ability to consume GSH, and the introduction of Fe3+ can amplify the GSH-consuming ability of CDs, reacting with excess H2O2 in the tumor microenvironment to generate highly oxidized •OH. This is a novel strategy through synergistic self-amplification therapy combining Fe3+ and CDs with GSH-consuming activity. The acid-triggered degradation material (FeCDs@PAE–PEG) was prepared by encapsulating FeCDs in an oil-in-water manner. Compared with other ferroptosis-triggering nanoparticles, the established FeCDs@PAE–PEG is targeted and significantly enhances the consumption efficiency of GSH and accumulation of excess iron without the involvement of infrared light and ultrasound. This synergistic strategy exhibits excellent ferroptosis-inducing ability and antitumor efficacy both in vitro and in vivo and offers great potential for clinical translation of ferroptosis.
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ENERGY & FUELS
·
2023
·
IF 5.3
Huihua Wang,Wenchang Li,Jinhong Wu,Deyong Wang,Dong Hou,Minqi Sheng,Ruiqi Guo
Water splitting through electrolysis has been recognized as a promising solution for the production of hydrogen and oxygen to advance many renewable energy conversion and storage systems, while the key is the innovative exploration of cost-efficient electrocatalysts. Herein, interface-modified Ni–Fe–P/Co–P/NF alloys were achieved through a facile electroless plating strategy, in which the constructed interfaces benefited not only from the strong electron interaction but also from the fast mass transfer, significantly boosting the oxygen evolution reaction and hydrogen evolution reaction catalytic performance. More interestingly, water-splitting cells assembled using Ni–Fe–P/Co–P/NF-5L alloys as the cathode and anode, respectively, only requires a cell voltage of ∼1.52 V at 10 mA cm–2, far lower than that of the integrated Pt–C/NF and RuO2/NF couple (1.61 V). Also, the Ni–Fe–P/Co–P/NF-5L||Ni–Fe–P/Co–P/NF-5L system shows an outstanding durability over a long-term operation of 48 h at 10 mA cm–2. The work demonstrates an innovative strategy to construct heterogeneous interfaces for high-performance electrocatalysts and is suggested to be readily extended to regulate heterogeneous interfaces among other binary and ternary electrocatalysts, such as transition metal phosphides/borides, for scaling up water-splitting technology.
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Water
·
2023
·Vol. 15
·期 21
·3801
·
IF 3.4
Yaoji Chen,Ruifu Chen,Xinglan Chang,Jingying Yan,Yajie Gu,Shuang Xi,Pengfei Sun,Xiaoping Dong
In order to realize the high value-added reuse of coal fly ash, a reusable Fe-modified fly ash catalyst was synthesized for ozone catalysis degradation of chemical oxygen demand (COD) in wastewater. Through enhancement of the pretreatment procedure and FeOxmodification, the resulting fly ash with Fe modification demonstrated increased specific surface area and porosity. The presence of Fe loading significantly enhances the reactivity of surface oxidizing reactive species, particularly oxygen vacancy, leading to improved adsorption and activation properties towards ozone molecules. Sodium acetate is chosen as a probe for contaminants due to its status as a small organic substance that remains resistant to further direct oxidation by ozone. This makes it suitable for evaluating the catalyst’s effectiveness in degrading chemical oxygen demand (COD). The quantitative detection of free radicals revealed the generation of •O2−was nearly 10 times that of •OH and dominated the reaction. This study showcases the potential of fly ash, an industrial byproduct, to be utilized as a cost-effective and easily prepared catalyst with consistent physical and chemical characteristics.Keywords:coal fly ash catalyst;iron oxide;ozone catalysis;radical oxidation;COD degradation
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Feilong Dong,Chuyun Fu,Zhu Meng,Qiufeng Lin,Jinzhe Li,Tao Zeng,Da Wang,Juntao Tang,Shuang Song
Ferrate (Fe(VI)) has been extensively studied as a green oxidant to treat wastewater. But Fe(VI) oxidation still faces several challenges for application, such as the sensitivity of Fe(VI) to pH and the restrictions on the Fe(VI) utilization efficiency for pollutant elimination at low concentration levels. This study proposed a two-stage Fe(VI) oxidation process to enhance the bisphenol A (BPA) removal for potential applicability, consisting of the adsorption by CNTs of stage I and the degradation by Fe(VI) of stage II. The Fe(VI) utilization efficiency in the two-stage process (0.848) was higher than that in one-stage processes (0.727) and Fe(VI) alone system (0.504) at pH 9. In stage I, the adsorption process had good compliance with the Langmuir isotherm model and pseudo-second-order kinetic