Materials
·
2021
·Vol. 14
·期 6
·1473
·
IF 3.623
Changhao Zhao,Fen Wei,Haolin Lv,Dengke Zhao,Nan Wang,Ligui Li,Nanwen Li,Xiufang Wang
It remains an urgent demand and challenging task to design and fabricate efficient, stable, and inexpensive catalysts toward sustainable electrochemical water splitting for hydrogen production. Herein, we explored the use of Fe(III) ion-assisted aniline polymerization strategy to embed bimetallic CoFeP nanospheres into the nitrogen-doped porous carbon framework (referred CoFeP-NC). The as-prepared CoFeP-NC possesses excellent hydrogen evolution reaction (HER) performance with the small overpotential (η10) of 81 mV and 173 mV generated at a current density of 10 mA cm−2in acidic and alkaline media, respectively. Additionally, it can also efficiently catalyze water oxidation (OER), which shows an ideal overpotential (η10) of 283 mV in alkaline electrolyte (pH = 14). The remarkable catalytic property of CoFeP-NC mainly stems from the strong synergetic effects of CoFeP nanospheres and carbon network. On the one hand, the interaction between the two can make better contact between the electrolyte and the catalyst, thereby providing a large number of available active sites. On the other hand, it can also form a network to offer better durability and electrical conductivity (8.64 × 10−1S cm−1). This work demonstrates an efficient method to fabricate non-noble electrocatalyst towards overall water splitting, with great application prospect.
研究领域:
材料科学
·
电化学
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RSC Advances
·
2026
·Vol. 16
·期 18
·16505-16511
·
IF 6.1
Cong Gao,Houfen Li,Jize Liu,Wenchao Yang,Hong Chen,Jianbo Han
The heterogeneous Fenton-like reaction is a promissing technology for removing organic pollutants in water. The reduction of Fe(III) to Fe(II), as the rate-limiting step for generating ˙OH, is crucial in heterogeneous Fenton-like reactions and may be improved using organic pollutants with lower redox potential than that of Fe(III)/Fe(II). In this work, the rapid reduction of Fe(III) to Fe(II) on the MIL-100-Fe catalyst was achieved by degrading methylene blue (MB, E0 = 0.01 V), which has the desired lower redox potential than that of MIL-100-Fe(III)/Fe(II) (E0 = 0.76 V). By contrast, organic pollutants with higher redox potentials than that of MIL-100-Fe, such as phenol (E0 = 0.97 V) and p-nitrophenol (E0 = 1.23 V), were incapable of reducing Fe(III) to Fe(II). As a result, the degradation rate constant of MB was one order of magnitude higher than those of phenol and p-nitrophenol. Notably, MB could also promote the reduction of Fe(III) to Fe(II) in the presence of phenol or p-nitrophenol; thus, the degradation rate constants of phenol and p-nitrophenol were significantly enhanced by 50 and 30 times, respectively. The results revealed that organic pollutants with lower redox potential than that of Fe(III)/Fe(II) could facilitate the reduction of Fe(III) to Fe(II), which is beneficial for producing more ˙OH, thus improving the heterogeneous Fenton-like catalytic performance.
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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yijun Chen,Meina Cheng,Yundong Wang,Long Jin,Juanhong Li,Hailiang Yang,Sanjian Ma,Guoliang Dai,Zixia Lin,Xin Liu
Both the iron sludge and usage of H 2 O 2 restrict the promotion of the Fenton reaction. Herein, we proposed a hydrogen-accelerated oxygen reduction Fenton reaction system named MHORF-UiO-66(Zr) to try to solve the two problems under normal temperature and pressure. The active hydrogen, which is derived from H 2 catalyzed by the composite of Pd/UiO-66(Zr), could accelerate the reduction of Fe(III) and promote the electron transfer of two-electron oxygen reduction reaction to realize the self-generation of H 2 O 2 . And 45.9 mM of H 2 O 2 could be detected. As expected, 91 % of trimethoprim (TMP) could be degraded within 30 min in this system in the condition of 25 μM Fe(II), H 2 30 mL·min −1 , and Pd/UiO-66(Zr) 2g·L −1 , which was 2.94 times that of the control Fenton system. Based on these results, the feasibility of fundamentally achieving zero emission of iron sludge was successfully verified. It was confirmed that both the hydroxyl radical and singlet oxygen played the dominant roles during the reaction process through the analysis of electron spin resonance spectroscopy. After six reaction cycles, the removal efficiency of TMP could be maintained at least 94 %. It found that both the properties and morphology of this composite could remain based on the systematic characterization.
