Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Xianxian Sheng,Yulong Liu,Mudassir Habib,Shuguang Lyu
In the advanced oxidation process for the remediation of organic contaminated water and soil, sodium percarbonate (SPC) is regarded as a potential oxidant. Iron sulfide (FeS) was chosen as an activator in this work for assisting fluoranthene (FLT) removal, with Fe(III) addition overcoming the solution pH constraint on FLT removal in the SPC/FeS process. At the optimal chemical dosages, SPC/FeS (pH = 3.0) and SPC/FeS/Fe(III) (pH = 5.7) processes removed approximately 100% and 92.8% of FLT, respectively. Based on the results of scavenging trials and electron paramagnetic resonance analysis, HO• was the dominant reactive oxygen species in FLT removal by SPC/FeS and SPC/FeS/Fe(III) processes. Dissolved oxygen (DO) played a crucial role in FLT removal, and SPC/FeS/Fe(III) process was more dependent on DO than SPC/FeS process. Both processes overcame the limitation of Cl – on the application of SPC-induced oxidation process. In actual groundwater experiments, 95.5% of FLT was removed in SPC/FeS/Fe(III) process at an initial solution pH of 5.0. In soil slurry trials, 12 h was the optimal reaction time for FLT removal, and the SPC/FeS and SPC/FeS/Fe(III) processes degraded 85.6% and 86.7% of FLT, respectively. In conclusion, the FeS-activated SPC-induced oxidation process offers perspectives for PAHs contaminated field decontamination and contributes to the optimization of modern oxidation methods.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2023
·Vol. 120
·期 25
·e2301011120
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IF 11.1
Fa Yang,Ping Song,Xin Ge,Yan Wang,Takao Gunji,Wei Zhang,Xiao Zhao,Weilin Xu
As a sustainable approach for N2 fixation, electrocatalytic N2 reduction reaction (N2RR) to produce ammonia (NH3) is highly desirable with a precise understanding to the structure-activity relationship of electrocatalysts. Here, firstly, we obtain a novel carbon-supported oxygen-coordinated single-Fe-atom catalyst for highly efficient production of ammonia from electrocatalytic N2RR. Based on such new type of N2RR electrocatalyst, by combining operando X-ray absorption spectra (XAS) with density function theory calculation, we reveal significantly that the as-prepared active coordination structure undergoes a potential-driven two-step restructuring, firstly from FeSAO4(OH)1a to FeSAO4(OH)1a′(OH)1b with the adsorption of another –OH on FeSA at open-circuit potential (OCP) of 0.58 VRHE, and subsequently restructuring from FeSAO4(OH)1a′(OH)1b to FeSAO3(OH)1a″ due to the breaking of one Fe-O bond and the dissociation of one –OH at working potentials for final electrocatalytic process of N2RR, thus revealing the first potential-induced in situ formation of the real electrocatalytic active sites to boost the conversion of N2 to NH3. Moreover, the key intermediate of Fe-NNHx was detected experimentally by both operando XAS and in situ attenuated total reflection–surface-enhanced infrared absorption spectra (ATR-SEIRAS), indicating the alternating mechanism followed by N2RR on such catalyst. The results indicate the necessity of considering the potential-induced restructuring of the active sites on all kinds of electrocatalysts for such as highly efficient ammonia production from N2RR. It also paves a new way for a precise understanding to the structure-activity relationship of a catalyst and helps the design of highly efficient catalysts.
