Sustainability
·
2024
·Vol. 16
·期 7
·3009
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IF 3.3
Jiahui Wang,Zhen Xi,Bo Niu,Ruitong Gao,Zhenming Xu
Deep and efficient debromination is a critical step in achieving environmentally friendly recycling and ensuring the sustainability of waste-printed circuit boards (WPCBs) because of their high toxicity and carcinogenicity. To this end, this study used a copper–iron (Cu/Fe) bimetal as a debromination agent to remove bromides from WPCBs using in situ catalytic pyrolysis technology. The results show that the maximum debromination efficiency was 97.14% under the following conditions: a Cu mole ratio of 0.20 (Cu/Fe-0.20), a Cu/Fe-0.20 dosage of 0.4, a pyrolysis temperature of 600 °C, and a retention time of 10 min. The main bromine species in pyrolysis oil and gas were bromophenol, bromomethane, HBr, and Br2. The conversion of bromine species and the debromination of the Cu/Fe-0.20 bimetal were analyzed in real time using a thermogravimetry-coupled Fourier transform infrared and mass spectrometer (TG-FTIR-MS). Using the Cu/Fe bimetal synergistic effect, we determined that the debromination mechanism could be used for bromide conversion and fixing. The Cu in the Cu/Fe-0.20 transformed the organic Br (bromophenol and bromomethane) into inorganic Br (HBr and Br2) by providing empty orbitals for lone pairs of electrons. Then, the generated HBr and Br2reacted with Fe in the Cu/Fe-0.20 and were fixed in pyrolysis residue. This study provides theoretical support and a practical method for WPCB deep debromination and recycling.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Zhenlei Wang,Yinxing Zhao,Tingting Zhang,Sizhe Lai,Qiwu Zhang,Yunliang Zhao
Arsenic (As) contamination in industrial wastewater on a large scale has posed a enormous threat to ecological security in recent decades. However, a key challenge at present is the efficient and cost-effective removal of As contamination, as Fe in the As removal process cannot quickly and stably form an active phase with high activity for arsenic removal. Here, we propose a strategy to use mechanical activation of dolomite to regulate the formation of newly formed Fe-hydroxide from Fe(II) with high arsenic-removal activity, while stably regulating the pH of water in the near-neutral range, thereby substantially improving the removal efficiency as well as the stability of Fe(II) for As. Activated dolomite can significantly enhance the oxidation rate of Fe(II) in water, and synergistically remove As contamination over 99.5 % of water with an initial concentration of 50 mg/L within 2 h, far superior to the performance of single Fe(II) or dolomite&Fe(II). The simulation and characterisation results reveal that in the presence of activated dolomite, the solution pH as well as the oxidation rate of Fe(II) are effectively regulated, which promotes the As in the solution to be significantly immobilised on the surface of activated dolomite as a ternary precipitate of Ca/Mg-Fe-As, conducive to the stability of the enhanced As removal precipitation. This study provides new insights into the role of carbonate mineral materials in As transformation, which is important for the efficient and cost-effective purification of As contamination in water.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Meirong Dong,Junchang Xiong,Hongchuan Liu,Zehua Huang,Huaming Hou,Youcai Liang,Jidong Lu
Fe-based oxygen carriers are regarded as a promising class of oxygen carriers in the field of chemical looping combustion. However, the elucidation of the detailed microscopic reaction mechanism of oxygen carriers remains a significant challenge. In this work, we combine in situ spectroscopy, density-functional theory (DFT) calculations, and micro-kinetic modelling to reveal the microscopic reaction mechanism of CH 4 combustion on α-Fe 2 O 3 . The macroscopic reaction characterization of hematite with CH 4 was carried out on a fixed bed, and gas chromatography (GC) was utilized to detect the combustion products (CO 2 , H 2 O and H 2 ). Subsequently, in situ spectroscopy and DFT were combined to reveal the detailed pathways for the CH₄ oxidation process. The results indicated that the reaction intermediates evolve from methoxy (CH 3 O*) to the bridged bidentate formate (b-HCOO*) to the monodentate formate (m-HCOO*), which ultimately leads to the formation of CO 2 through a combination of H transfer and lattice oxygen oxidation. A micro-kinetic model was developed which incorporates surface reaction with the oxygen transport. This revealed that CH 3 O* and CH 3 O* → CH 2 OO* are the key intermediates and radical reactions, respectively, for CO 2 production. The elucidation of the reaction mechanism may prove beneficial for the future development of novel Fe-based oxygen carriers.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Qian Cheng,Xiaohan Liu,Chuhan Huang,Hongman Sun,Fazle Subhan,Xinyi Zhou,Yuankai Liu,JiaHui Yang,Qi Li,Youhe Wang,Zifeng Yan
Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C 3 N 4 heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a "triple win scenario" strategy to fabricate the S-scheme MIL-101(Fe)/g-C 3 N 4 heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E g ) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C 3 N 4 heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C 3 N 4 to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e - ) on the g-C 3 N 4 CB with a more negative reduction potential and the holes ( h + ) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N 2 to NH 3 . The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g cat -1 h -1 , representing an 8-fold and 2.8-fold improvement over pristine g-C 3 N 4 (20 µmol g cat -1 h -1 ) and MIL-101(Fe) (57 µmol g cat -1 h -1 ), respectively.
