JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2021
·Vol. 168
·期 5
·056523
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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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Nature Communications
·
2021
·Vol. 12
·期 1
·1-10
·
IF 14.919
Liu Gongquan,Zhao Yi-Lei,He Fangyuan,Zhang Peng,Ouyang Xingyu,Tang Hongzhi,Xu Ping
Biodegradation of aromatic and heterocyclic compounds requires an oxidative ring cleavage enzymatic step. Extensive biochemical research has yielded mechanistic insights about catabolism of aromatic substrates; yet much less is known about the reaction mechanisms underlying the cleavage of heterocyclic compounds such as pyridine-ring-containing ones like 2,5-hydroxy-pyridine (DHP). 2,5-Dihydroxypyridine dioxygenase (NicX) from Pseudomonas putida KT2440 uses a mononuclear nonheme Fe(II) to catalyze the oxidative pyridine ring cleavage reaction by transforming DHP into N -formylmaleamic acid (NFM). Herein, we report a crystal structure for the resting form of NicX, as well as a complex structure wherein DHP and NFM are trapped in different subunits. The resting state structure displays an octahedral coordination for Fe(II) with two histidine residues (His 265 and His 318 ), a serine residue (Ser 302 ), a carboxylate ligand (Asp 320 ), and two water molecules. DHP does not bind as a ligand to Fe(II), yet its interactions with Leu 104 and His 105 function to guide and stabilize the substrate to the appropriate position to initiate the reaction. Additionally, combined structural and computational analyses lend support to an apical dioxygen catalytic mechanism. Our study thus deepens understanding of non-heme Fe(II) dioxygenases.
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Nano-Micro Letters
·
2020
·Vol. 12
·期 1
·1-12
·
IF 12.264
Xu Weiqing,Kang Yikun,Jiao Lei,Wu Yu,Yan Hongye,Li Jinli,Gu Wenling,Song Weiyu,Zhu Chengzhou
The two functional groups (nitro and amino) were introduced into MIL-101(Fe) for tuning the atomically dispersed metal active sites.
Benefiting from both geometric and electronic effects, the nitro-functionalized MIL-101(Fe) shows a superior electronic structure of active sites and low reaction energy barrier for the HO* formation.
Nitro-functionalized MIL-101(Fe)-based biosensor was successfully employed to detect acetylcholinesterase activity and organophosphorus pesticide.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 28
·期 4
·4136-4146
·
IF 3.056
Sun Runze,Wang Jie,Peng Yutao,Wang Hongmei,Chen Qing
Arsenic (As) contamination of aquatic and soil environments is a global concern, highlighting the importance of As removal via high-efficiency and low-cost removal technologies. In the present study, novel trimetallic biochar was developed through pyrolyzing corn straw impregnated with inexpensive metal Fe/Al/Zn (hydr)oxides. The results of SEM, FTIR, and XRD verified the formation of metal oxyhydroxides on the surface of the modified biochars, and the modification increased the specific surface area (SSA), total pore volume (TPV), and surface charge of the Fe/Al/Zn (hydr)oxides modified biochar (FAZ-CB). Compared with the original biochar, higher sorption rates and capacities was observed for the FAZ-CB. The maximum As (V) adsorption capacities of FAZ-CB reached 82.9 mg g −1 . A pot experiment showed that application of FAZ-CB decreased bioavailable As fractions in the red soil significantly reduced the uptake of As by arugula in edible part and root (42.6 and 56.8%, respectively). The present study demonstrated the superiority of FAZ-CB in the As(V) immobilization in red soil, suggesting that it is a promising candidate for practical application for As immobilization. Therefore, FAZ-CB can be used as a promising functionalized biochar to remediate As contaminated red soil.