研究领域:
环境科学
·
化学工程
·
催化材料
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Jinjuan Xue,Meng Yuan,Jiamin Gao,Zewu Zhang,Mingxin Wang,Shuaishuai Ma
In this work, a novel PCN-222 metal−organic framework based multitasking membrane was developed for separation of emulsified oils as well as photo-Fenton degradation of refractory aromatic pollutants and inactivation of pathogenic bacteria in water. Fe(III)@PCN-222 nanorods were prepared via impregnation method and subjected to amino-modification, and then robustly anchored on polydopamine (PDA) decorated PVDF membrane via catechol-amine reaction. The as-prepared N-Fe(III)@PCN-222/PDA/PVDF composite membrane exhibited underwater superoleophobicity, and showed high separation efficiency (above 99.4 %) as well as relatively favorable permeation flux (874.9–1592.3 Lm −2 h −1 ) in the separation of emulsified oils ranged from nanoscale to microscale from water. Meanwhile, the membrane serving as a recyclable photo-Fenton platform showed an extensive degradation capacity towards aromatic contaminants and high inactivation activity against bacteria under visible light. The grafted Fe(III) is used as an electron acceptor to promote the separation of photo-generated charge carriers, adjusted the band structure to shorten the bandgap value, and can be reduced to Fe(II) by photo-generated electrons as a Fenton-like catalyst. The photo-Fenton mechanism was studied in detail from the aspects of photoelectric properties, band structure and reactive oxygen species . This work could promote the application of PCN subclass MOFs based superwetting membrane as a recyclable platform for complex wastewater treatment .
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WATER RESEARCH
·
2022
·
IF 13.4
Siqi Liu,Andrey M. Kuznetsov,Weiqing Han,Alexei N. Masliy,Gregory V. Korshin
Methylated arsenic species are ubiquitous in the environment and resistant to removal by conventional treatment technologies. This study addressed this challenge based on the examination of the removal of dimethylarsinic acid (DMA) in a system that combines zerovalent iron (ZVI) and powdered activated carbon (PAC). The removal of DMA in the ZVI/PAC system was compared to that by coagulation, adsorption, electrochemical and Fenton oxidations, and other conventional methods. While only the electrochemical oxidation using a PbO 2 /Sb-SnO 2 /Ti anode allowed removing up to 60% DMA at several hours-long treatment times, the removal of DMA in the ZVI/PAC system containing 10 g/L ZVI and 2.5 g/L PAC with an initial pH of 2.0 was 95% for a 30 min reaction time. Specific roles of PAC, ZVI and its oxidation products in DMA removal were examined based on the spectroscopic data and quantum chemical modeling for the DMA/Fe(II) and DMA/Fe(III) systems. These methods demonstrated the formation of moderately strong DMA/Fe(II) and DMA/Fe(III) complexation. These results and relevant kinetic data were interpreted to indicate that the removal of DMA is governed by the rapid generation of Fe 2+ ions released as a result of accelerated ZVI corrosion in the galvanic ZVI/PAC microcells and ensuing formation of DMA/ Fe 2+ complexes that are readily adsorbed by PAC.
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CHEMOSPHERE
·
2021
·
IF 7.086
Peipei Huang,Lili Yao,Qing Chang,Yunhan Sha,Guodong Jiang,Shenghua Zhang,Zhe Li
The slow redox rate of Fe(III)/Fe(II) couples is a rate-limiting step for Fenton-like performance of Fe-MOFs. In this study, a series of catalysts (MIL-101) with various p-phthalic acid/2-aminoterephthalic acid (H 2 BDC/NH 2 –H 2 BDC) molar ratios were prepared using a simple and mild chemical method and applied for catalyzed degradation of bisphenol A (BPA). Interestingly, the –NH 2 modified MIL-101(Fe) can adjust Fe-Oxo node by increasing the electron density of Fe(III) in the presence of –NH 2 group with high electron density, thus forming Fe(II) in situ in MOFs. Meanwhile, the –NH 2 groups used as electron-donors can promote electron transfer , resulting in faster Fe(III)→Fe(II) half-reaction and active H 2 O 2 to continuously generate •OH radical. The BPA degradation and rate constant of Fe-BDC-NH 2 /H 2 O 2 system are 15.4-fold and 86.8-fold higher than that of Fe-BDC/H 2 O 2 system, respectively. The density functional theory (DFT) calculations showed that Fe-BDC-NH 2 possesses higher Fermi level energy (−4.88 eV) and lower activation energy barriers (0.32 eV) compared with Fe-BDC. Moreover, Fe-BDC-NH 2 showed good reusability and stability. This work offers a highly efficient and stable MOFs-based Fenton-like catalyst to rapidly degrade organic pollutants over a wide pH range for potential applications in wastewater treatment .