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Nanomaterials
·
2022
·Vol. 12
·期 19
·3472
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IF 5.719
Hongwei Tang,Mengyue Liu,Lingna Kong,Xiaoyan Wang,Yue Lei,Xige Li,Yan Hou,Kun Chang,Zhaorong Chang
In this paper, a series of Fe3O4/MoS2/NiS composite electrodes were synthesized by a simple coprecipitation method. The influence of different ratio additives (MoS2and NiS) on the performance of iron anodes for Ni-Fe batteries was systematically investigated. In this paper, the mixed alkaline solution of 6 mol/L NaOH and 0.6 mol/L LiOH was used as electrolyte, and sintered Ni(OH)2was used as counterelectrode. The experimental results show that the MoS2and NiS additives can effectively eliminate the passivation phenomena in iron electrodes, reduce the electrode polarization, and increase the reversibility capacity. As a result, the Fe3O4/MoS2/NiS composite electrodes exhibit a high specific capacity, good rate performance, and long cycling stability. Especially, the Fe3O4/MoS2(5%)/NiS (5%) electrode with a suitable ratio of additives can provide excellent electrochemical performance, with high discharge capacities of 657.9 mAh g−1, 639.8 mAh g−1, and 442.1 mAh g−1at 600 mA g−1, 1200 mA g−1, and 2400 mA g−1, respectively. This electrode also exhibits good cycling stability.Keywords:nickel-iron battery;iron anode;Fe3O4;sulfide additives
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Catalysts
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2022
·Vol. 12
·期 11
·1363
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IF 4.501
Haimei Chen,Shaofei Wang,Lilan Huang,Leitao Zhang,Jin Han,Wanzheng Ren,Jian Pan,Jiao Li
The preparation of heterogeneous Fenton catalysts with both adsorption and catalytic properties has become an effective strategy for the treatment of refractory organic wastewater. In this work, 4A-Fe@Cu bimetallic Fenton catalysts with a three-dimensional core-shell structure were prepared by a simple, template-free, and surfactant-free methodology and used in the adsorption and degradation of Congo red (CR). The results showed that the open three-dimensional network structure and the positive charge of the surface of the 4A-Fe@Cu catalyst could endow a high adsorption capacity for CR, reaching 432.9 mg/g. The good adsorption property of 4A-Fe@Cu for CR not only did not inactivate the catalytic site on 4A-Fe@Cu but also could promote the contact between CR and the active sites on the catalyst surface and accelerate the degradation process. The 4A-Fe@Cu bimetallic catalyst exhibited higher catalytic activity than monometallic 4A@Cu and/or 4A-Fe catalysts due to low work function value. The effects of different pH, H2O2dosages, and catalyst dosages on the catalytic performance of 4A-Fe@Cu were explored. In the conditions of 7.2 mM H2O2, 2 g/L 4A-Fe@Cu, and 1 g/L CR solution, the degradation ratio of CR by 4A-Fe@Cu could reach 99.2% at pH 8. This strategy provided guidance to the design of high-performance Fenton-like catalysts with both adsorption and catalysis properties for dye wastewater treatment.Keywords:fenton reaction;Fe/Cu bimetallic catalyst;congo red;adsorption;catalysis
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Huaiyang Chen,Xiaoping Shen,Zhenyuan Ji,Jia Cheng,Guangxiang Liu,Leiming Lang,Yao Chen
In this paper, porous Mn 3 O 4 –Fe 3 O 4 nanoparticles with highly uniform composition are in-situ anchored on reduced graphene oxide (rGO) nanosheets by a simple cyanometallic framework template method . Thanks to the synergistic effects between the porous Mn 3 O 4 –Fe 3 O 4 nanoparticles and the well-conductive rGO nanosheets, the Mn 3 O 4 –Fe 3 O 4 /rGO composites present superior electrochemical lithium storage performances with a great reversible capacity of 1013 mAh g −1 after 100 cycles at 0.1 A g −1 , satisfactory rate capability of 510 mAh g −1 at 3.0 A g −1 , and eminent long-term cycle stability of 804 mAh g −1 after 500 cycles at 0.5 A g −1 . It is demonstrated that the rGO can not only act as a conducting matrix, but also buffer the volume expansion and avoid the aggregation of the Mn 3 O 4 –Fe 3 O 4 nanoparticles during charging-discharging. The work provides a simple strategy for designing and fabricating advanced multi-component metal oxide-based anodes for high-performance lithium-ion battery.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2022
·Vol. 414
·期 26
·7741-7751
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IF 4.478
Liu Yuqian,Hu Xianyun,Liang Fangyuan,Cao Yajing
Exploring sensors based on Förster resonance energy transfer (FRET) systems enables the continuous development of biological sensing technologies. Herein, we report the construction of a FRET sensor with dual-emissive quantum dots (QDs) and meso -tetra(4-sulfonatophenyl) porphine (TSPP). The sensor is composed of mesial green-emissive QDs with a thick silica shell (gQD@SiO 2 ) and circumjacent blue-emissive QDs coated with ultra-thin silica spacer, on which is linked TSPP (bQD@SiO 2 -TSPP). The gQD@SiO 2 endows the sensor with a fluorescent background. Due to the ultra-thin silica spacing, coupled with the superior resonance effect of bQD fluorescence and the Soret-band absorption of TSPP, the FRET efficiency is highly sensitive to the chelation state of TSPP. Relying on the absorbance transition of TSPP complexed with Fe(III), the FRET sensor is applied for ultra-sensitive Fe(III) detection. In aqueous solution, the sensor is demonstrated to linearly detect Fe(III) in the range of 0–1 μM, with a limit of detection (LOD) of 40 nM. More importantly, reliable Fe(III) detection can be achieved via the specific complexation of Fe(III) by TSPP and the ratiometric fluorescent response. As such, the inter-/intra-day precisions in standard samples, as well as the recovery rate in biological matrices, are fully validated. The excellent analytical performance, in combination with the excellent biocompatibility of the FRET sensor, allows semi-quantitative Fe(III) imaging in living cells. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Jing Wu,Jiabing Li,Gary Owens,Zuliang Chen
