ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Shusheng Wan,Xiaojun Wang,Guiru Zhang,Yongcheng Wang,Jie Chen,Qiaoxia Li,Yixiao Zhang,Liwei Chen,Xiaoming Wang,Guang Meng,Kun Jiang
Utilizing renewable energy to produce green hydrogen from saline water electrolysis is becoming increasingly important yet is largely challenged by the sluggish oxygen evolution reaction kinetics, the competitive anodic chlorine evolution reaction, and the resultant electrode corrosion. Here, we report an electrochemically activated Ni-Fe oxyhydroxide catalyst that delivers an early onset potential of 1.51 V at 100 mA cm–2 within mimic saline water of 0.5 M NaCl + 1 M NaOH. During the electrochemical activation, ex situ X-ray radiation and in situ Raman characterizations reveal the structural reconstruction of amorphous Ni (oxy)hydroxide generation and electronic structure modulation from Fe intercalation. Headspace gas chromatography and iodine titration results confirm the ∼100% Faradaic efficiency toward O2 evolution on activated NiFeOxHy, whereas the long-term stability is assessed by an anion exchange membrane electrolyzer, demonstrating only 350 mV voltage decay during the 100 h continuous electrolysis at 500 mA cm–2.
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高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 24
·8728-8733
·
IF 9.48
Qun Liu,Dan Pan,Tingting Ding,Mengchao Ye,Fengjiao He
The spent pickling solution, which comes from the pickling process of iron and steel, is indispensable in the manufacturing industry. Iron gets dissolved in the acid solution during the pickling process. When the concentration of metal ions in the acid solution accumulates to a certain value, it cannot to be used to wash iron and steel materials and becomes spent pickling solution that should be treated before discharge. At present, spent pickling solutions are treated via neutralization precipitation techniques in industries. This treatment method has a large discharge of wastewater, and the cost is high due to which it cannot meet the needs of green cycle in industry production. In this study, a new method, which is based on the formation of quaternary ammonium salt precipitate in a strong acid solution, is proposed to treat the spent pickling solution. The spent pickling solution was recycled and reused by precipitation separation of iron ion. The quaternary ammonium salt was recycled by dissolving the obtained precipitate in an alkali solution. The new ferric hydroxide precipitate formed and quaternary ammonium salt was returned to the solution. In the whole process, only a few amount of alkali was consumed. The removal rate of iron ion was up to 99.72%. Compared with the traditional neutralization precipitation method, the acid is not consumed and it can be reused; the alkali was consumed only for the precipitation of iron ions, not for the neutralization of the acid. The proposed method is an effective and economic method for the recovery of the spent pickling solution. It is expected to satisfy the requirements of green cycle and environmental protection in industry production.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Zhifei Hu,Zejiao Wang,Mingming Wang,Zhigang Wang,Yuanyuan Chu,Xiaoyao Tan,Yunxia Hu,Tianjia Chen,Shaomin Liu
Dense metal membranes are widely studied due to their promising performance in hydrogen separation. In this work, the low-cost dense iron (Fe) hollow fiber membranes (FeHFMs) were developed via the phase inversion and high-temperature sintering method. By tuning the preparation conditions, two typical gas-tight hollow fibers referred to as the sandwich- and honeycomb-structured membranes were successfully synthesized. H 2 permeation behavior was well described by Sieverts equation based on the solution-diffusion mechanism. The sandwich-structured FeHFMs had an H 2 flux of up to 7.51 mmol m −2 s −1 when operated at a temperature of 850 °C. In comparison, the honeycomb-structured FeHFMs further enhanced the H 2 flux by a factor of 3.2 due to the optimized membrane morphology with only one single dense iron layer. The developed FeHFMs showed superior H 2 permeation stability in thermal shock tests (40 h) and long-term stability tests (120 h). This work also expanded the potential application horizons of the FeHFMs, which can be easily tailored into porous or dense structures by tuning the sintering conditions.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Peng Wang,Chenyu Gao,Qianpeng Dong,Lianlian Wang,Dianming Chu,Yan He,Wenjuan Bai
s The application of carbon nanotubes in materials science is rapidly expanding, leading to an increasingly urgent demand for large-scale synthesis. Central to the growth of carbon nanotubes is the development of effective catalysts; thus, the large-scale production of these catalysts becomes crucial for successful carbon nanotube synthesis. Extensive research has been conducted on the mechanisms and regulation of interfacial interactions between metals and supports during catalyst synthesis. This paper is based on the interface interactions between common metal catalysts such as Fe, Co, Ni, and Al 2 O 3 , and Fe-Co, Fe-Ni, and Fe-Co-Ni metal catalysts were prepared by a one-step method. The catalysts were synthesized through a "one-step process," and the formation mechanisms of bimetallic and trimetallic catalysts, as well as the influence of interfacial interactions on catalyst formation and catalytic activity, were thoroughly investigated. The results indicate that with the involvement of Fe, Co and Ni on the surface of Al 2 O 3 maintain a small size morphology due to interfacial interaction. Meanwhile, the nanoparticles form a doped structure with Al 2 O 3 , effectively avoiding the deactivation of nanoparticles caused by agglomeration. In addition, the three catalysts for growing CNTs were analyzed in order to investigate the effects of different concentrations of metal ratios and time of carbon source on the catalytic activity, which provides new ideas for improving the catalyst design system.
