INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Shaokang Su,Wei Zhang,Ying Xie,Lihong Qi,Song Wang,Limin An,Kai Pan
Cobalt phosphide has been widely used in various catalytic reactions due to its excellent catalytic activity and stability. In contrast to the conventional synthesis of Co2P nanorods using expensive and toxic trioctylphosphine (TOP), this study employs a dual-ligand strategy to prepare iron-atom-doped monodisperse Co2P nanorods. The strategy involves the use of triphenylphosphite (TPOP) as a cost-effective and relatively less toxic strong ligand, alongside hexadecylamine (HDA) as a weaker ligand. The resultant atom-doped Co2P nanorods exhibited a large aspect ratio, providing a plentiful supply of active sites for electrocatalytic hydrogen evolution. In both alkaline and acidic electrolytes, achieving a current density of 10 mA cm–2 required overpotentials of 91 and 141 mV, respectively, with the optimal Co:Fe molar ratio of 1:0.2. The introduction of Fe atoms through doping increased the electron density at the Co atom sites, thereby enhancing H adsorption. This research offers a cost-effective and relatively low-toxicity method for the controlled fabrication of monodisperse transition-metal phosphide nanorods, enabling efficient catalytic reactions.
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高影响因子
WATER RESEARCH
·
2022
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IF 13.4
Dongbo Wang,Chuli Pan,Lisha Chen,Dandan He,Longhu Yuan,Yifu Li,Yanxin Wu
The treatment and disposal of sludge is a complex environmental problem because of the high moisture content. Herein, We reported the process of Fe(II) activating Urea hydrogen peroxide (UHP) to improve waste activated sludge (WAS) dewaterability for the first time. Fe(II)/UHP was proven to significantly improve WAS dewaterability. Specifically, under the optimal conditions with 60/35-Fe(II)/UHP mg/g TSS, the CST, SRF, and WC SC of WAS reduced from 215.3 ± 7.5s, 9.2 ± 0.32 (× 10 12 m/kg), and 92.2 ± 0.7% (control) to 62.3 ± 4.3s, 2.8 ± 0.09 (× 10 12 m/kg), and 70.4 ± 0.4%, respectively. Further analysis revealed that •OH was generated in the Fe(II)/UHP system and played the dominant role in enhancing WAS dewaterability. •OH was found to attack extracellular polymeric substances (EPSs) and cells, causing EPSs fragmentation and decomposition part of EPSs into micro-molecule organics or even inorganics, and leading to cell destruction, thus liberating the EPSs-bound and cells-bound water. •OH also degraded the protein in centrifugal liquor (CL) into micro-molecule organics such as amino acids, which could reduce the viscosity and electronegativity of CL. The above facts ultimately reduced solid-liquid interface interaction but increased hydrophobicity , flocculation , and flowability of WAS. Meanwhile, the broken WAS flocs were then re-flocculated via adsorption bridging and charge neutralization induced by Fe(II) and Fe(III). Moreover, Fe(II)/UHP treatment achieved the reduction and stabilization of heavy metals of dewatered sludge, which further enabled its land application. Finally, the Fe(II)/UHP process was found to be more attractive than the Fe(II)/persulfate, classical Fenton processes, and cPAM in terms of cost savings and practical implementation.