The widespread use of antibiotics, such as oxytetracycline (OTC) and levofloxacin (LEV), has led to dangerous levels of environmental contamination. In this study, functionalized iron/manganese nanoparticles (Fe/Mn NPs), which act as both adsorbent and Fenton catalyst, were green-synthesized using a reducing agent derived from a tea extract. The resulting pre-sorption/Fenton-like oxidation system effectively removed both OTC and LEV from the aqueous solution with adsorption capacities of Fe/Mn NPs for OTC and LEV of 58.8 and 192.3 mg·g −1 , respectively. In addition, Fe/Mn NPs also showed high catalytic activity, oxidizing more than 99.9 % of both OTC and LEV, while sodium persulfate (PDS) removed only 26.6 and 29.0 % of OTC and LEV, respectively. Mechanisms of PDS activation typically involve either catalyst-initiated or mediated electron transfer reactions. Fe/Mn NPs through heterogeneous catalytic and metal leaching-induced homogeneous Fenton reactions, which generated various reactive oxygen species (ROS) including 1 O 2 , ·OH, SO 4 - · and ·O 2 – . Characterization of Fe/Mn NPs before and after reaction, and the identification of specific OTC and LEV degradation products by LC-MS, helped to elucidate a potential degradation pathway, as well as the removal mechanism. Finally, the practicality of using this system for wastewater treatment was demonstrated using real wastewater samples indicating that the system has great potential for simultaneously degrading both OTC and LEV in contaminated wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Zihao Hu,Beiyang Guo,Huiqi Wu,Fang Zhu,Sridhar Komarneni,Jianfeng Ma
In this paper, MIL-101(Fe) and MoS 2 composites (MIL-101(Fe)/MoS 2 ) were synthesized using a facile solvothermal method . As a new degradation system, the synthesized composites were investigated using persulfate (PS) activation based on visible light (Vis). To establish the superiority of a heterogeneous photochemical catalysis system, the MIL-101(Fe)/MoS 2 was used as the catalyst in the presence of Na 2 S 2 O 8 with visible light irradiation. In the system mentioned, the MIL-101(Fe)/MoS 2 catalyst presented a much better catalytic ability than that of either a single photocatalysis or chemocatalysis system. The better catalytic ability suggests that the MIL-101(Fe)/MoS 2 catalyst was capable of effectively integrating photocatalysis and chemocatalysis leading to the highest degradation efficiency of 85% in 40 min with tetracycline as the target pollutant. The catalytic system MIL-101(Fe)/MoS 2 /PS/Vis degraded TC pollutant by forming species of O 2 ‾, 1 O 2 , hydroxyl radicals (•OH) and sulfate radicals (•SO 4 ‾) to degrade TC. Furthermore, the MIL-101(Fe)/MoS 2 catalyst displayed better catalytic performance compared to those materials that were previously reported, as verified by the good stability (reached 80% after three cycles) and the high TC degradation rate (85%) of the currently developed material. This system may be applicable to the degradation of TC and other challenging organic pollutants .
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Jingshun Shen,Qi Liu,Qiqi Sun,Jianwei Ren,Xue Liu,Zuoxu Xiao,Chuanwang Xing,Yuexing Zhang,Guangwu Yang,Yanli Chen
A novel two-dimensional (2D) single-atom Fe/N/C catalyst (Fe 1 Zn 30 NC PDI ) has been prepared upon pyrolyzing a well-designed quasi-Fe-/Zn-phthalocyanine-based polymer (qFePc 1 @qZnPc 30 @PDI). In the qFePc 1 @qZnPc 30 @PDI precursor, qFePc moieties containing Fe-N 4 sites are efficiently segregated by lots of qZnPc moieties connected together by perylene linkers, which not only leads to the larger specific area in the resulting Fe 1 Zn 30 NC PDI but more importantly ensures the in-situ formation of Fe-N 4 sites on the self-supporting 2D N-doped carbon backbone. Impressively, Fe 1 Zn 30 NC PDI exhibites its superior oxygen reduction reaction (ORR) electro-catalytic activity and peroxidase (POD)-like activity. For ORR in an alkaline medium, it exhibites a much higher onset potential of 0.97 V and half-wave potential of 0.89 V than 20 wt% Pt/C catalyst with good durability of 92 % retention rate after 20000 s. And, Fe 1 Zn 30 NC PDI also shows better peak power density (86 mW cm −2 ) compared with 20 wt% Pt/C in Zn-air battery. Benefiting from the specific POD-like activity of Fe-N 4 , the Fe 1 Zn 30 NC PDI also shows excellent and selective performance in colorimetric H 2 O 2 sensing, with the ultrafast response (30 s), a low limit of detection (10 nM), and good robustness. This work sheds light on a promising design concept for synthesizing 2D polymer-derived single-atom multifunctional catalysts.
