Nano Energy
·
2023
·
IF 17.6
Rui Ma,Xun Cui,Xiaoxue Xu,Yonglin Wang,Gaoqiang Xiang,Likun Gao,Zhiqun Lin,Yingkui Yang
The rational design and facile synthesis of cost-effective and high-performance carbon-based catalysts for oxygen reduction reaction (ORR) is of great significance but remain challenging. Herein, we report the crafting of a robust Fe,N,P-codoped, ultrafine Fe 2 P nanocrystals decorated, highly hierarchical porous carbon nanoshells (denoted Fe,N,P-CNSs/Fe 2 P) via a simple yet robust one-step synergetic phosphorization and pyrolysis approach for highly-efficient ORR. Specifically, well-defined polypyrrole- co -polyaniline hollow nanospheres with a shell thickness of ≈ 43 nm (PPy- co -PANI-HNs) are first elaborately synthesized via a facile soft-templating (Triton X-100 micelles) copolymerization of pyrrole and aniline monomers . Subsequent one-step synergetic phosphorization and pyrolysis of PPy- co -PANI-HNs pre-impregnated with NaH 2 PO 2 ·H 2 O and FeCl 3 (H 2 PO 2 - ,Fe 3+ @PPy- co -PANI-HNs) yields Fe,N,P-CNSs/Fe 2 P with a well-crafted ultrathin nanoshell (shell thickness of ≈13 nm) architecture containing abundant hierarchical porosity . Remarkably, an alkaline electrolyte capitalizing on the resulting Fe,N,P-CNSs/Fe 2 P manifests excellent ORR performance with the half-wave and onset potentials ( E 1/2 of 0.854 V and E onset of 0.955 V) comparable to Pt/C, diffusion limited current density ( J L of −5.98 mA cm −2 ) higher than Pt/C, and long-time durability and methanol resistance better than Pt/C, demonstrating great potential as air cathode in zinc-air batteries (maximum power density of 170 mW cm −2 and specific capacity of 824.5 mA h g −1 ). Combined experimental and theoretical studies reveal that the impressive ORR performance of Fe,N,P-CNSs/Fe 2 P originates from simultaneous compositional (i.e., Fe,N,P-codoping and ultrafine Fe 2 P nanocrystals decorating) and structural (i.e., hierarchically porous ultrathin nanoshell architecture) tailoring enabled by the judicious one-step synergetic phosphorization and pyrolysis.
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高影响因子
PHYSICA STATUS SOLIDI A-APPLICATIONS AND MATERIALS SCIENCE
·
2022
·Vol. 220
·期 2
·2200581
·
IF 2.17
Linlin Dang,Kai Zhang,Qiguan Wang,Changhua Xu,Sumin Wang
Active bifunctional electrocatalysts for both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are badly required for high-efficiency zinc–air batteries (ZABs). Herein, a Fe-alloyed MoNi nanohybrid (MoNiFe) as bifunctional catalyst is reported. The alloyed MoNiFe architecture with the decreased size compared with MoNi is obtained by a hydrothermal reduction method, which enhances the exposed active sites and promotes the charge transfer. Accordingly, MoNiFe exhibits good bifunctionality, with a positive half-wave potential (0.896 V) near Pt/C (0.812 V) in ORR reaction and a low overpotential (0.295 V) similar to IrO 2 (0.29 V) in OER process. The as-derived rechargeable ZAB cells based on the bifunctional MoNiFe catalyst show the peak power density of 58 mW cm −2 with a high open-circuit voltage of 1.319 V. Thus, this work paves a new alloying avenue for synthesizing effective bifunctional electocatalysts for ZABs.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Luwei Wang,Chenliu Tang,Pengfei Huang,Xiang Hu,Zhirong Sun
The widespread detection and potential adverse effects of antibiotics in the aquatic environment call for effective treatment technology. Electro-Fenton is a promising strategy, but the preparation of efficient and stable cathodes is still challenging. In this study, a novel metal-organic framework (MOF)-derived N-doped cathode Fe/Cu-C400Ar was synthesized successfully for the degradation of ceftazidime (CAZ) in heterogeneous electro-Fenton (hetero-EF) system. The doping of copper could enhance electrocatalysis with a high electrochemical surface active area and low resistance. Fe/Cu-C400Ar cathode achieved CAZ removal efficiency of 99.5 ± 0.4% within 120 min, and it exhibited excellent stability after six recycle runs. Quenching experiments and electron paramagnetic resonance (EPR) tests proved that the primary species was hydroxyl radical during the CAZ degradation. In addition, the degradation pathway of CAZ was proposed including the cleavage of the pyridine ring and the shedding of the thiazole ring. Moreover, the prediction of intermediates toxicity by Ecological Structure Activity Relationships (ECOSAR) software indicated the environmentally friendly features of the CAZ degradation process. This study provided a promising cathode for the electrocatalytic degradation of antibiotic wastewater in hetero-EF system.