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WATER RESEARCH
·
2025
·
IF 12.4
Yang Wang,Ziyuan Huang,Zhang Yan,Zhenchao Lei,Huanxin Ma,Chunhua Feng
Acid mine drainage (AMD) is characterized by high concentrations of Fe(II) and Fe(III), which can be harnessed for the in-situ formation of schwertmannite, enabling the efficient immobilization of toxic heavy metals. However, existing biological and chemical methods for schwertmannite synthesis face significant challenges, including low Fe(II) oxidation rates and particularly limited Fe(III) precipitation efficiency in acidic environments. In this study, we develop a visible light-assisted photo-electrochemical (PEC) system that effectively overcomes these barriers. By leveraging anodically evolved O 2 and cathodically generated OH − , we achieved facile Fe(II) oxidation at pH 3.0, and an impressive Fe(III) precipitation efficiency of 82.8 %, significantly exceeding the < 30 % efficiency reported by other methods. Mössbauer spectroscopy and X-ray diffraction confirmed that the generated minerals are high-purity schwertmannite. Experimental and theoretical analyses revealed that in the presence of cathodic alkalinity, Fe(III) undergoes further hydrolysis to form [(H₂O) 3 Fe(OH) 2 (SO 4 )] − species, which are thermodynamically capable of spontaneous polymerization and mineralization. Furthermore, the photoreduction of [(H₂O) 4 Fe(SO 4 ) 2 ] − within the PEC system, followed by subsequent oxidation, plays a crucial role in facilitating Fe(III) mineralization. The PEC system also effectively transformed As(III) to As(V) and Cr(VI) to Cr(III) in AMD, promoting their immobilization in the resultant schwertmannite.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Baixin Liu,Xuelian Chen,Guojuan Hai,Wenwen Zhao,Kai Li,Zhicong Yuan,Xiaoyong Zhang
The design and synthesis of metal–organic frameworks (MOFs) for direct use as electrode materials are crucial for enhancing the electrocatalytic oxygen evolution reaction (OER). Herein, the ultrathin MIL-53(Fe) nanosheet arrays with enriched coordinatively unsaturated metal sites (denoted as MIL-53(Fe)/NF-B0.2-2) are obtained under the inhibition and modulation of benzoic acid (BA) ligands via a substitution-suppression process. The results confirm that this unique ultrathin structure effectively increases the electrochemical active surface areas (ECSA) and exposes the coordinatively unsaturated metal sites. More importantly, the enriched coordinatively unsaturated metal sites acting as active sites facilitate the adsorption of OH– during the OER process. Additionally, MIL-53(Fe)/NF-B0.2-2, with its optimized energy band structure, exhibits superior charge transfer ability and diffusion processes, significantly improving the reaction kinetics in alkaline electrolytes. As a result, the MIL-53(Fe)/NF-B0.2-2 electrode only requires extremely low overpotentials of 190 and 229 mV to reach current densities of 10 and 100 mA cm–2 for OER, respectively. This research not only proposes a novel strategy for designing efficient electrocatalysts but also provides insights into the structure–activity relationship, advancing the rational design of MOFs as effective electrode materials.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xueai Li,Kexin Jin,Xiangyan Qu,Yuning Shi,Chunsheng Wang,Wanchun Guo,Kesong Tian,Yahui Wang,Haiyan Wang
The dispersion of diverse magnetic metallic in a single particle plays an important role in microwave absorption; however, its contribution is not clear due to the challenge of controllable synthesis of magnetic bimetallic nanoparticles in one micro/nanostructure. Herein, a series of magnetic bimetallic nanoparticles separately confined growth in a hollow multi-shell microsphere with proper impedance matching characteristic were prepared, which can be used as theoretical models to elucidate magnetic coupling effect between diverse magnetic metallic nanoparticles in a single particle on electromagnetic attenuation. The coupling effect of magnetic Co and Fe nanoparticles dispersed in different shell effectively enhance the microwave absorption performance of void@Fe@SiO 2 /Co/C particles with minimum reflection loss (RL min ) of −62.3 dB (RL=-20 dB, 99 % absorption) at a thickness of 2.05 mm, provoking the maximum radar cross-section (RCS) reduction value of perfect electric conductor (PEC) 37.37 dBm 2 . Meanwhile, broad effective bandwidth (EBW, RL≤-10 dB, ≥90 % absorption) response of 7.04 GHz at a thickness of 2.44 mm was achieved. These findings can provide guidance for the designation of novel magnetic broadband microwave absorbing materials (MAMs).
