ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Kuang Wang,Zhanqiang Fang
In the homologous series of polybrominated diphenyl ethers (PBDEs), the debromination of low-brominated diphenyl ethers with higher toxicity remains a challenge. Nano zero-valent iron (nZVI) has been extensively studied for the debromination of PBDEs, but its inherent direct electron transfer mechanism is less efficient for low-brominated diphenyl ethers, and there are issues with high preparation costs. In this work, we synthesize Ni-doped oxalated submicron ZVI (Fe OX bm /Ni) using a low-cost ball-milling method. Fe OX bm /Ni exhibits a debromination rate constant of 0.48 day −1 for 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) in tetrahydrofuran (THF)/water. The debromination rate of Fe OX bm /Ni for BDE-47 in water is even faster (0.98 day −1 ), with the yield of the complete debromination product, diphenyl ether, reaching 76.71%. In real groundwater, Fe OX bm /Ni also shows high reactivity toward BDE-47, with a rate constant of 0.33 day −1 . Kinetic experiments, quenching experiments, and degradation pathway indicate that the attack of atomic hydrogen on C-Br bonds is the primary degradation mechanism. Electrochemical analysis further show that Ni 0 sites could cleave hydrogen into absorbed atomic hydrogen (H∗ ABS ) and adsorbed atomic hydrogen (H∗ ADS ), with H∗ ADS playing the main role. These findings contribute valuable insights into advancing the large-scale application of ZVI and offer promising strategies for thorough remediation of PBDEs pollution.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
·
2024
·
IF 4.7
Hui-chuan REN,Xiao-bo MIN,Yong KE,Long-gong XIA,Yun-yan WANG,Cong PENG,Yun LI,Rong-he TAN,Chuan-fu ZHANG
A method to upgrade the iron grade in copper slag was proposed using lime to decompose Al 2 O 3 -containing fayalite melt (AFMT). Thermodynamic calculations indicated that adjusting the CaO/AFMT ratio can yield a residual melt with a FeO concentration of 75-88 wt.% and produce Ca 2 SiO 4 . In-situ observations suggested that the reaction was impeded in some way. Quenching experiments revealed that the initial reaction products consisted of calcium ferrite compounds and FeO-CaO melt. At the FeO-CaO melt/AFMT interface, Ca 2 SiO 4 particles precipitated, forming a dense Ca 2 SiO 4 film that significantly impeded mass transfer. Although trace amounts of Al 2 O 3 in AFMT temporarily enhanced mass transfer, they were insufficient to overcome this retardation effect. The decomposition reaction was far from achieving equilibrium, demonstrating a self-retardation effect. Measures must be implemented to eliminate this self-retardation effect and enhance the efficiency of reaction kinetics.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Tong Hu,Wenjun Zhou,Haijiao Xie
Lattice engineering of Fe 0 based on heteroatom doping holds great promise in water purification owing to their tunable geometric and electronic structure. However, there is limited understanding of how nitrogen atom in Fe 0 lattice structure affects its local microenvironment and corresponding reactivity toward target contaminants. Herein, microscale zero-valent iron with interstitial N doping (N-mZVI) was successfully prepared by a facile mechanochemical method for heavy metal pollution control. N-mZVI exhibited excellent reactivity for Cr(VI) elimination, and both removal efficiency and conversion rate could reach 100 %, which was 8.06 and 2.73 times higher than that of pristine ball milled mZVI, respectively. Besides, the rate constant of various heavy metals sequestration (Cr(VI), Ni(II), Pb(II), Cu(II), and Cd(II)) over N-mZVI was 61.3 ∼ 115.6-fold faster than that of pristine ball milled mZVI. N-mZVI was also demonstrated to be pH-universal, long-term stability, and environmental applicability. Experimental results and theoretical calculations indicated that tensile strain induced by interstitial N doping expanded Fe 0 lattice and weakened the lattice Fe-Fe interaction, thus significantly accelerating electron transport dynamics in Fe 0 core. Meanwhile, iron nitride species on the surface of N-mZVI promoted electron transfer from iron shell layer to heavy metals. This work comprehensively investigates the structure–property relationships of lattice engineering-based N-mZVI, and provides a new insight into rational design of modified mZVI with high reactivity.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yinghao Shi,Dong Wang,Feilong Gao,Linan Liu,Qinglong Liu,Lan Wang,Jingchun Tang