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高影响因子
Water Supply
·
2020
·Vol. 21
·期 3
·1016-1024
·
IF 0.9
Dong Zijun,Li Mu,Chen Meifen,Gu Yurong,Jiang Chengchun,Sun Feiyun
The transformation of iodide (I − ) and hypoiodous acid (IO − ) by Fe (II)-activated peroxydisulfate (PDS) in the presence of natural organic matter (NOM) was investigated. In the water of a reservoir in Shenzhen, four kinds of organic matter were detected: iodoform > diiodo-bromomethane > dibromo-iodomethane > dichloromethane. As pH increased from 3 to 10, I − conversion rate decreased from 31.0% to 11.0%. There is basically no iodic acid ( ) generated under alkaline conditions, probably due to these organic matters. When PDS concentration is low, PDS can oxidize part of I − to IO − , and the oxidation of I − into reaction and continued oxidation reaction exist at the same time, so some is generated in the system. As the proportion of Fe (II) increases, the generation rate of gradually increases. When Fe 2+ /PDS is 1:5, 2:5, and 3:5, the conversion rates of are 4.7%, 6.5%, and 8.4%, respectively. There are two main reasons for this: (i) the reaction of IO − produced in the system with humic acid (HA) inhibits the further conversion of IO − to ; (ii) both HA and I- in the system can react with PDS, resulting in a reduction in the oxidation rate of I − . Formation of I-DBPs by Fe (II)/PDS process in real water was evaluated. I-DBPs generation in various reaction conditions was examined. Existence of HA showed apparent inhibition on IO 3 − generation.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Ting Yang,Shisuo Fan,Yang Li,Qi Zhou
A high-efficient iron-based heterogeneous catalyst is desired to active peroxymonosulfate (PMS). Due to a large catalytic contribution of atomically dispersed Fe-N x sites, single-atom iron–nitrogen-carbon catalysts exhibit superior performance in the catalytic activation of PMS. Herein, a sequence of Fe-N-C SACs with atomically dispersed Fe-N x sites, Fe SA -N-C and Fe SA -N/C, were prepared from Fe-doped ZIF-8 and FePc@ZIF-8, respectively. Single-atom Fe-N x sites were confirmed to be the main active sites for PMS activation. Fe SA -N/C-20 with a higher density of Fe-N x sites exhibited superior catalytic performance to N/C, Fe SA -N-C, Fe SA -N/C-15, and Fe SA -N/C-25 for BPA degradation. Integrated with chemical quenching experiments, electron spin resonance (ESR), in-situ Raman spectra, and electrochemical analysis, a nonradical pathway was demonstrated to dominate the degradation of BPA in the PMS + Fe SA -N/C-20 system. More importantly, the nature of this nonradical pathway was found to be an electron-transfer regime instead of a high-valent iron or singlet oxygenation process. The BPA was adsorbed onto the Fe-N x site by a “donor–acceptor complex” mechanism to form a nonradical PMS* intermediate during the process. Benefiting from this mechanism, the PMS + Fe SA -N/C-20 system showed wide pH adaptation and high resistance to inorganic anions.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lei Su,Yifan Li,Zhenkai Wang,Yao-Yin Lou,Qi-Zheng Zheng,Zhangxiong Wu,Sheng-Peng Sun
Iron-based catalysts are widely used in peroxysulfate-based AOPs but suffering from low catalytic performance at neutral pH conditions, which limits the application in groundwater remediation. Herein, this study investigated the efficacy, mechanism and long-term durability of Fe-doped nitrogen carbon (Fe@NC) armor catalysts toward peroxysulfate activation for the degradation of anthropogenic phenolics (APs) in groundwater matrices. The results showed that nonradical activation of Oxone (i.e., HSO 5 – ) was obtained over the as-prepared Fe-3 % @NC-700 catalyst, high-valent Fe species ( Fe(IV) O) and 1 O 2 were identified as the dominant reactive species for the efficient degradation of APs by experiments and density functional theory (DFT) calculations. Notably, the DFT results indicated that HSO 5 – was favorably adsorbed on the Fe atoms owing to the electrostatic interaction, which transformed exothermically into SO 4 2– and 1 O 2 over Fe 3 C, accompanied by the generation of Fe(IV) O. Additionally, the Fe-3 % @NC-700 catalyst displayed long-term activity for in situ activation of Oxone in groundwater matrices without pH adjustment, resulting in ΔAPs: ΔOxone stoichiometry efficiencies at 4.2–5.0 % . Wheat seeds germination tests revealed that the biotoxicity of the treated water was reduced notably by the present catalytic system, which holds large potential application in treatment of APs-contaminated groundwater.