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Materials Chemistry Frontiers
·
2024
·Vol. 8
·期 14
·2592-2598
·
IF 6
Jinfu Hou,Yongqi Jian,Chengjie Chen,Dengke Zhang,Fangyan Xie,Jian Chen,Yanshuo Jin,Nan Wang,Xiang Yu,Hui Meng
FeNC is a promising non-precious metal catalyst that can replace platinum-based catalysts in proton-exchange membrane fuel cells (PEMFCs) and zinc–air battery applications. The study utilized Fe-ZIF-8 as a precursor to improve the oxygen reduction reaction (ORR) activity of the catalyst. This was achieved by growing ruthenium particles of approximately 0.32 μm in situ using a physical milling method under a reducing gas atmosphere. This paper demonstrates that in situ grown ruthenium nanoparticles can alter the spin state of iron atoms from the high-spin state FeN4(II)-(t42ge2g) to the medium-spin state FeN4(II)-(t52ge1g). This alteration changes the interactions of the π* antibonding orbitals of the oxygen and thus improves the ORR activity. The rotating ring-disk (RDE) electrode test resulted in a half-wave potential of (E1/2) + 0.80 V vs. RHE in 0.1 M HClO4, indicating remarkable ORR performance. Zinc–air battery tests showed a high peak power density of 148 mW cm−2.
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Environmental Technology & Innovation
·
2024
·
IF 6.7
Binbin Wu,Zheng Wang,Yannan Jia,Nannan Xu,Lisha Liao,Chenyue Zhang,Zhiwei Wang,Yuanxiang Shan,Wanting Feng,Hongqin Xue
Biochar loaded with bimetallic Fe/Mo (Fe/Mo-BC) was prepared as a cost-effective catalyst for the degradation of organic matter by activated peroxydisulfate, in which MoO 2 was used as a co-catalyst to enhance Fe 2+ /Fe 3+ cycling. The tetracycline-degradation efficiency of the system reached 74.49 % within 10 min, and it showed high removal rates over a wide pH range (3–9). Quenching experiments and electron paramagnetic resonance analyses showed that 1 O 2 , •OH, O 2 • - , and SO 4 • − produced by the Fe/Mo-BC/PDS system are involved in tetracycline degradation, with 1 O 2 and •OH being the dominant active substances. X-ray photoelectron spectroscopy analysis revealed that Mo(IV) reduces Fe 3+ to Fe 2+ and oxidizes itself to Mo(VI). In addition, the Fe/Mo-BC remained stable and could be recycled three times, indicating the feasibility of this system for practical applications. The possible pathways of TC degradation by this system were investigated by LC-MS and DFT calculations. Thus, the present study provides a feasible strategy for the use of biochar-loaded bimetallic materials and PDS for the degradation of organic matter.