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CHEMOSPHERE
·
2021
·
IF 7.086
Liu-Xi Yang,Jia-Cheng E. Yang,Ming-Lai Fu
In this study, porous magnetic CoFe 2 O 4 nanocrystals (NCs) were successfully synthesized by using bimetal-organic framework (MOF) as a precursor, and used as catalysts to activate peroxymonosulfate (PMS) for the removal of chloramphenicol (CAP) in the solution. The structure and physicochemical properties of CoFe 2 O 4 NCs were thoroughly examined by a series of characterization techniques. The results revealed as-synthesized CoFe 2 O 4 had a nanorod-shaped structure with high specific surface area (83.00 m 2 g −1 ) and pore volume (0.31 cm 3 g −1 ). Furthermore, the degradation efficiency (100%) and the removal of total organic carbon (68.09%) were achieved after 120 min with 0.1 g/L CoFe 2 O 4 NCs, 2 mM PMS and 10 mg/L CAP at pH of 8.20. In addition, effects of catalyst dosage, PMS dosage, initial pH values, CAP concentration and co-existing anions as well as natural organic matters in the solution on the degradation efficiencies were studied and all the removal can be well fitted with pseudo-first-order kinetic model (R 2 > 0.96). Sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO•) were proved to be two main reactive species for CAP removal in CoFe 2 O 4 /PMS system based on quenching experiments. CAP was degraded by the main pathways of dichlorination, denitration, decarboxylation , hydroxylation, ring cleavage and chain cleavage on CoFe 2 O 4 /PMS system through high performance liquid chromatograph-mass spectrometry analysis. We believe that this study would be very meaningful to promote the applications of MOFs-derived catalysts on the SO 4 •− based advanced oxidation processes (SR-AOPs) for the environmental remediation.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Cheng Liu,Lei Jin,Jia-Qiang Yang,Fang-Zu Yang,Zhong-Qun Tian
In this paper, the effects of complexing agents (oxalic acid and glycine) and Fe(II) ions on the electro-reduction of Cr(III) ions are studied carefully. Based on the electrochemical analyses, both the complexing agents and Fe(II) ions can obviously decrease the cathodic polarization in the electro-reduction of Cr(III) ions, and the Fe(II) ions can also be co-deposited with Cr(III) ions. One water molecule in [Cr(III)(H 2 O) 6 ] 3+ ion is substituted by one oxalic acid or glycine to form an electrochemically active penta-aqua-Cr(III) coordination ion. In situ infrared spectroscopy and energy dispersive spectroscopy reveal the typical induced-deposition mechanism of ferrochrome alloy. Fe(II) ions are firstly reduced to Fe crystal nuclei, then Cr and Fe atoms grow on the Fe nuclei to form ferrochrome alloy.
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JOURNAL OF FLUORINE CHEMISTRY
·
2020
·
IF 2.332
Yongyang Chen,Dan Guo,Xiaochun Dong,Yahui Li,Yixuan Huang,Hao Chen,Shanping Li
Perfluorooctanoic acid (PFOA), as a refractory organic pollutant, seriously harms the environment and damages human health. Here, the electrocatalytic method was selected to degrade PFOA. In this work, perovskite catalysts doped with different elements, and corresponding gas diffusion electrodes (GDE) were prepared by the gel-sol method and citric acid complexation method. The crystal structure, microscopic morphology, and electrochemical properties of the LaNi x Y 1-x O 3 (Y = Fe, Cu, Co, Sr) perovskite catalyst electrode were analyzed by XRD, TEM, and CV. Moreover, the electrocatalytic performances of the as-prepared electrodes were assessed by the degradation of PFOA, and the Sr-doped GDE exhibited the highest degradation rate of PFOA. The optimum degradation conditions, such as the current density, pH, and initial concentration were also investigated. It was observed that when the current density was 20 mA/cm 2 , pH was 5, and initial concentration was 0.25 mmol/L, the Sr-doped GDE had the best degradation and defluorination efficiency of PFOA reached 90.0 % and 75.1 %, respectively. High performance liquid chromatography-mass spectrometry (HPLC-MS) was used to analyze the intermediate products of PFOA degradation and obtain the degradation pathway. With the combined action of OH and O 2 , PFOA was degraded by stepwise removal of CF 2 groups, which were ultimately degraded into F − and CO 2 .
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
·
IF 3.99
De-Yu Gao,Zan Liu,Zhi-Lin Cheng
The crucial challenge of 2D inorganic nanomaterials-filled composite hydrogel with outstanding mechanical properties was concentrated on the surface modification that was capable to access a better interface between 2D inorganic nanomaterials and hydrogel in past. In this paper, for the first time, we extensively studied the application of as-synthesized 2D Ni-Fe MOF nanosheets with natural organic interface and interlayer structure in PVA hydrogel. The morphology and structure of the as-prepared 2D Ni-Fe MOF/PVA composite hydrogels were determined by a series of characterizations. The results indicated that the as-prepared 2D Ni-Fe MOF/PVA composite hydrogel with porous structure exhibited a desirable dispersion due to the existence of the potential interfacial interaction. Furthermore, the swelling, mechanical and tribological properties of the composite hydrogel were intensively investigated. Dramatically, the tensile strength and compression modulus of the as-prepared 2D Ni-Fe MOF/PVA with 0.1 wt.% filling content were increased by 62.5 % and 113 % relative to pure PVA hydrogel, respectively. Owing to the presence of the interlayer structure of 2D Ni-Fe MOF nanosheets, the friction coefficient of the 2D Ni-Fe/PVA composite hydrogel with 0.15 wt.% filling content was reduced by 41 % compared to pure PVA hydrogel.