The performance optimization of zero-valent iron (ZVI) based materials for reductive dechlorination remains challenging. After extensive research on sulfidation modification, the doping of heteroatom nitrogen (N) into ZVI for reductive dechlorination of chlorinated hydrocarbons (CHCs) becomes a new promising trend. In this study, surface modification of microscale ZVI (mZVI) was carried out by a facile ball milling method, and Fe–N(C) coated mZVI (abbreviated as N(C)-mZVI bm ) synthesized from different N sources of dimethylimidazole, urea and melamine were characterized. The effects of nitrogen-to-iron ratios (N/Fe), ball milling time and speed on the reductive dechlorination of trichloroethylene (TCE) were further investigated. A series of characterization and mechanistic analysis showed that the high reactivity of N(C)-mZVI bm with melamine as nitrogen source (abbreviated as N(C)-mZVI bm (M)) was attributed to the properties and thickness of its particle passivation layer, and faster electron transfer from the reduced iron species to the surface layer. In addition, N(C)-mZVI bm (M) exhibited great performance for dechlorination at a wide pH range of 3 to 11, due to alleviated passivation of the Fe 0 core under alkaline conditions by Fe–N(C). This study presents new ideas and evidences for the environmentally friendly synthesis of N-modified ZVI materials and their practical application in groundwater remediation.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2024
·
IF 9.7
Jianyong Che,Wenjuan Zhang,Shuyue Feng,Yian Zuo,Chengyan Wang
Mechanochemistry has rapidly advanced as an effective method for recovering metals from hazardous wastes due to its mild reaction conditions, while understanding the underlying mechanisms remains a significant challenge. This work investigates the mechanochemical reduction of lead compounds using iron powder at room temperature , focusing on physicochemical properties and electrochemical performance. Notable transformations were observed in the crystal structures, morphologies, and thermal stability of PbSO 4 and PbCl 2 . Electrochemical tests indicated enhanced redox reactivity, decreased reduction potential, and reduced charge transfer impedance after mechanochemical treatment . Additionally, the reduction of PbSO 4 proved more challenging than PbCl 2 under the same conditions. Our findings provide valuable insights into the management of toxic lead waste and improve the understanding of the mechanochemical effects on redox reactions , with important implications for environmental applications.
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2024
·
IF 9
Yuting He,Jun Li,Liang Zhang,Xun Zhu,Qian Fu,Yuan Pang,Qiang Liao
To address the urgent need for developing carbon-neutral technologies, microbial electrosynthesis (MES), as an important contributor to the renewable energy field, can convert carbon dioxide to multi-carbon chemicals using microbes serving as living catalysts at the cathode. However, the performance of the cathode is restricted by the weak electrochemical reaction kinetics of the organisms, the specific area of the electrode, and the mass transfer under high current. Herein, we report a facile 3D-printed graphene aerogel (GA) electrode built with a nanozero-valent iron (NZVI)-functionalized graphene ink. The 3D-printed GA electrode was designed to possess hierarchical pores with an enhanced high specific surface area for microbial colonization while ensuring mass transfer. NZVI can assist in-situ hydrogen generation, facilitating biofilm formation and methane (CH 4 ) production in the indirect electron transfer pathway. Consequently, the optimized 3D-printed electrode achieved a maximum CH 4 production rate of 6993 ± 832 mmol/m 2 /d with a faradaic efficiency of 83.7%, which increased by 3.24-fold to the carbon felt electrode. In addition, integrating the proposed cathode into a PV-electrolyzer cell yielded a solar-to-CH 4 efficiency of 4.70%. This study provides a unique method for the development of advanced cathodes and underscores the potential of integrating MES with renewable energy technologies.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zimo Lou,Ludi Song,Xuanlong Zhang,Xiaofei Wen,Dong Cheng,Jianming Yu,Xinhua Xu
