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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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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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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FOOD CHEMISTRY
·
2023
·
IF 8.8
Xinrou Wang,Huan Liu,Cailin Qiao,Yi Ma,Huibo Luo,Changjun Hou,Danqun Huo
Traditional methods of tannins detection suffer from complex pretreatment, long detection time, and limited sensitivity. Modern techniques like liquid chromatography require expertise, involve tedious result processing, and lack effective data visualization. Therefore, there is a need for an alternative detection method that simplifies pretreatment and detection steps, reduces analysis time, and provides visualized results. In this study, a novel colorimetric sensor based on single-atom Fe nanozyme (Fe@CN-20) was developed for tannins detection. Fe@CN-20 exhibited laccase-like and oxidase-like activities, enabling simultaneous oxidation of tannins and a substrate called TMB. Tannins competed with TMB, allowing quantification of tannins content. The Fe@CN-20/TMB system provided a detection range of 5–100 mg/L tannic acid, with a detection limit of 0.13 mg/L (S/N = 3). Analysis time was approximately 30 min. The platform successfully quantified tannins in brandy, showing less than 5% deviation compared to the standard method. The sensor was simple, sensitive, rapid, and provided strong visualization.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Changrong Zhao,Bin Liu,Tingting Zhu,Xuewu Zhu,Xiaoxiang Cheng
Advanced oxidation is an effective method for removing hard-to-degrade organic pollutants from water. In this paper, a novel structure of a single atom Fe anchored g-C 3 N 4 (FeCN) membrane was proposed to remove pollutants from water by coupling membrane technology with photocatalytic and peroxyacetic acid oxidation. The presence of zero-dimensional Fe atoms in FeCN membranes allows for the removal of acetaminophen (APAP) in mobile membrane filtration systems without compromising permeation performance by simultaneously possessing visible photocatalytic capability and peroxyacetic acid (PAA) activation. Existence of inter-membrane domain-limiting conditions led to 100 % degradation of APAP within 10.5 ms, which is 5 orders of magnitude faster than conventional catalytic systems. Notably, photo-generated electrons/holes generated by light and HClO generated by Cl - promote the conversion of Fe(V) and the removal of pollutants during the catalytic process. The spatial separation ability of the membrane catalytic layer surface mitigates the catalyst's passivation by macromolecular organics. Furthermore, surface photocatalysis of the membrane and interlayer catalysis generated by PAA mitigate the surface and interlayer pollutants of the membrane, respectively. This study explores a novel approach for the development of highly efficient atom-catalyzed membrane systems with multiple purposes.
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Journal of Cleaner Production
·
2024
·
IF 9.7
Zhengshuai Sun,Rujiao Jiang,Wenbin Hua,Qi Wei,Qiaoxia Yuan,Baojun Yi
Biomass-based graphitic carbon is a promising material, but the effect mechanism of inherent alkali metals on the catalytic pyrolysis of biomass is still unclear. In this study, cellulose was selected as the model substance, and the influence mechanism of Na on the graphitization of cellulose catalytic pyrolysis was investigated through a combination of experiments and theoretical calculations. The results indicate that Na can interact with the carbon skeleton through van der Waals forces, thereby altering the spatial structure of graphite crystals and increasing the interlayer spacing of graphite by 27.7%. In addition, Na can coexist with Fe(III) in the form of oxides, while also increasing the reaction energy barrier of reverse hydroxylation and dehydration cyclization, decreasing the generation of reducing gases mainly composed of CO. This impedes the reduction of iron-based catalysts, thereby affecting the formation of the graphite microcrystalline structure. The research indicates that maintaining the ratio of Na content to iron-based catalysts within a 1:1 range is optimal for producing graphite carbon from cellulose.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhuo-Yu Li,Yu-Lei Liu,Pei-Nan He,Xin Zhang,Lu Wang,Hai-Teng Gu,Hao-Chen Zhang,Jun Ma
Hydroxylamine is commonly known to enhance the performance of Fe(II)-based advanced oxidation processes (AOPs) by promoting Fe(II) regeneration from Fe(III). Recently, ferryl ion (Fe(IV)) was found as an important reactive specie in Fe(II)/peroxydisulfate (PDS) system, while the interaction between hydroxylamine and Fe(IV) in Fe(II)/hydroxylamine/PDS system was still ambiguous. Therefore, the role of hydroxylamine, especially in interaction with reactive species, was systematically studied therein. With methyl phenyl sulfoxide (PMSO) as a probe compound, an original function of hydroxylamine to transform the major reactive species from Fe(IV) to radicals (SO 4 - and OH) for potential pollutants oxidation was clarified. Experimental results combined with Density Functional Theory (DFT) calculations showed that SO 4 - , OH and Fe(IV) all contributed to PMSO oxidation. Hydroxylamine showed the greatest promotional effect on the production of SO 4 - , while the production of Fe(IV) was inhibited with concentrations of hydroxylamine increasing from 0.2 to 1.4 mM. Compared with PMSO, hydroxylamine showed stronger scavenging ability towards Fe(IV) than SO 4 - and OH. Thus, more than 50% of radicals was consumed by PMSO and Fe(IV) mainly reacted with hydroxylamine to regenerate Fe(II). In a word, hydroxylamine played a dual role during potential pollutants oxidation in Fe(II)/hydroxylamine/PDS system, namely (1) transforming the major reactive species from Fe(IV) to radials (SO 4 - and OH) and (2) regenerating Fe(II) from both Fe(IV) and Fe(III). This study provides an insight into the role of hydroxylamine and its interactions with Fe(IV), which advances our understanding on similar Fe(II)/reductants/PDS systems.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 5
·056523
·
IF 4.316
Xiansen He,Xiaokun Li,Suxiang Feng,Xueying Li,Cuijie Nong
In this study, a novel photoelectrochemical (PEC) sensor based on FeMoSe2 was developed for the detection of berberine hydrochloride (BRH). The photosensitive material Fe-doped MoSe2 (FeMoSe2) was prepared by a simple hydrothermal method. Compared with MoSe2, FeMoSe2 shows superior PEC performance for the sensitive detection of BRH under blue light. Under the best experimental conditions, the PEC sensor presented a wide detection range of 0.025–15.0 μM with a detection limit of 8.4 nM. Therefore, the PEC sensor is considered an effective analytical method for detecting BRH. Moreover, the PEC sensor has good reporducibility and stability. Eventually, the proposed sensor was successfully applied to detect two different types of BRH tablets. This project provides a new pathway for detecting BRH.
