ENVIRONMENTAL POLLUTION
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2023
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IF 8.9
Yurong Gao,Hanbo Chen,Zheng Fang,Nabeel Khan Niazi,Kwasi Adusei-Fosu,Jianhong Li,Xing Yang,Zhongzhen Liu,Nanthi S. Bolan,Bin Gao,Deyi Hou,Chenghua Sun,Jun Meng,Wenfu Chen,Bert F. Quin,Hailong Wang
Sorption and oxidation are two potential pathways for the decontamination of trivalent antimony (Sb(III))-bearing water, using iron (Fe)-modified biochar (FeBC). Here we investigated the sorption and oxidation behavior of FeBC for Sb(III) in aqueous solutions. Results revealed that Sb(III) removal by FeBC was significantly improved showing the maximum Sb(III) sorption (64.0 mg g −1 ). Density functional theory (DFT) calculations indicated that magnetite (Fe 3 O 4 ) in FeBC offered a sorption energy of −0.22 eV, which is 5 times that of non-modified biochar. With the addition of peroxymonosulfate (PMS), the sorption of Sb(III) on FeBC was 7 times higher than that on BC, indicating the sorption capacity of FeBC for Sb(III) could be substantially increased by adding oxidizing agents . Electrochemical analysis showed that Fe modification imparted FeBC higher electron-donating capacity than that of BC (0.045 v. s. 0.023 mmol e − (g biochar) −1 ), which might be the reason for the strong Sb(III) oxidation (63.6%) on the surface of FeBC. This study provides new information that is key for the development of effective biochar-based composite materials for the removal of Sb(III) from drinking water and wastewater. The findings from this study have important implications for protecting human health and agriculture.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Meiling Chen,Lin Ding,Shijun Zhu,Xiuqin Xiong,Xinkai Yuan,Yanhua Peng,Liming Yang,Hui Shi,Penghui Shao,Xubiao Luo
The slow Fe(II)/Fe(III) cycle during the Fenton reaction process strongly impedes oxidation efficiency in practical applications. In this study, an activated carbon (AC) assisted Fenton reaction system was used to treat electroplating wastewater containing Ni-ethylenediaminetetraacetic acid (Ni-EDTA). AC was found to enhance the removal of Ni-EDTA in Fenton/Fenton-like reactions. The reported results revealed that AC could effectively promote the regeneration of Fe(II) from Fe(III) species via electron transfer to improve the reaction rather than directly enhancing the H 2 O 2 decomposition to accelerate the production of hydroxyl radicals (•OH). Quenching experiments and EPR also demonstrated that •OH and •O 2 − took part in the radical oxidation process, in which the contribution of •OH was dominant. XPS and FT-IR analysis further confirmed that the carbonyl group (C O) on the surface of AC could indeed act as the dominant active site and an electron donor to directly reduce Fe(III). In addition, electrochemical tests indicated that AC could increase the oxidation potential of Fe(III) to boost the reaction between Fe(III) and H 2 O 2 , thus enabling the transfer of electrons from H 2 O 2 to Fe(III) to facilitate the Fe(II)/Fe(III) cycle. This study might contribute to a new insight into the mechanisms of AC-catalyzed Fenton oxidation processes for the decomplexation heavy metal-EDTA.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Xinqiang Liu,Haoran Yin,Shifan Zhang,Menghan Huang,Tayirjan Taylor Isimjan,Xiulin Yang,Dandan Cai
Strategically tuning the composition and structure of transition metal phosphates (TMPs) holds immense promise in the development of efficient oxygen evolution reaction (OER) electrocatalysts. However, the effect of crystalline phase transformation for TMPs on the catalytic OER activity remains relatively uncharted. In this study, we have deftly orchestrated the reaction process of anion-etched precursor to induce the amorphization process of FeCo-PO x from crystalline to amorphous states. The as-obtained amorphous FeCo-PO x (A-FeCo-PO x ) exhibited an optimized OER performance with a low overpotential of 270 mV at a current density of 10 mA cm −2 , which could be attributed to the flexibility of its amorphous structure and the synergistic effect of oxygen vacancies . Moreover, when incorporated into an overall water splitting (OWS) device configured as A-FeCo-POx (+) ||Pt/C (–) , it displayed long-term solid stability, sustaining operation for 300 h at a current density of 200 mA cm −2 . This work not only provides valuable insights into understanding the transformation from crystalline to amorphous states, but also establishes the groundwork for the practical utilization of amorphous nanomaterials in the field of water splitting.