model. In stage II, the effective utilization of low-concentration Fe(VI) was 2.45 times more than Fe(VI) alone, and the reduction of reaction volume was beneficial to further enhance utilization. The probe experiments (sulfoxide) and the degradation experiments of other electron-donating/withdrawing pollutants (e.g., atrazine, benzoic acid) demonstrated that Fe(IV) and Fe(V) were major oxidizing species in the two-stage process. The regeneration experiments showed that CNTs still had acceptable adsorption and catalytic capabilities after five cycles. Finally, the intermediate products in the two-stage process were detected and four possible degradation pathways of BPA were proposed. These findings were meaningful for the practical application of Fe(VI) oxidation to overcome the conditional limitation and improve the utilization.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 23
·9826-9836
·
IF 9.8
Shuai Liu,Meiting Yang,Ruijia Xu,Xinghe Xiang,Guangming Yang,Haoran Xu,Gang Xiao,Ran Ran,Wei Zhou,Zongping Shao
Efficiently converting CO2 into value-added fuels or chemicals is a significant target for reducing CO2 emissions and achieving carbon neutrality. Solid oxide electrolysis cells (SOECs) are devices where the CO2 reduction reaction (CO2RR) takes place with high efficiency and fast kinetics at high temperatures. Since the CO2RR occurring at the cathode side is a sluggish reaction over whole electrode reactions, it is crucial to develop innovative cathode materials with high activity and good durability. Here, we demonstrate a strategy to synergistically optimize the bulk properties of Sr2Fe1.5Mo0.5O6−δ (SFM) and the morphology of the exsolved nanoparticles (NPs) to enhance the CO2RR activity, electrochemical performance, and durability. The partial replacement with zinc in the Fe-site of SFM not only increases the oxygen vacancy concentration of perovskite bulk and improves the CO2 adsorption capacity, but also passivates in situ exsolution of Fe NPs and improves the active sites on the perovskite surface, thus enhancing CO2 electrolysis performance. A novel cathode, Sr2Fe1.4Zn0.1Mo0.5O6−δ (SFZM01), used in a La0.8Sr0.2Ga0.8Mg0.2O3−δ electrolyte-supported single cell, shows a high current density of 2.74 A cm−2 at 850 °C (1.6 V) and excellent durability when operated at a current density of −1.0 A cm−2 at 750 °C. These findings can guide the development of high-activity and stability catalysts for carbon capture and utilization.
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THIN SOLID FILMS
·
2023
·
IF 2.1
Xinkuai He,Ruqing Guo,Qingtian Zou,Jingjing Yang,Zhousi Hu,Luye Wu
The co-deposition behavior of Co +2 and Fe +2 in ethylene glycol (EG) are investigated using cyclic voltammetry (CV) techniques. These results imply that Co +2 species can accelerate the Co-Fe co-deposition, while Fe +2 can inhibit the reduction of Co +2 . Moreover, the two effects can be improved as Co +2 or Fe +2 concentration increases. Microstructural and compositional characteristics of the samples show that Co-Fe deposits with various Fe content can be obtained from anhydrous FeCl 2 and CoCl 2 in EG. Scanning electron microscopy imaging of the surfaces of these Co-Fe alloy coatings shows that they present a dense structure with spherical “nodules”, the size of which is related to the Fe content. The electrocatalytic activity for hydrogen evolution reaction (HER) on the Co-Fe coatings is also investigated. These results indicate that its electrocatalytic activity can be improved as Fe contents increase from 2.2 to 9.8 wt.% and the Co-Fe alloy with 9.8 wt.% Fe exhibits the high electrocatalytic activity for HER with an overpotential of 124 mV at 10 mA cm −2 in 1 M KOH.
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Journal of Materials Chemistry B
·
2023
·
IF 7
Mengmeng Zhang,Tianze Wu,Hui Zhang,Zhenxia Chen,Yannan Yang,Yun Ling,Yaming Zhou
Asymmetric carbon has emerged as an important material to enrich morphologies as well as enhance functions for bioapplications. Here, asymmetric mesoporous carbon hemispheres (CHS) integrated with γ-Fe2O3 and GdPO4 (Fe–Gd) nanoparticles are proposed and prepared for potential imaging-guided photothermal therapy (PTT). Interestingly, Fe–Gd/CHS contributes to an almost 1.5 times enhancement in light harvesting and photothermal conversion efficiency as compared with its corresponding spherical analogue. The possible underlying mechanism is discussed in view of the unique asymmetric structure-featured carbon. Further identification of the inherited photoacoustic (PA) and magnetic resonance (MR) imaging properties leads to the consequent in vivo evaluation of its imaging and PTT performances, which demonstrates its capability as a function-integrated system for potential theranostics.