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CHEMOSPHERE
·
2021
·
IF 7.086
Zeyu Wang,Luyao Dai,Jiachao Yao,Tianjiao Guo,Dzmitry Hrynsphan,Savitskaya Tatsiana,Jun Chen
Multi walled carbon nanotubes (MWCNTs) have attracted more and more attention as adsorbents due to their excellent adsorption properties. By loading metal particles on MWCNTs, the chemical reduction ability of adsorbed pollutants could be provided, so as to achieve the purpose of adsorption and degradation of pollutants. Therefore, the removal process of NO 3 − -N by Fe–Pd–Fe 3 O 4 /MWCNTs was studied, including rapid adsorption of initial pollutants, gradual reduction of intermediate products and re-adsorption of final products. The results showed that Fe–Pd–Fe 3 O 4 /MWCNTs completely removed NO 3 − -N within 2 h, 39% and 25% of which were converted into NO 2 − -N and NH 4 + -N. The adsorption efficiency, kinetics, capacity and adsorption energy all followed the order of NH 4 + -N > NO 2 − -N > NO 3 − -N. With the recoverability and reusability of Fe–Pd–Fe 3 O 4 /MWCNTs having been confirmed in 5 consecutive cycles, the removal rate of NO 3 − -N still reached 43%. It has been shown that MWCNTs prolonged the reducing power for NO 3 − -N, due to avoiding the aggregation of metal particles. The rapid adsorption of initial pollutants, effective stepwise reduction and convenient recovery processes were of great value for the rehabilitation of polluted water.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Hongwei Luo,Chenyang Liu,Ying Cheng,Yifeng Zeng,Dongqin He,Xiangliang Pan
The biggest problem with Fe/PMS (peroxymonosulfate) system is the slow generation rate of SO 4 − due to inefficient Fe 3+ /Fe 2+ cycle and the low decomposition efficiency of PMS . Here, we report the Fe 3+ -enhanced decomposition of PMS by a two-dimensional transition metal dichalcogenide WS 2 for pollutant degradation and E. coli disinfection. Experimental results showed that the removal rates of six representative pollutants were all above 90% under various pH conditions. Over a wide range of pH values (2–9), the removal rate of carbamazepine (CBZ) in PMS/WS 2 /Fe 3+ system almost reached 100% within 10 min, and E. coli could be inactivated by 97.3% within 1 min. WS 2 in the system accelerated the Fe 3+ /Fe 2+ cycle and participated in the activation of PMS. Electron paramagnetic resonance (EPR) measurements and scavenging experiments demonstrated that the SO 4 − and HO radicals were the main active oxidative species. The degradation pathway of CBZ was revealed based on its intermediates as determined by liquid chromatograph-mass spectrometer (LC-MS). The presence of common anions such as Cl − and HCO 3 − in PMS/WS 2 /Fe 3+ system noticeably affected the CBZ degradation. The characterization results verified the structural stability and the reusability of WS 2 . These research findings suggest that the combination of Fe 3+ and WS 2 is a promising method for PMS activation to remove organic pollutants and inactivate pathogenic bacteria during the process of wastewater treatment .
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CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Yurun Feng,Xue Guo,Junbin Lu,Jie Liu,Guantong Wang,Hongyu Gong
The SiCN(Fe) fibers with excellent one-dimensional microstructure and electromagnetic wave (EMW) absorption performance were synthesized by combining polymer-derived ceramics (PDCs) method and electrospinning. The in-situ generation of Fe 3 Si and CNTs by adding ferric acetylacetonate (FA) into the raw materials effectively improved the dielectric properties , magnetic properties and the impedance matching performance of the SiCN(Fe) fibers. The EMW absorption performance of SiCN(Fe) fibers were mainly based on dipole polarization loss, interface polarization loss and eddy current loss. The RL min value of SiCN(Fe) fibers reached −47.64 dB at 1.38 mm and the effective absorption band (EAB, RL ≤ −10 dB) reached 4.28 GHz (13.72–18 GHz, 1.35 mm).
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