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Foods
·
2023
·Vol. 12
·期 14
·2794
·
IF 5.2
Shushan Gao,Chonghao Zhu,Liangfei Ma,Chenghai Liu,Hongqiong Zhang,Shengming Zhang
To reduce the usage of petroleum-based plastic products, a lignin-based film material named aminated lignin/Fe(III)/PVA was developed. The mixture of 8 g lignin, 12 mL diethylenetriamine, 200 mL NaOH solution (0.4 mol·L−1), and 8 mL formaldehyde was heated at 85 °C for 4 h; after the aminated lignin was impregnated in the Fe(NO3)3solution, a mixture of 3 g aminated lignin/Fe(III), 7 g PVA, and 200 mL NaOH solution (pH 8) was heated at 85 °C for 60 min; after 2 mL of glycerin was added, the mixture was spread on a glass plate to obtain the aminated lignin/Fe(III)/PVA film. This film demonstrated hydrophobicity, an UV-blocking function, and a good slow-release performance. Due to the formation of hydrogen bonds between the hydroxyl groups of lignin and PVA, the tensile strength, the elongation at break, and the fracture resistance of the film were 9.1%, 107.8%, and 21.9% higher than that of pure PVA film, respectively. The iron content of aminated lignin/Fe(III)/PVA was 1.06 wt%, which mainly existed in a trivalent form. The aminated lignin/Fe(III)/PVA film has the potential to be used as a food packaging material with anti-ultraviolet light function and can also be developed as other packaging materials, such as seedling bowls, pots for transplanting, and coating films during transport.Keywords:lignin;polyvinyl alcohol;Fe(III);packaging material;slow-release function
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2023
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IF 4.3
Chu Shushu,Xia Mingyuan,Xu Peng,Lin Dalei,Jiang Yuanyuan,Lu Yizhong
Although traditional Fe-based nanozymes have shown great potential, generally only a small proportion of the Fe atoms on the catalyst’s surface are used. Herein, we synthesized single-atom Fe on N-doped graphene nanosheets (Fe-CNG) with high atom utilization efficiency and a unique coordination structure. Active oxygen species including superoxide radicals (O 2 •− ) and singlet oxygen ( 1 O 2 ) were efficiently generated from the interaction of the Fe-CNG with dissolved oxygen in acidic conditions. The Fe-CNG nanozymes were found to display enhanced oxidase-like and laccase-like activity, with V max of 2.07 × 10 −7 M∙S −1 and 4.54 × 10 −8 M∙S −1 and K m of 0.324 mM and 0.082 mM, respectively, which is mainly due to Fe active centers coordinating with O and N atoms simultaneously. The oxidase-like performance of the Fe-CNG can be effectively inhibited by ascorbic acid (AA) or hydroquinone (HQ), which can directly obstruct the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB). Therefore, a direct and sensitive colorimetric method for the detection of AA and HQ activity was established, which exhibited good linear detection and limit of detection (LOD) of 0.048 μM and 0.025 μM, respectively. Moreover, a colorimetric method based on the Fe-CNG catalyst was fabricated for detecting the concentration of AA in vitamin C. Therefore, this work offers a new method for preparing a single-atom catalyst (SAC) nanozyme and a promising strategy for detecting AA and HQ.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Na Yang,Wei Yang,Xiaodong Yang,Xiaoming Xiao,Longfei Zhang,Luhong Zhang
Morphological design and interfacial engineering are pivotal strategies for advancing electrocatalysis , however, achieving the optimization of both simultaneously remains a major challenge. To address this, we designed a multi-heterostructured bifunctional electrocatalyst cobalt-nickel-iron-phosphorus-sulfur composite (CoNiFe-PS) with a two-dimensional/three-dimensional (2D/3D) hierarchical structure, which was synthesized through simultaneous phosphating and sulfuration based on cobalt-nickel layered double hydroxide (CoNi-LDH) nanosheets grafted with Prussian blue analogue (PBA) nanocubes. Notably, due to the distinctive morphology and synergistic effect between multi-heterostructure, the CoNiFe-PS catalyst demonstrated excellent performance in terms of ultralow overpotentials of 196 and 263 mV for oxygen evolution reaction (OER), as well as 63 and 235 mV for hydrogen evolution reaction (HER) at current densities of 10 and 100 mA cm −2 . Moreover, the CoNiFe-PS|| CoNiFe-PS cell was constructed for overall water splitting in alkaline condition and exhibited minimal voltage requirements of 1.479 and 1.693 V to achieve 10 and 100 mA cm −2 , respectively. This study provides a new perspective on fabricating multi-heterostructured bifunctional catalysts with unique morphology for highly efficient overall water splitting.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 38
·13047-13055
·
IF 6.4
Xuemei Zhou,Lingmin Kong,Junkai Hao,Jing Feng,Shuo Sun,Chuanzhen Zhou,Yanmin Liu,Zhengquan Yan,Xiao Zhu,Lei Hu