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POLYMER ENGINEERING AND SCIENCE
·
2024
·
IF 3.2
Wenlong Ma,Tianxu Hao,Xinya Wang,Wei Zhang,Yonggui Li,Mingxing Chen
In this paper, a high-performance composite nanofiber membrane with excellent air filtration and dye degradation properties was prepared by incorporating MIL-53(Fe) nanoparticles into the electrospinning solution. The results showed that the filtration efficiency for PM2.5 of the PP/PVDF-HFP/MIL-53(Fe) composite nanofiber membrane reached up to 99.3% with the addition of 2 wt% MIL-53(Fe). Moreover, the composite nanofiber membrane exhibited steady filtration efficiency across different parameters, including air velocity, PM2.5 concentration, and extended testing time. Furthermore, the incorporation of MIL-53(Fe) significantly enhanced the removal efficiency of the composite nanofiber membrane toward Rh B, resulting in a remarkable 91% removal rate. The polymer/MOF composite nanofiber membranes prepared by simple and cheap electrospinning technology have a wide range of practical applications in the field of environmental protection. Highlights PPM composite nanofiber membrane was prepared via electrospinning method. MIL-53(Fe) nanoparticles were introduced to PPM composite nanofiber membrane. PPM composite nanofiber membrane showed excellent removal efficiency for PM2.5. PPM composite nanofiber showed a good removal performance for RhB in solution.
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Chemistry-An Asian Journal
·
2024
·
IF 3.5
Lijuan Ma,Han Wang,Jing Zang,Xinna Wang,Hao Li,Yanwei Li,Yanhui Li
The rational design of efficient, stable, low-cost non-precious metal-based electrocatalysts with enhanced oxygen reduction reaction (ORR) activity has attracted widespread attention. In this study, a novel electrocatalyst, Fe/Co-N-MWCNT, was prepared by in-situ growth of ZIF-8 and Fe/Co-Phen on multi-walled carbon nanotubes (MWCNTs), then pyrolysis under different temperature to obtain optimal one. During the pyrolysis process, the incorporation of Fe and Co facilitated the formation of metal active sites and Fe-Co alloy, thereby promoting electron transfer and enhancing the ORR activity. Compared to Pt/C (E1/2 = 0.854V, JL = 4.90 mA cm-2), Fe/Co-N-MWCNT demonstrated a comparable half-wave potential (E1/2 = 0.812V) and an enhanced limiting current density (JL = 5.37 mA cm-2). Furthermore, Fe/Co-N-MWCNT was stable and showed no significant change after 2000 cycles, with only a negative shift of 7 mV in E1/2. Ampere response testing revealed that the current decay of Fe/Co-N-MWCNT after 10000 s was only about 7.8%, while that of Pt/C was about 18.4%. Due to its excellent catalytic stability, Fe/Co-N-MWCNT was demonstrated to be an excellent candidate for rechargeable zinc-air batteries. The outstanding electrocatalytic performance of Fe/Co-N-MWCNT can be attributed to its high pyridinic nitrogen content, the unique structure and abundant metal active sites.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Anli Liu,Zhixue Zhang,Zhikui Zhou,Chengwan Wang,Yue Yuan,Qinmei Zhong,Sheng-Tao Yang
As commonly observed water pollutants, organophosphates (OPs) can induce eutrophication of water bodies and pose serious risks to the environment and human health. In this study, we investigated the degradation of tetramethylphosphonate (THPS), an OP, using micron-scale iron-copper (Fe/Cu) bimetals activated peracetic acid (PAA) system. Interestingly, the iron groups (i.e., Fe, Fe/Cu and Fe-PAA system) exhibited a biphasic response: an initial rapid response within the first 10 min followed by a slower degradation lasting from 10 to 60 min. However, the copper groups (i.e., Cu, Cu-PAA and Fe/Cu-PAA) exhibited an initial response within the first 10 min coupled with a subsequent plateau with no significant alterations thereafter. In terms of reactive oxidized species (ROS) verification, only hydroxyl radical ( • OH) was detected in the Fe and Fe-PAA systems; only singlet oxygen ( 1 O 2 ) was detected in the Cu system; organic radicals (R-O • ) and 1 O 2 were detected in the Cu-PAA and Fe/Cu-PAA systems respectively; while • OH, R-O • and 1 O 2 were all detected in the Fe/Cu-PAA system. The presence of Cu promoted the release of electrons from iron and strengthened the single-electron transfer mode. Notably, after five consecutive runs, the removal efficiency of THPS remained above 80 %, and the k obs during the first ten minutes (11.28, 10.11, 9.12, 8.29, and 8.45 min −1 ) remained high and stable throughout the cycles. XPS spectra analysis demonstrated that for 5 cycles, the surface content of Fe 0 /Fe 2+ and Cu 0 /Cu + in the utilized materials surpassed that of the pristine Fe/Cu bimetals, indicating the self-renewal of Fe/Cu bimetals. These findings highlight the potential of Fe/Cu bimetals in effectively degrading THPS and reducing its environmental impact.
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