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 39
·期 12
·3305-3314
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IF 3.146
Liu Zhihao,Qiu Kui,Dong Yu,Jin Zhaobo,Liu Luwei,Wu Jirong
A non-aqueous phase (Sb/Fe/NMP) desulfurization system for the removal of hydrogen sulfide from natural gas was constructed by introducing SbCl 3 and FeCl 3 in a specific ratio into N-methylpyrrolidone (NMP). The desulfurizing agent and its sulfur product were characterized, and the absorption pattern of H 2 S by the system was investigated by static desulfurization experiments. The results indicate that the desulfurizer’s sulfur capacity can reach 16 g/L at room temperature and pressure, and that adding the optimum amount of water and appropriate temperature increase can assist to increase desulfurization efficiency. The system maintained a sulfur capacity level of more than 90% of the initial sulfur capacity after five consecutive desulfurization-regeneration cycles. XRD and XPS spectrogram revealed that the regenerated solid product was high purity sulfur. Sb 3+ is a key component to ensure the effective absorption of H 2 S. The presence of a moderate amount of Fe 3+ can oxidize and absorb small amounts of H 2 S and promote the oxidative regeneration of the system. In addition, we combined the obtained experimental data with density flooding theory (DFT) theoretical calculations to show that the effective coordination of Sb(III) with HS − in the NMP environment is the main reason for the effective absorption of H 2 S by the desulfurizer. NMP is not involved in the coordination absorption process of hydrogen sulfide.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
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IF 7.926
Miao Jiang,Kun Wang,Ruiyuan Xue,Qingliang Zhao,Long Wang,Weiye Wang,Jing Ding
Antimony (Sb) finds its wide application in industries, however, the research on Sb solidification/stabilization (S/S) in the Sb-contaminated soil is currently insufficient, particularly in seasonal freezing regions. Here six composite materials of Fe/Fe 2+ -fly ash-concrete additive (Fe-FA-CA) were employed and optimized to remediate the Sb-contaminated soil subject to 40 freezing-thawing (F-T) cycles. After remediation, FeSO 4 -fly ash-calcium lignosulfonate (FFC) exhibited the best resistance performance to F-T. The stabilization efficiency was evaluated with TCLP at 92.92%. Meanwhile, Sb concentration met the criteria of landfill for inert waste assessed with the compliance test for leaching (CT) of European Standard . The S/S efficiency of Sb dropped slightly from 92.68% to 88.22% (TCLP) and from 97.18% to 93.37% (CT), respectively, after aging 40 F-T cycles. The fraction of residual Sb in the soil treated by FFC was increased by 10.41%, and the strength of the S/S soil was much higher than 350 kPa, the requirement of landfills in the U.S. during F-T cycles. Additionally, the poorly crystalline Fe in the soil remediated by FFC was increased by 4.54 g/kg, suppressing Sb migration. The feasibility and effectiveness of FFC in S/S of Sb demonstrated its potential to remediate Sb-contaminated soil in seasonal freezing regions.
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MATERIALS RESEARCH BULLETIN
·
2022
·
IF 5.6
Qianyu Wei,Qiuhu Lin,Zezhen Zhang,Lili Wu,Chaocan Zhang
Polyvinylidene fluoride (PVDF)/polyhexamethylene guanidine (PHMG)/tannic acid (TA) coatings have some degree of hydrophilicity but lack stability. To improve the hydrophilicity and stability of antimicrobial PVDF/PHMG/TA membranes, Fe(III) is introduced into the composite system. As a weakly acidic hydrophilic nanoion, Fe(III) can enhance the hydrophilicity and resistance to contamination of the membranes. Furthermore, the stability can be enhanced because a three-dimensional cross-linked coating structure is formed by the complexation of Fe(III), TA and PHMG. This work investigates the effects of different tannic acid concentrations and pH conditions on the hydrophilicity, anti-pollution and stability of the modified coatings. The surface morphology of the membranes was analyzed by field-emission scanning electron microscopy. Additionally, the hydrophilicity and the antipollution performance were evaluated based on the water contact angle, submerged oil contact angle, emulsion flux and flux recovery rate. The stability was evaluated by the changes in flux recovery rate and water contact angle before and after emulsion scouring and ultrasonic treatment. The results show that the modified membranes have favorable hydrophilicity and stability after the addition of Fe(III). The water contact angle can be reduced to 19°, the pure water flux can reach 13,850 L·m −2 ·h −1 , and the emulsion flux can reach 2650 L·m −2 ·h −1 . Moreover, 99.68% flux recovery was achieved after 7 days of deionized water flushing, and the water contact angle remained almost unchanged.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 39
·18744-18750
·
IF 3.925
Dawang Chu,Hui Zhou,Zhicheng Luo
Selective conversion of glycerol to lactic acid requires the synergistic activation of C–H, C–O, and O–H. Herein, we report an inexpensive Fe–Cr/TiO2 catalyst that achieves lactic acid formation with a high selectivity of 60.5%. By changing the Fe/Cr ratios and reduction temperatures, the structures of Vő and Vő-OH were altered, which determined the overall oxidation–dehydration–isomerization process. The in situ ATR-IR experiments confirmed the activation of glycerol by adsorbing the primary −OH, and a series of control experiments verified that Fe was responsible for the cleavage of C–H and O–H, while CrOx catalyzed the activation of C–O and C–H. This work designs a hydrothermal catalyst with multifunctional ability, which may guide the rational catalyst design for the selective oxidation of glycerol to lactic acid.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Hao Liu,Chao Huang,Ping Wang,Su Huang,Xiong Yang,Haiyin Xu,Jian Zhu,Dingxun Ling,Chonglin Feng,Zhiming Liu
A novel 3D α-FeOOH@MoS 2 /rGO nanocomposite was successfully fabricated by a simple in situ hydrothermal method. It is a highly efficient heterogeneous catalyst in activation of peroxymonosulfate (PMS) for rapid degradation of rhodamine B (RhB), with 99.9% of RhB removed within 20 min. The introduction of rGO contributes to uniform dispersion and sufficient contact of α-FeOOH and MoS 2 nanosheets. Highly active Mo(IV) enhances the reduction of Fe(III), improves Fe(III)/Fe(II) conversion and promotes the generation of O 2 1 , which ensures an improved catalytic activity . MoS 2 /rGO hybrid can effectively solve the problem of material reunion and make α-FeOOH exhibit excellent catalytic performance. The α-FeOOH@MoS 2 -rGO/PMS system is a co-catalytic system based on the active components of α-FeOOH and MoS 2 . The main reactive oxygen species in the α-FeOOH@MoS 2 -rGO/PMS system are O 2 1 , S O 4 . − and ⋅ O 2 − , which contribute to a high reactivity over a wide range of pH (5–9). Besides, this system is highly resistant to anions ( C l − , S O 4 2 − ) and natural organic matter (humic acid), and can be widely used for degradation of common organic pollutants. The α-FeOOH@MoS 2 /rGO is a promising Fenton-like catalyst for refractory organic wastewater treatment .