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Acta Biomaterialia
·
2020
·
IF 7.242
Jin He,Ju Fang,Pengbo Wei,Yulei Li,Hui Guo,Qingsong Mei,Fuzeng Ren
Three-dimensional (3D) porous zinc (Zn) with a moderate degradation rate is a promising candidate for biodegradable bone scaffolds. However, fabrication of such scaffolds with adequate mechanical properties remains a challenge. Moreover, the composition, crystallography and microstructure of the in vivo degradation products formed at or near the implant-bone interface are still not precisely known. Here, we have fabricated porous [email protected] scaffolds with skeletons consisting of an inner core layer of Fe and an outer shell layer of Zn using template-assisted electrodeposition technique, and systematically evaluated their porous structure, mechanical properties, degradation mechanism, antibacterial ability and in vitro and in vivo biocompatibility. In situ site-specific focused ion beam micromilling and transmission electron microscopy were used to identify the in vivo degradation products at the nanometer scale. The 3D porous [email protected] scaffolds show similar structure and comparable mechanical properties to human cancellous bone. The degradation rates can be adjusted by varying the layer thickness of Zn and Fe. The antibacterial rates reach over 95% against S. aureus and almost 100% against E. coli . A threshold of released Zn ion concentration (~ 0.3 mM) was found to determine the in vitro biocompatibility. Intense new bone formation and ingrowth were observed despite with a slight inflammatory response. The in vivo degradation products were identified to be equiaxed nanocrystalline zinc oxide with dispersed zinc carbonate. This study not only demonstrates the feasibility of porous [email protected] for biodegradable bone implants, but also provides significant insight into the degradation mechanism of porous Zn in physiological environment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Sijin Zuo,Xuming Jin,Xinwei Wang,Yunhao Lu,Qi Zhu,Jiangwei Wang,Weiping Liu,Yonghua Du,Juan Wang
ABSTRACT Atomically dispersed heterogeneous metal catalysts are promising in dealing with the ever-growing environment and energy issues. However, the practical uses of such catalysts are challenged by the concerns of low reliability and reusability of current compositions under changeable conditions. Here we demonstrate a strategy to stabilize the atomically dispersed Fe catalysts through anchoring the Fe atoms in between a C 3 N 4 -rGO double-layered support. The layered structure is found to significantly prohibit acid leaching and agglomeration of Fe atoms while maintaining activity of the reaction sites, even under extreme pH conditions (pH < 3 or> 11). This allows us to realize high performance Fenton-like reaction via activation of persulfate with unforeseen reactive and recycling abilities over all pH values (0 to 14). This work offers opportunities for understanding the Fenton-like system at extreme reaction conditions, while providing keen insights into the development of stable atomic metal catalysts for practical use.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Song Cheng,Chen Shen,Hao Zheng,Fuqiang Liu,Aimin Li
Preparing heterogeneous electro-Fenton (HEF) catalysts without sacrificing activity towards the two-electron (2e − ) oxygen reduction reaction (ORR) is a challenge, since Fenton-like active sites consist mainly of transition metals that prefer the 4e − ORR pathway. In this study, oxidized carbon nanotubes (OCNTs), which are promising ORR catalysts for the 2e − ORR, were uniformly attached to the surface of Prussian blue analogue (PBA) microcubes, forming a unique chainmail-like catalyst (OCNTs/PBA). 50 mg/L of sulfamethazine (SMZ) was completely removed within 30 min over OCNTs/PBA HEF process, with the first-order kinetic constant increased by 287.2 % compared with that PBA alone. To reveal the mechanism behind the enhanced catalytic activity, several possible interactions between the OCNTs and PBA were proposed and investigated further. This study not only offers a facile method to prepare a chainmail-like HEF catalyst, but also provides valuable insights into the rational design of HEF electrocatalysts with dual Fenton-like and ORR activity.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2020
·
IF 2.726
Guoqiang Li,Feifei Li,Jianxin Liu,Caimei Fan
The nitrogen activation is the Achilles’ heel of photocatalytic nitrogen fixation . Herein, metal-organic frameworks (MOFs), for first time, are proposed to solve the above bottleneck. A series of Fe-Based MOFs (MIL-101(Fe), MIL-100(Fe), MIL-88(Fe)) demonstrated excellent photocatalytic nitrogen fixation activity. To gain insight into the reaction mechanism, MIL-101(Cr) and MIL-101(Fe), with same molecular structure except the central metal ions , selected for system comparison. Photocatalytic nitrogen fixation activity of MIL-101(Fe) and MIL-101(Cr) are 50.355 μmol L −1 h −1 and inactive, respectively. This suggested that the nitrogen fixation activity originated from the Fe catalytic center. The results of in situ FTIR and quantum computation verifies Fe catalytic center have a higher electron density, a lower reaction activation energy and more generation of N–H bond than those of Cr catalytic center. In view of the analogous outer electron configuration of Cr and Fe, it was suspect that two extra d-orbitals electronics of Fe element are the basic reason of the excellent photocatalytic nitrogen fixation activity. This work provides a new application of MOFs in photocatalytic nitrogen fixation field and emphasizes the vital of d-orbitals electronics during the nitrogen activation process.
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