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MOLECULAR PHARMACEUTICS
·
2020
·
IF 4.321
Fabiao Hu,Ruihuan Zhang,Wei Guo,Ting Yan,Xiujuan He,Fengzhi Hu,Fuzheng Ren,Xingyuan Ma,Jiandu Lei,Wenyun Zheng
Biodegradable poly(lactic-co-glycolic acid) nanoparticles (PLGA NPs) have been widely used as delivery vehicles for chemotherapy drugs. However, premature drug release in PLGA NPs can damage healthy tissue and cause serious adverse effects during systemic administration. Here, we report a tannic acid–Fe(III) (FeIII–TA) complex-modified PLGA nanoparticle platform (DOX-TPLGA NPs) for the tumor-targeted delivery of doxorubicin (DOX). A PEGylated-PLGA inner core and FeIII–TA complex outer shell were simultaneously introduced to reduce premature drug release in blood circulation and increase pH-triggered drug release in tumor tissue. Compared to the unmodified NPs, the initial burst rate of DOX-TPLGA NPs was significantly reduced by nearly 2-fold at pH 7.4. Moreover, the cumulative drug release rate at pH 5.0 was 40% greater than that at pH 7.4 due to the pH-response of the FeIII–TA complex. Cellular studies revealed that the TPLGA NPs had enhanced drug uptake and superior cytotoxicity of breast cancer cells in comparison to free DOX. Additionally, the DOX-TPLGA NPs efficiently accumulated in the tumor site of 4T1-bearing nude mice due to the enhanced permeability and retention (EPR) effect and reached a tumor inhibition rate of 85.53 ± 8.77% (1.31-fold versus DOX-PLGA NPs and 3.12-fold versus free DOX). Consequently, the novel TPLGA NPs represent a promising delivery platform to enhance the safety and efficacy of chemotherapy drugs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Cheng Chen,Yongyi Wang,Yajing Huang,Jian Hua,Wei Qu,Dehua Xia,Chun He,Virender K. Sharma,Dong Shu
Applications of Fenton-like reactions (Fe(III)/H 2 O 2 ) without catalyst have low efficiency in remediating pollutants. Herein, pollutants containing phenolic moiety (P, e.g., paracetamol (PCM)) were demonstrated to make Fe(III)/H 2 O 2 system highly effective in degrading a wide range of contaminants. Kinetics analysis shows the self-catalytic degradation of PCM with optimum performance at pH 4.0, and Fe(III)/Fe(II) conversion was accelerated without the assistance of cocatalyst. Based on state-of-art spectroscopy measurements and theoretical calculations, the overlooked self-catalytic mechanism was revealed. In the presence of phenolic moiety, a yellow-colored high-spin P-Fe(III)-OOH complex can be formed in Fe(III)/H 2 O 2 system, which subsequently converts to Fe(II). Afterwards, the oxidation of P gives hydroquinone that also facilitates the cycling of Fe(III)/Fe(II). The accumulated Fe(II) reacts with H 2 O 2 to generate hydroxyl radicals, the major species responsible to oxidize pollutants, thereby achieving efficient decontaminant performance. Results provide new insights into the self-catalytic Fenton-like process for remediating a mixture of pollutants.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 29
·13619-13625
·
IF 3.3
Xuequan Jing,Jiaming Liu,Meina Guo,Guoliang Chen,Guoqing Ren,Jiarong Li,Haonan Qin,Zhangwei Yao,Yinhua Wan,Weijie Song,Huifeng Zeng,Feifei Yang,Da Zhao,Kang Hu
It is critical to detect Fe3+ and Al3+ rapidly and accurately due to their high risk to humans and the ecological environment. In this work, a kind of terbium-based metal–organic framework fluorescent probe (Tb-MOF) is facilely fabricated that displays ultra-high selective detection of Fe3+ and Al3+ over various coexisting ions (i.e. Mn2+, Co2+, K+, Ca2+, Na+, Mg2+, Cd2+, Cu2+, Fe2+, Zn2+, Ni2+, Pb2+ and Cr3+). The obtained Tb-MOF exhibits emission at 547 nm and possesses outstanding thermal, fluorescent and chemical stability. The Tb-MOF shows a ratiometric fluorescence signal for Al3+, and the detection limits for Fe3+ and Al3+ are 0.91 and 6.10 μM, respectively. Moreover, the fluorescence intensities and concentrations of Fe3+ and Al3+ have good linear relationships across wide concentration ranges. Furthermore, the quantifications of Fe3+ and Al3+ are achieved in complex tap and river water samples with good recoveries. This study offers a facile and efficient method of developing a fluorescent probe that possesses the ability to quantify Fe3+ and Al3+ in real environmental water samples.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Yu Chen,Yajing Li,Yongjian Wang,Igor Ying Zhang,Rongfu Huang