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Materials Today Chemistry
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2022
·
IF 7.613
Z. Cheng,H. Yang,Y. Xu,J. Jiang,Q. Xu
Fabrication of active and durable non-noble metal heterogeneous electrocatalysts to settle the relatively slow kinetic process and poor stability during the oxygen evolution reaction (OER) process is of great significance. Herein, we fabricate in-situ 2D Fe-based trimetallic complex spinel oxide nanosheets (FeCoNi)O 4 via a polyethylene glycol-barbituric acid deep eutectic solvent-assisted route. Multiple analytical characterizations illustrate a deep understanding of the structure and composition of (FeCoNi)O 4 , disclosing Fe, Co, and Ni ions occupy both tetrahedrally and octahedrally coordinated positions. Meanwhile, the synergistic actions of preparing multiple-cations substitution and constructing oxygen vacancy activate covalent Fe–O–Co bonds in (FeCoNi)O 4 . Due to the active bimetallic Fe–O–Co sites, enhanced electronic conductivity and unique structure stability, the synthesized 2D (FeCoNi)O 4 nanosheets exhibit excellent OER performance with relatively low overpotential (421 mV for 1000 mA/cm 2 ) and long-term stability (720 mA/cm 2 for 6 h) in alkaline media, which is much better than that of Fe-based bi/monometallic spinel oxides. In-situ Raman spectra and quasi-in-situ X-ray photoelectron spectroscopy results depict that O-bridged Fe–O–Co bimetallic sites promote the formation of μ(O–O) intermediates and undergo the direct O 2 evolution route, thus accelerating OER.
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CHEMOSPHERE
·
2022
·
IF 8.943
Lina Qian,Su Yan,Xiaoyu Yong,Manickam Selvaraj,Hamed A. Ghramh,Mohammed A. Assiri,Xueying Zhang,Mukesh Kumar Awasthi,Jun Zhou
Excess sludge produced from biological wastewater treatment plant in petroleum industry is a kind of hazardous solid waste. Converting the sludge into biochar catalysts may help to reduce its environmental risk, recover resources and increase economic efficiency. However, the role of the sludge biochar in persulfate activation remains unclear, limiting its application in removing organic pollutants from water body. In this study, metal-rich petrochemical sludge was used to produce activated sludge biochar (ASC) via a two-step method of pyrolytic carbonization (400 °C–800 °C) and subsequent KOH activation (abbreviated as ASC 400–800). The physio-chemical properties of ASC 400–800 were characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), Scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) and Raman. The chloramphenicol (CAP) removal performances of ASC 400-800/peroxymonosulfate (PMS) systems were evaluated. Results showed that porous sludge biochar was successfully prepared by the two-step method. At 800 °C, the specific surface area of ASC reached the highest value of 202.92 m 2 g −1 . At 600–800 °C, Fe 3 O 4 , Fe 0 , and graphitized carbon were formed in ASC. Among ASC 400–800, ASC 800 exhibited the best CAP removal performance in ASC 800/PMS system by adsorption combined with catalytic degradation. The optimal conditions identified for 0.31 mM CAP removal were ASC 800 2.0 g L −1 , PMS 6.2 mM, and pH 2.0. SO 4 •- , •OH, and 1 O 2 may contribute to CAP degradation. The degradation pathways of CAP were proposed based on the identified degradation intermediates. Overall, this study confirmed that porous biochar derived from petrochemical sludge was an effective adsorbent or PMS catalyst to remove organic pollutants from wastewater.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Ling Wu,Feng Li,Haidong Yu,Luping Shen,Mingxi Wang
Spectrophotometry is an economic and rapid method for detecting oxalic acid (OA), while the reported methods have some drawbacks, such as narrow linear range, long response time, delicate operation and required expensive reagents. Herein, we found that the as-synthesized Fe(III)-sulfosalicylate (FeSSA) could be used as an efficient colorimetric chemosensor to detect OA, and the established FeSSA-based fading spectrophotometry showed prominent advantages over the existing ones in detecting OA. The as-established method has wider linear range of 0.80–160 mg/L with regression coefficient ≥ 0.999, while the widest linear range is just 2.7–54 mg/L among the reported ones. Moreover, the method has low limit of detection (0.74 mg/L), extremely fast response (several seconds), satisfactory selectivity, high accuracy and precision. Most importantly, its reliability was further verified by employing it to determine OA concentration during the degradation process of organic pollutants. The measured OA concentration at any time interval was perfectly consistent with those determined by the well-recognized high performance liquid chromatography (HPLC). These confirmed that the FeSSA-based fading spectrophotometry is an efficient, simple, fast, accurate and economic method to determine OA in a wide concentration range.
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