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 9
·097501
·
IF 4.386
Dongmei Ren,Xingwen Wang,Chunpeng Leng,Wei Meng,Jingrui Zhang,Chao Han
4-Nitrophenol (4-NP) is a typical organic pollutant, thus it is urgent to detect it in environmental samples. This study rationally designed a novel electrode material of P-doping Fe/Fe3O4@C (P-Fe/Fe3O4@C) prepared with MIL-88 as precursor. P2h-Fe/Fe3O4@C-700 was synthesized by calcining MIL-88 at 700 °C, followed by annealing process with NaH2PO2 for 2 h. The P2h-Fe/Fe3O4@C-700 modified glassy carbon electrode (P2h-Fe/Fe3O4@C-700/GCE) showed a high electrocatalytic activity toward 4-NP reduction due to its active metal center, fine-tuned electronic structure by P-doping, as well as good electrical conductivity. It exhibited excellent sensing behaviors in 4-NP detection with rather high sensitivities of 1415.43 μA·mM−1·cm−2 and 424.63 μA·mM−1·cm−2 in the 4-NP concentration of 5 to 100 μM and 100 to 1200 μM, respectively, with a low detection limit of 0.462 μM. The P2h-Fe/Fe3O4@C-700/GCE still had good selectivity for 4-NP detection in the presence of common interferences. In addition, it was found that the current response towards 4-NP at P2h-Fe/Fe3O4@C-700/GCE retained more than 97% of its initial value after one week, indicating a good long-term stability. Furthermore, the P2h-Fe/Fe3O4@C-700/GCE exhibited a good reproducibility. The constructed P2h-Fe/Fe3O4@C-700/GCE achieved practical uses for the sensing of 4-NP in tap water with satisfactory recoveries.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xinfa Cai,Fei Ma,Jun Jiang,Xianglong Yang,Zhaowei Zhang,Zelang Jian,Meijuan Liang,Peiwu Li,Li Yu
Sensitive, on-site and multiple detection of mycotoxins is a vital early-warning tool to minimize food losses and protect human health and the environment. Although paper-based lateral flow immunoassay (LFIA) has been extensively applied in mycotoxins monitoring, low-cost, portable, ultrasensitive and quantitative detection is still a formidable challenge. Herein, a series of Fe-N-C single-atom nanozymes (SAzymes) were synthesized and systematic characterized. The optimal Fe-N-C SAzyme with highly efficient catalytic performance was successfully used as both label and catalyst in lateral flow immunoassays for mycotoxin detection. By taking advantage of the catalytic amplified system, the qualitative and quantitative detection can be easily and flexibly done via observing the test lines by naked eyes or a smartphone, with the limit of detections (LODs) of 2.8 and 13.9 pg mL −1 for AFB 1 and FB 1 , which were respectively over 700- and 71,000-fold lower than the maximum limit set by the European Union. Besides, underlying catalytic mechanisms and the active sites of the Fe-N-C SAzyme are also investigated by DFT simulation. This work not only provides a promising detection strategy for the application of advanced SAzymes but also offers experimental and theoretical guidelines to understand the active centers of Fe-N-C SAzymes and the catalytic process.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 4.446
Xu Pan,Wenjing Wang,Ye Chen,Qing Wen,Xiaoqian Li,Cunguo Lin,Junhong Wang,Haitao Xu,Liuqingying Yang
As a promising green and storage/conversion technology, the microbial fuel cell (MFC) was generally restricted by the lower power density in application. Three carbonized derivatives of the same precursor metal organic framework (MOF) MIL-53(Fe) were prepared via carbonization at 385 ℃, 600 ℃ and 750 ℃ in argon atmosphere. Experiments showed that carbonized MIL-53(Fe) (CM53) derivative at 750 ℃ produced Fe 3 O 4 /Fe@C structure and revealed the best performance as bioanode in MFC. As anticipated, the MFC with CM53–750/Ti anode demonstrated superb maximum power density of 1179.08 mW/m 2 , which was 88.04% and 36.24% higher than that of MFC with CM53–385/Ti