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高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hui Wang,Xuefeng Zhang,Xiangfeng Wu,Yewei Kang,Yirui Huang,Zhaoye Zhao,Ziyan Li,Tingting Zhou,Junchuan Wang,Wei Zhu,Chengsi Pan
Bimetallic iron-based metal organic frameworks (MFe-MOFs) exhibit promising photocatalytic properties but face challenges typical of pristine MOFs, including low photoresponsive activity, inadequate band gap regulation, and weak photoconductivity. Here, we designed porphyrin-based COFs (TpPAM-COFs) to serve as a shell grown on NH2-Fe-MIL-101 nanoparticles (NPs) using an in situ solvothermal approach. Subsequently, a ligand-anchoring full-range metallization process was applied to introduce hetero metal ions throughout the core–shell composites, establishing a type-II scheme heterojunction (Fe/Cu-M@PC-Cu) via covalent bonding between NH2-Fe/Cu-MIL-101 and Cu-TpPAM-COFs. The Cu-TpPAM-COF shell, with broad light absorption range, enhanced the generation of photogenerated electrons, facilitating the reduction of Cu2+ and Fe3+ within the Fe/Cu-M@PC-Cu heterojunction and promoting the regeneration of Cu+ and Fe2+ Fenton active sites. Moreover, rapid electron transfer between Fe3+ and Cu+ centers amplified the Fe3+/Fe2+ redox cycle, accelerating the catalytic decomposition of H2O2 and increasing ·OH radical production. Additionally, the optimized bandgap structure of Cu-TpPAM-COFs enhanced the oxidation capacity, as evidenced by the Fe/Cu-M@PC-Cu composite achieving exceptional photo-Fenton catalytic efficiency with 92.7% tetracycline hydrochloride (TCH) degradation in 35 minutes, surpassing that of most reported similar catalysts. Furthermore, the composite showed excellent stability, with only an 11.9% loss in photo-Fenton degradation efficiency after 8 cycles, highlighting its great potential for addressing challenging environmental pollutants.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Beizhao Chen,Meng Zhang,Li Wang,Li Li,Qi Han,Xun Liu,Mengxia Wang,Bei Liu,Yi Jiang,Zhongying Wang
The singlet oxygen ( 1 O 2 )-based nonradical AOP process, realized in carbon materials after nitrogen and metal doping, has drawn much attention in recent years. However, the exclusive generation of 1 O 2 in the specialized two-dimensional (2D) catalytic membranes and the associated contaminant degradation mechanisms remain unclear. Herein, a Fe-doped crystalline carbon nitride (Fe-CCN) material without additional nitrogen doping was developed to preferentially initiate 1 O 2 -based nanoconfined oxidation of organic pollutants in the 2D Fe-CCN membrane/PMS system. Density functional theory calculation revealed that the Fe-O-N configuration formed after Fe doping altered the electronic structure of Fe centers, enhancing PMS adsorption and promoting the thermodynamically favorable generation of the –O* intermediate, leading to fast and highly selective 1 O 2 generation. EPR characterization and ROS quenching experiment also confirmed that the Fe-CCN activated PMS, generating nearly 100 % 1 O 2 . The Fe-CCN membrane/PMS system exhibited excellent resistance to natural organic matter (NOM) interference and dramatically increased Bisphenol A (BPA) degradation kinetics, approximately 590 times faster than in conventional batch systems. Enhanced 1 O 2 exposure concentration within the Fe-CCN membrane nanochannels was supported by EPR data and 1 O 2 exposure simulations. Furthermore, The Fe-CCN membrane/PMS system showed wide pH tolerance, excellent pollutant degradation performance, and high stability. This work underscores the practical significance of 1 O 2 -based oxidation reactions in membrane-confined AOPs for the rapid and efficient removal of organic contaminants from water.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Bin Nie,Haojun Dong,Jincan Yan,Shengyu Zhang,Shuang Zhong
The activation of peroxymonosulfate (PMS) by heterogeneous catalysts presents an exciting but challenging strategy for degrading persistent organic pollutants in water. Iron oxychloride (FeOCl) is considered a promising heterogeneous catalyst due to its unique oxygen bridge structure, which could render it more active by facilitating the iron valence transitions between Fe(II) and Fe(III). However, the limited Fe(II)/Fe(III) conversion cycle rate hinders its catalytic activity, leading to unsatisfactory PMS activations in practical applications. Herein, we demonstrated the performance and the mechanistic pathway of enhanced FeOCl (CNFeOCl) catalytic activation using a graphitic carbon nitride (g-C 3 N 4 ) with a unique electronic structure as a carrier employing 2,4-dichlorophenol (2,4-DCP) as a representative pollutant. The CNFeOCl/PMS system achieved complete degradation of 2,4-DCP (30 mg/L) in a short time (<5 min), whereas the FeOCl/PMS system degraded only 35.98% under the same conditions. The high 2,4-DCP degradation rate of CNFeOCl was due to its improved Fe(II)/Fe(III) ratio (34.34%/40.03%), increased specific surface area (30.32 m 2 /g), and reduced charge-transfer resistance. Combining a series of characterizations, electron spin resonance (ESR) detection, and quenching experiments, the investigations elucidated the enhanced catalytic activation mechanism of CNFeOCl which includes dominant reactive oxygen species (ROS) generation and some key factors that generally affected the efficiency of oxidative degradation. We believe this study offers new insights into the intrinsic role of g-C 3 N 4 supported FeOCl for PMS activation and provides theoretical support to guide the rational design for developing efficient iron-based catalysts toward heterogeneous catalysis.