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ACS ES&T Engineering
·
2023
·
IF 7.1
Junna Yan,Mengyu Ma,Keyi Liu,Yang Bao,Feihu Li
Efficient removal and recovery of phosphorus (P) from wastewater is critical for addressing both phosphate rock depletion and eutrophication-related deterioration of surface water quality. Herein, we present a promising platform approach integrating cerium-doped NH2-MIL-101(Fe) with melamine sponge (MS) scaffolds for rapid and high-efficiency recovery of P from wastewater. The as-prepared MIL-101@sponge composites (denoted as MIL-101@CS, MIL-101@PVDF, and MIL-101@SDBS, respectively) are featured by flexibility and stability according to many characterization techniques. Batch adsorption of P over these composite adsorbents indicates that these MIL-101@sponge composites exhibit a maximum adsorption capacity (e.g., 253.66 mg g–1 for MIL-101@CS) at the optimum pH of 6.0 and that adsorption equilibrium can be attained within 150 min and well described by the pseudo-second-order kinetic model. In addition, these composites show a high selectivity for P over carbonate and other common monovalent anions under environmentally relevant conditions. The results of desorption and recycling tests indicate that MIL-101@CS retains good adsorption and desorption efficiency even in a much short operating time (i.e., 5 min), which allows such a composite to be applied in enriching and recovering P efficiently from wastewater via a rapid adsorption/desorption operation. Moreover, the high feasibility of MIL-101@CS in actual scenarios was validated by efficiently enriching the P from a sludge dewatering liquid. Furthermore, the main mechanisms for P adsorption are elucidated from various microstructural characterizations. Overall, this work presents a strategy of integrating MIL-101 with sponge scaffolds for rapidly and efficiently recovering P from wastewater, which may be potentially extended to the recovery of other value-added elements of interest from waste streams.
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FOOD CHEMISTRY
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2022
·
IF 9.231
Hui Shu,Tingrun Lai,Zhichao Yang,Xuechun Xiao,Xiumin Chen,Yude Wang
High sensitivity and ultra-trace detection of imidacloprid are important and challenging in the field of food. In this study, we prepared a Fe-rich FeCoNi-MOF in-situ modified nickel foam working electrode by one-step hydrothermal method, and achieved a highly sensitive detection of the imidacloprid. The characterization techniques confirmed that Fe-rich FeCoNi-MOF had excellent crystallinity, tighter structure, and exposed rich active sites. The detection results showed that Fe-rich FeCoNi-MOF electrochemical sensor had a minimum detection limit of 0.04 pmol/L (100 times lower than that of the bioelectrochemical sensors), a wide response range (1 pmol/L–120 μmol/L), and high sensitivity (124 μA pmol/L -1 cm −2 ). These advantages of the electrochemical sensor were revealed theoretically by the valence change of active metal and the first principle calculation. Lastly, the Fe-rich FeCoNi-MOF electrochemical sensor was applied to detect imidacloprid in apple, fresh tea leaves, tomato, cucumber, and had an excellent recovery of 98–102.8 %.