This work investigated the activation of peroxymonosulfate by electrochemical (EC) system assisted with Fe(III)-nitrilotriacetic acid (NTA) complex for degradation of persistent naphthenic acids (NAs) under neutral initial pH conditions. As NAs are a complicated mixture, 1-adamantanecarboxylic acid (ACA) was selected as the model NA compound for degradation experiment. The addition of NTA is to chelate with Fe(III), gaining stability under neutral pH condition to facilitate the circulation of Fe(II)/Fe(III) by the electrochemical process to activate PMS. The EC/Fe(III)-NTA/PMS system was explored with applicable pH range of 3–9 and an optimized molar ratio 1: 2 for Fe: NTA. Results of quenching and chemical probe experiment together with results of electron paramagnetic resonance (EPR) analysis revealed the main reactive species of the system, including • OH, SO 4 •− , 1 O 2 and possibly Fe(IV). With the addition of NTA, the yields of • OH, SO 4 •− , 1 O 2 were enhanced. Results of mass spectrometry analysis and DFT calculations indicated the formation of 9 degradation byproducts of ACA via three primary degradation pathways such as hydroxyl substitution, carbonyl substitution, and decarboxylation . Furthermore, the EC/Fe(III)-NTA/PMS system could achieve excellent removal efficiency of ACA with different anions such as Cl - , HCO 3 - , NO 3 - and H 2 PO 4 - in the background. The practical applicability of the system was also verified with the high removal of commercial NAs mixture standard. Overall results have indicated the EC/Fe(III)-NTA/PMS system could be utilized for efficient reclamation of authentic oil and gas industrial wastewater under natural pH conditions.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 8
·2066-2076
·
IF 7.3
Jiahui Zhou,Xuesong Li,Qiuying Yi,Zhiwei Wang
Heterogeneous Fenton-like processes based on Fe-based catalysts are effective technology to degrade emerging organic pollutants in water and wastewater such as tetracycline (TC). However, the kinetically limited redox cycling between Fe2+ and Fe3+ is still a persistent challenge for their widespread application. To address this issue, we designed a novel Fe-based catalyst by coating reduced iron powder (RIP) with ferroferric oxide nanoparticles (FONP@RIP) using a simple chemical co-precipitation method. The reduced iron could rapidly reduce Fe(III) to Fe(II) and accelerate the cycle of Fe(II)/Fe(III) in the heterogeneous Fenton-like system. Benefiting from the accelerated cycle of Fe(II)/Fe(III), TC could be efficiently degraded in the FONP@RIP/H2O2 system over a wide pH range of 3–6, with a removal efficiency of 94.5% within 60 min (TC0 = 150 ppm). The predominant reactive oxygen species were identified as ˙OH and HO2˙. Based on the identified intermediates, the possible pathway of TC degradation was deduced and the toxicity of pollutants could also be significantly reduced during the degradation process. Moreover, FONP@RIP exhibited stable catalytic performance during multiple cyclic tests with only a marginal loss of catalytic components. This study presents a new catalyst design strategy for heterogeneous Fenton-like processes, which provides a promising way for the degradation of residual antibiotics in water and wastewater.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2017
·
IF 4.421
Xian-Lei Shi,Yongju Chen,Qianqian Hu,Feng Wang,Peigao Duan
An efficient, recyclable and large-scalable fiber-supported Fe(III) catalytic system verifed in the one-pot multicomponent Biginelli reactions, is presented. The fiber catalyst was prepared conveniently from commercially available polyacrylonitrile fiber according to a simple two-step procedure by amination and chelation in water, and characterized detailedly with ICP analysis, morphology, mechanical properties, elemental analysis, FTIR spectroscopy, and SEM during the modification and utilization processes. Moreover, the fiber catalyst-mediated reactions showed broad applicability and proceeded smoothly to afford a series of substituted 3,4-dihydropyrimidin-2-(1 H )-ones/-thiones (yields 81–94%) in ethanol under mild conditions. Furthermore, the newly developed fiber catalyst held high strength, good flexibility and exhibited excellent stability and recyclability (over 10 cycles), and the procedure was operationally concise and effectively amenable to the gram-scale on a simple fixed-bed reactor with potential industrialization prospect.
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危险品化学品经营许可证（带存储）