To strengthen the enzyme-mimetic catalytic activity of the classical transition metal oxide of copper and iron, bimetal Cu–Fe oxide mesoporous nanoparticles (Cu–Fe MNPs) were prepared in one pot under microwave-assisted conditions. The proposed Cu–Fe MNPs possessed a well-distributed mesoporous structure with an average aperture of 3.91 nm and a high BET specific surface area of 197.93 m2 g−1. Their peroxidase-like kinetic parameters (Km/Vmax) toward catalyzing the redox reactions of TMB and H2O2 were 0.013 mM/3.01 × 10−8 M s−1 and 56.58 mM/4.12 × 10−8, respectively. In particular, both toxic o-aminophenol (o-AP) and bioactive glutathione (GSH) could deteriorate their peroxidase-like property with an obvious color change from blue to colorless in the proposed Cu–Fe MNPs-TMB-H2O2 system. Under optimized conditions, Cu–Fe MNPs-TMB-H2O2 showed selective response to o-AP and GSH with quite low detection limits of 1.57 × 10−8 mol L−1 (S/N = 3) and 3.35 × 10−8 mol L−1 (S/N = 3), respectively. When they were applied for the visual monitoring of o-AP and GSH in real aqueous, fruit juice and medicinal samples, the detection recovery (%) was between 96.8–101.4% for o-AP and 97.1–105.8% for GSH. The mechanisms of the synergetic enhancement of the peroxidase-like activity of Cu–Fe MNPs and the selective recognition of o-AP and GSH were investigated in detail.
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FUEL
·
2023
·
IF 7.4
Yanjie Niu,Jie Xu,Liqing Chen,Sixi Guo,Fanhui Guo,Yixin Zhang,Jianjun Wu
As a typical coal-based solid waste, coal gasification fine slag (GFS) will have an annual discharge of more than 50 million tons in 2025 in China alone. However, the difficulty of its resource utilization lies in the precise separation of carbon and ash due to their complex distribution pattern. There is an urgent need to develop GFS-based materials for comprehensive utilization of carbon and ash. In this study, a combined process of acid leaching and pyrolysis was designed, in which active metal iron was leached from ash and immobilized on the surface of residual carbon in the form of Fe-N-C. The unique structure of Fe-N doped carbon/ash synergistically improved the efficiency of electrocatalytic degradation of organic wastewater by 72.78 ± 1.37%. The hierarchical porous structure of residual carbon considerably enhanced the accessibility of ash catalytic sites. Abundant ash defects and Fe-N active sites promoted the conversion of free radical precursors to reactive oxygen species (ROS). The removal rate of various organic wastewater within 35 min reached more than 100 ± 1.83% %, with excellent electrocatalytic performance and pH adaptability. Fe-NCPE had a high specific surface area (318.36 m 2 ·g −1 ), orderly graphite phase (002 crystal surface size 1.3 nm), and abundant catalytic sites. We also proposed the catalytic mechanism by combining molecular simulation with experiments. The high adsorption capacity above 24.07 ± 0.12 mg·g −1 ensured the continuous and rapid supply of pollutants and H 2 O 2 near the catalytic site·H 2 O 2 was converted into ROS mainly composed of hydroxyl groups through the valence state change of aluminum or Fenton-like reaction of nitrogen-linked iron. The ROS then attacked organic molecules to degrade pollutants. The above two processes corresponded to two cyclic catalytic reactions. Therefore, this study provides an innovative and promising approach for comprehensive utilization of carbon and ash in GFS.
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CHEMOSPHERE
·
2023
·
IF 8.8
Xue Bai,Xuan Dao,Qin Wang,Jiangna Xing,Ting Wang,Xin Huang,Hongxun Hao
Tetracycline (TC) as a common antibiotic has adverse effects on human healthy and biological survival. In this study, a novel MXene/TiO 2 /Fe hybrid was designed and successfully synthesized by combination method of calcination and hydrothermal reduction. The photocatalysts were characterized by PXRD , SEM , TEM , VSM and XPS, etc. It was found that MXene/TiO 2 /Fe exhibited 2D multilayer structure like MXene. The in-situ synthesized TiO 2 through calcinating MXene exhibited an octahedral biconical structure with exposed (001) and (101) facets. Surface heterojunction of (001) and (101) facets was formed within TiO 2 , which enhanced the separation of photogenerated electrons and holes. The residual MXene could play a role in co-catalyst to capture the photo-generated electrons from TiO 2 . Moreover, Fe nanoparticles not only optimize the band gap structure and increase the specific surface area, but also store the electrons as a good electrons acceptor, which further promote the separation of electrons and holes. The TC removal efficiency of optimal MXene/TiO 2 /Fe could reach 92% within 120 min. Moreover, the influence of external environment factors such as pH, catalyst dosages and common anions were investigated in detail. Mechanism analysis show that h + , •OH and •O 2 − are the main active substances. Finally, the degradation pathways were proposed according to LC-MS.