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PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
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
·
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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高影响因子
Catalysts
·
2022
·Vol. 12
·期 11
·1363
·
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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Chemosensors
·
2023
·Vol. 11
·期 2
·114
·
IF 4.2
Hao Liu,Qing Zhang,Ning Bao,Shou-Nian Ding
As the most widely used disposable paper-based diagnostic tool in the world, immunochromatographic test strips (ICTS) have occupied more and more positions in the field of rapid diagnosis due to their ease of operation and affordability. Therefore, the development of an easily prepared, sensitive, and accurate signal reporter is of great significance for the detection of some low-abundance biomarkers in clinical diagnosis. Herein, Mg/Fe layered double hydroxide nanoflowers (MF NFs) were selected as adsorption templates and sulfhydryl-functionalized, followed by one-step loading of hydrophobic CdSe/ZnS quantum dots in the organic phase via a metal-thiol covalent bond. After coating the reporter with branched polyethyleneimine (PEI), a novel ICTS fluorescent reporter was prepared. The modification of PEI not only improved the hydrophilicity of MF@CdSe/ZnS NFs but also introduced amino functional groups on the surface of the reporter for subsequent conjugation with antibodies. X-ray photoelectron spectroscopy, UV-vis absorption, X-ray diffraction, fluorescence spectroscopy, and infrared spectroscopy were used to characterize the composition of MF@CdSe/ZnS NFs. Under the optimal experimental conditions, the detection range of MF@CdSe/ZnS@PEI-ICTS for the model analyte HCG was 0.1–500 mIU/mL, and the limit of detection (LOD) reached was 0.1 mIU/mL. The potential for practical application was validated by the detection of HCG in spiked healthy human serum, showing overall recoveries between 90.48 and 116.1% with coefficients of variation that ranged from 3.66 to 12.91%.
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Journal of Superconductivity and Novel Magnetism
·
2023
·Vol. 36
·期 2
·733-743
·
IF 1.8
Wu Fangyi,Liu Zhonghao,Dong Yaqiang,Zhang Ruiheng,He Aina,Ling Yufan,Li Jiawei,Liu Xincai
Reducing the low-frequency loss (≤ 1 kHz) of the soft magnetic powder cores (SMPCs) while maintaining high saturation magnetic induction ( B s ) is beneficial to the high efficiency and energy saving of motor applications. Herein, the effects of silicone resin content (SI), compaction pressure, and annealing temperature on the magnetic softness, microstructure, and magnetic domains of Fe-6.5 wt.%Si SMPCs were systematically studied. The SMPCs with 1 wt.% SI content and pressed at 1800 MPa not only have good forming ability but also exhibit low total loss and high B s . According to the loss separation at 1 T and 1 kHz, the hysteresis loss accounts for more than 75% of the total loss. Annealing at 850 °C induces dense and large recrystallized grains with large-angle grain boundaries and easily mobile domain walls, resulting in low hysteresis and total loss. A higher temperature of 950 °C damages the cladding layer and causes direct powder-to-powder contact, which thus slightly increases hysteresis and eddy loss. The correlation between the core loss, microstructure, and magnetic domain provides a reference for the development of high- B s and low-loss SMPCs for high-efficiency motors.
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高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Liping Tan,Yamei Sun,Changjun Yang,Bingguang Zhang,Kejian Deng,Xiaofeng Cao,Yanchuan Guo
Photocatalytic selective oxidation of glycerol to value-added C 3 products is a promising strategy for the valorization of glycerol. In this work, an inorganic/organic composite material by integrating zinc oxide (ZnO) with iron thioporphyrazine (FePz) was prepared to act as photocatalyst for photocatalytic oxidation of glycerol in water. The effects of FePz surface modification on the physicochemical properties and photocatalytic performance of ZnO were systemically studied. More importantly, the integration of ZnO with FePz could markedly improve the visible light absorption ability and effectively promote the separation of photogenerated charges. Meanwhile, introducing FePz onto the ZnO surface was beneficial to the adsorption capacity of glycerol. Just because of this, ZnO/FePz composite exhibited excellent photocatalytic activity for oxidizing glycerol in water, C 3 products including glyceraldehyde and dihydroxyacetone were obtained from this composite photocatalytic system. Additionally, the active species responsible for glycerol oxidation were also determined.
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