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POLYMERS FOR ADVANCED TECHNOLOGIES
·
2023
·
IF 3.4
Xiaodong Jin,Xinyi Wu,Qinyong Liu,Shibing Sun,Suping Cui,Sheng Zhang,Chen Chen
In this work, a metal organic framework (Fe-MOF) with the effect of absorbing toxic gases and good compatibility was synthesized by chelating a novel organic ligand contained carbonization groups (reacted by tris(hydroxymethyl) aminomethane and 1,4-piperazine dialdehyde) with iron salt. Then, it was used as the synergist to improve the efficiency of intumescent flame retardant (IFR) within polystyrene (PS) substrate. With the addition of 20% IFR and 2% Fe-MOF, the obtained PS composites exhibited a limiting oxygen index (LOI) value of 28.3% and a UL rating of V-0. Moreover, the peak heat release rate (pHRR), total heat release (THR), and total smoke production (TSP) of PS composites were decreased by 77.6%, 35.2%, and 33.7%, respectively. According to the mechanism analysis, it was found that Fe-MOF mainly acted in the condensed phase, contributing to the existence of dense char residues with the presence of IFR system. In addition, the good compatibility of organic ligand in Fe-MOF with PS substrate could partially alleviate the deterioration of mechanical properties due to the addition of IFR. For PS-20%IFR/2%Fe-MOF, the impact strength was improved from 1.7 kJ/m 2 (PS-22%IFR) to 2.2 kJ/m 2 , the tensile strength was also increased from 21.3 MPa (PS-22%IFR) to 22.4 MPa.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Ying Zhu,Yifan Gao,Yiqing Lu,Yuanhui Cheng
Highly efficient electrochemical interfaces are significant for the oxygen reduction reaction (ORR). However, previous efforts have been mainly paid to design catalytic sites with high intrinsic activity and neglect the electrode/electrolyte interfaces, especially the noncovalent interactions in the outer Helmholtz plane (OHP). Herein, an Fe–N–C single-atom catalyst is synthesized and acts as the model catalyst to demonstrate the effect of noncovalent interactions on the ORR performance. Two specific molecules of THA+ and TEA+ with different structures and functional groups have been selected to tune the OHP through noncovalent interactions. TEA+ can adjust the OHP, improve the oxygen diffusion coefficient, and increase the double-layer capacitance. Therefore, TEA+ enhances the activity, selectivity, and stability of Fe–N–C single-atom catalysts toward the ORR. This provides a new approach to finding new directions in designing electrochemical interfaces beyond the intrinsic catalytic sites in acidic electrolytes.
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Polymers
·
2023
·Vol. 15
·期 18
·3728
·
IF 5
Lin Zhang,Xiaofei Zhang,Yingcai Gui
Coordination polymers (CPs) have attracted greater scientific attention as promising electrode materials for lithium–ion batteries (LIBs) due to their diverse and versatile structural chemistry. This study introduces a croconate-based one-dimensional CP, namely [Fe(C5O5)(H2O)3]n) (referred to as Fe-CP), as an efficient anode material with high-performance characteristics for rechargeable LIBs. The ligand with abundant redox sites coordinating to the transition metal ion endowed the anode material with a remarkable stability in the electrolyte, in addition to high capacity, high-rate capability, and high cycling performance during charging/discharging process. The Fe-CP has a unique chain-based supramolecular structure, setting it apart from other porous three-dimensional molecular materials. The presence of unrestricted channels between the chains facilitates the diffusion of lithium ions in this unique structure. When tested at 100 mA g−1over a range of voltages between 0.01 and 2.4 V, the Fe-CP anode demonstrated a noteworthy specific capacity of 521 mA h g−1over 140 cycles. Moreover, the Fe-CP anode material exhibited excellent rate performance and demonstrated favorable cyclability. Following exposure to high charging and discharging rates of 2 A g−1, the anode ultimately regained its initial capability when the current rate was back at 100 mA g−1.Keywords:coordination polymers;one-dimensional;croconate-based;anode
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