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Materials Today Communications
·
2023
·
IF 3.8
Jianye Shi,Jin Chen,Xinle Wang,Zhikang Liu,Yuzhao Ma,Xiaofeng Yang,Meidan Que,Yanjun Li
Developing a lightweight microwave absorbing materials with high absorption capacity and wide absorption bandwidth at low thickness is a perennial challenge in practical applications in the microwave absorption (MA) field. Herein, sandwich-like heterogeneous Ti 3 C 2 T x /TiO 2 /Fe 3 O 4 /Fe are designed by synergistically incorporating dielectric-magnetic components with a simple solvothermal method and post-annealing. The sandwich-like heterogeneous interface produces sufficient conduction loss for Ti 3 C 2 T x /TiO 2 /Fe 3 O 4 /Fe, with TiO 2 crystals and amorphous carbon anchored on its surface to enhance interface polarization and Debye relaxation. Additionally, the presence of Fe nanoparticles induces magnetic loss, including natural resonance and eddy current loss. By bidirectionally regulating the ratio of Ti 3 C 2 T x and Fe 3 O 4 , the minimum reflection loss (RL min ) value reaches − 64.6 dB at 17.49 GHz with a 1.48 mm thickness, and the corresponding effective absorption bandwidth (EAB, RL < −10 dB) is 4.59 GHz (13.41–18 GHz). The results suggest that the exceptional EMW absorption performance of composites can be attributed to the dielectric-magnetic synergistic effect and sandwich-like heterostructures . This study offers a rational approach for synthesizing ultrathin and lightweight Ti 3 C 2 T x -based absorbers.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Desen Zhou,Xuan Zhang,Zheng Li,Jun Zhang,Tielin Wang,Shaowen Cao
Photocatalytic conversion of CO 2 to usable fuels provides a new strategy for solving energy problems and the greenhouse effect. Porphyrin-based metal-organic frameworks (MOFs) are promising in photocatalysis due to their remarkable light harvesting ability, and the metal active site and its coordination environment can be further adjusted to achieve the high activity. In this work, g-C 3 N 4 /PCN-222 composites with different porphyrin metal centers were fabricated and the g-C 3 N 4 /PCN-222(Fe III ) catalyst showed the highest photocatalytic CO 2 reduction performance than that of g-C 3 N 4 /PCN-222(Fe II ) and other g-C 3 N 4 /PCN-222( M , M = Co, Ni, Cu, Zn) composites. Experimental studies and theoretical calculations showed that the axial coordination in g-C 3 N 4 /PCN-222(Fe III ) distorts the square planar field (Fe-N4) to quasi-octahedral coordination, which led to the moderate adsorption ability of CO 2 reduction intermediate (*CO), resulting in the high photocatalytic activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yihua Cao,Xueli Yin,Yonghao Gan,Ying Ye,Run Cai,Bo Feng,Qi Wang,Xiaoping Dai,Xin Zhang
Designing bifunctional electrocatalysts with high efficiency and low cost for water splitting is urgently required for the production of green hydrogen. Herein, a bifunctional iron-doped cobalt borate/cobalt phosphide hybrid supported on nickel foam (Fe-CoB i /CoP/NF) was fabricated via hydrothermal and phosphating process. Benefit from the unique nanoneedle architecture for faster mass transfer, the existence of borate on CoB i for accelerating proton transfer , the moderate adsorption of H* species on CoP, Fe doping and the synergistic effect between CoB i and CoP, Fe-CoB i /CoP/NF hybrid exhibits a low overpotential of 137 mV and 260 mV at 100 mA cm −2 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Moreover, Fe-CoB i /CoP/NF||Fe-CoB i /CoP/NF also presents a low cell potential of 1.65 V@100 mA cm −2 for overall alkaline water splitting and excellent durability (128 h) without decay. This work provides a new insight into the design of bifunctional electrocatalysts simultaneously through the morphological engineering and heteroatomic doping.
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