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Renjie Pan,Zongchen Li,Tian-Yang Zhang,Qi Fu,Zheng-Xiong Zheng,Jun Shi,Jian Lu,Chen-Yan Hu,Yu-Lin Tang,Mohamed Gamal El-Din,Bin Xu
Peracetic acid-based advanced oxidation processes (PAA–AOPs), which generate various reactive radicals, have garnered substantial attention for degradation emerging contaminants (ECs). However, nonselective radical-based PAA–AOPs often suffer from interference by water matrix components, causing low contaminants removal efficiency. This study explores the use of amino-(NH 2 )-functionalized metal–organic frameworks (MIL-101(Fe)-NH 2 ) as heterogeneous catalysts for PAA activation, enabling the generation of high-valent iron- (Fe)–oxo species (Fe(IV)) capable of efficiently degrading ECs (80 −100 %, within 30 min). The Fe(II) clusters in MIL-101(Fe)-NH 2 , modulated by electron-donating −NH 2 groups, play a pivotal role in Fe(IV) generation. Scavenger and probe experiments confirmed Fe(IV) as the primary reactive species responsible for ECs degradation. Density functional theory calculations demonstrated that the four-electron transfer to generate Fe(IV) has lower free energy than the two-electron transfer to generate organic radicals (e.g., CH 3 COO • and CH 3 C(O)OO • ). Furthermore, thermodynamically unfavorable CH 3 COO • desorption further promotes Fe(IV) generation. The PAA/MIL-101(Fe)-NH 2 system efficiently degraded SMX ( k app = 121.2 −287.2 M −1 s −1 ) and other ECs ( k app = 40 −432 M −1 s −1 ) with minimal interference from water matrix components and excellent reusability. This study demonstrates that MIL-101(Fe)-NH 2 is a robust catalyst for PAA activation and provides a novel approach for selectively generating Fe(IV) for ECs degradation.
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PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Xuecong Qian,Shilong Wang,Haijun Cheng,Luwei Li,Yun Liu,Jinhao Duan,Da Wang,Jun Ma
Fe(II) and Mn(II) are abundant in groundwater and require operationally simple and efficient method to remove in drinking water treatment. The rapid oxidation of Mn(II) is essential in water treatment. This study investigates the efficiency of Mn(II) oxidation by free chlorine in the presence of Fe(II). The results demonstrate that the presence of Fe(II) significantly accelerates the oxidation rate of Mn(II) by free chlorine under neutral and alkaline conditions. The rapid oxidation of Fe(II) by free chlorine and the presence of Mn(II) promote the formation of in situ Mn(II)-doped ferrihydrite. Kinetic modeling and characterization of Fe(III) oxides confirm that the heterogeneous catalytic effect of the Mn(II)-doped ferrihydrite, rather than manganese oxides or their coupled catalytic effect, is responsible for the enhanced oxidation rates. The doped Mn(II) substitutes the tetrahedral Fe(III) ions in the ferrihydrite, introducing additional negative charges at the doped sites. The increased charge enhances Mn(II) adsorption and lowers its redox potential, thereby accelerating Mn(II) oxidation rate through direct electron transfer with adjacent free chlorine. Additionally, the lepidocrocite formed by the reaction between Fe(II) and dissolved oxygen significantly impedes the catalytic performance. These findings provide new insights into the catalytic co-oxidation mechanism of Fe(II) and Mn(II), and help the optimization of water treatment engineering practices.
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