and CM53–600/Ti anode. Moreover, the charge transfer resistance of CM53–750/Ti (0.23 Ω) bioanode in MFC was 90.49% and 87.29% lower than that of CM53–385/Ti (2.42 Ω) and CM53–600/Ti (1.81 Ω) in MFC. The BCA method and high-throughput sequencing proved that CM53–750/Ti bioanode exhibited good biocompatibility and the function of screening the dominant bacteria for electricity generation. The results were mainly attributed to the synergistic effect of derived carbon, iron and Fe 3 O 4 nanoparticles (NPs). Fe 3 O 4 NPs and porous rod-like carbon promoted the enrichment and cultivation of microorganisms on the anode surface, while Fe NPs provided an efficient path for the transmission of extracellular electrons. This article proved that the carbonized derivatives of MOF have application potential in MFC.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Lu Zhang,Jianhao Qiu,Guanglu Xia,Dingliang Dai,Xiang Zhong,Jianfeng Yao
Photocatalytic oxidation of aromatic alcohol into aromatic aldehyde using O 2 has received huge attention, while the reaction that occurred in ambient air is rarely studied but follows the green-chemistry principles. Herein, spindle-shaped MIL-53(Fe)-NH 2 @ZnIn 2 S 4 photocatalysts with a Z-scheme heterostructure were facilely developed for photocatalytic oxidation of aromatic alcohol in air under visible light. The benzyl alcohol conversion can be notably enhanced to 73% over the optimal MIL-53-NH 2 @ZnIn 2 S 4 sample with a benzaldehyde production rate of 1825 μmol g –1 h –1 . However, in the O 2 atmosphere, the benzyl alcohol conversion is only 56%, indicating that O 2 is not required and has an adverse effect on the reaction. The hierarchical structure and Z-scheme heterojunction of MIL-53-NH 2 @ZnIn 2 S 4 impart an efficient separation and strong redox abilities of photo-induced electrons and holes, which are responsible for the impressive photocatalytic performance. This study could motivate the ingenious design of Z-scheme heterostructures for green organic conversion based on MOFs.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yin Li,Jiahui Hu,Yubin Zou,Lin Lin,Hebin Liang,Huaxin Lei,Bing Li,Xiao-yan Li
High-valent iron–oxo species (Fe V =O) generated through peroxide activation by Fe-based catalysts can realize the selective and efficient degradation of organic pollutants in water treatment. However, the rapid and efficient generation of Fe V =O for the selective degradation of pollutants over a wide pH range with high stability is challenging. In this study, a N, P, and S co-doped Fe-single atom (SA) catalyst (Fe SA -NPS@C) with FeN 4 active center was synthesized as a highly efficient catalyst for the peroxymonosulfate (PMS)-based oxidation. The Fe SA -NPS@C catalyst exhibited an excellent catalytic performance at low dosages of both the catalyst and PMS for the degradation of pollutants over a wide pH range with high stability. For the degradation of ofloxacin (OFX), the rate constant pertaining to PMS with Fe SA -NPS@C was 1.68 min −1 , considerably higher than those obtained using the N -doped and N and P co-doped Fe-SA catalysts. The degradation pathway of OFX revealed that the electrostatic effect was of significance in its degradation by Fe V N 4 =O with Fe V N 4 =O being the dominant reactive species. Density functional theory calculations revealed that the heteroatom doping effectively altered the electronic structure of the FeN 4 site of Fe SA -NPS@C, which strengthen its coordination with PMS, promote the electron transfer to PMS, and facilitate the interaction between Fe V N 4 = O and OFX, and thus significantly enhanced its catalytic activity. These findings provide new insights into the oxidation mechanism of Fe V =O in heterogeneous systems and the catalytic ability enhancement through heteroatom doping.
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