Exogenous ferrous ion dosing allows depassivation of aged zerovalent iron (ZVI) for industrial wastewater treatment, while sustaining the persistent existence of Fe(II) species for continuous depassivation throughout decontamination remains challenging. To tackle this dilemma, pre-oxidized microscale ZVI (poZVI bm ) is proposed via ball milling with peroxydisulfate (PDS) solids, for tailoring an “continuous self-driven depassivation” scenario with Fe 0 /Fe(II) symbiosis. The poZVI bm exhibits a 4.4 ∼ 19.0 times higher equilibrated adsorption capacity for hexavalent chromium (Cr(VI)) than the referenced ball milled ZVI (ZVI bm ) and other benchmarked mZVI composites (e.g. oxalated ZVI bm , sulfidized ZVI bm , and nanoscale ZVI), following a chemisorption-reduction process. It also demonstrates a 4.5 ∼ 18.7 folds faster surface area-normalized removal rate for nitrobenzene (NB) than all these counterparts, mediated by reductive transformation. Cr(VI) removal and NB reduction depend on the dissolved and surface-sorbed Fe(II), respectively, which can be optimized by regulating pre-oxidation degree of poZVI bm . The “continuous self-driven depassivation” of poZVI bm starts with the local microenvironment acidification due to the adsorption of abundant dissolvable Fe(II) over surface-located Fe(III), which drives continuous dissolution of Fe 0 core to create more reactive Fe(II), and therefore repeats the above procedure. Owing to wide pH adaptability (pH 3 ∼ 9) and impressive corrosion behavior of poZVI bm , these findings inspire the intimate integration of Fe 0 /Fe(II) component for high-efficient remediation of multicomponent industrial wastewater.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Bo Guo,Yue Chen,Haishuang Xing,Yushi Yang
Green Fe-Ce nanoparticles (GFC-NPs) synthesized in-situ by adding grape-seed extracts and Fe 2+ /Ce 3+ solution synchronously, were combined with H 2 O 2 for simultaneous enhancing sludge dewatering and phosphorus (P) recovery. GFC-NPs/H 2 O 2 (Fe/Ce molar ratio of 4:1) was demonstrated as a novel and efficient pretreatment even at pH 6.8 (without adjustment), where the values of specific resistance to filtration, Time to filtration and water content of mud cake were respectively decreased by 74.9 %, 47.0 % and 12.8 % under the optimal conditions of 30 mg (Fe+Ce) /g·TSS (total solid sludge), 100 mg H 2 O 2 /g·TSS, and reaction time 30 min. Meanwhile, excellent performances were also exhibited with above 95.9 % of P recovery in all investigated GFC-NPs/H 2 O 2 process. Compared with Fe 0 /H 2 O 2 or GF-NPs/H 2 O 2 , better performances were presented on both sludge dewaterability and P recovery after GFC-NPs/H 2 O 2 pretreatment. The Fe-Ce bimetallic catalysis significantly facilitated ·OH production (0.92 times higher than that of Fe 0 /H 2 O 2 ) and P could be recovered in the sludge simultaneously. Under GFC-NPs/H 2 O 2 oxidation, the larger reduction of PN and PS was examined in the LB-EPS and TB-EPS, as well as sludge particle size and the absolute value of zeta potential. Further analysis verified that GFC-NPs/H 2 O 2 oxidation could induce the looser conformation of protein secondary structure and cause the more release of bound water. In summary, GFC-NPs/H 2 O 2 is an eco-friendly and practical technology for enhancing sludge dewaterability and P recovery simultaneously.
✓ 已验证
产品关联
DOI
高影响因子
Matter
·
2025
·
IF 17.5
Shining Wu,Yuting Zhang,Guanwu Li,Yifeng Hou,Mengyang Cao,Chengyu Wei,Pengkun Yang,Lu Huang,Yingpeng Wu
High-entropy alloys (HEAs) have a wide range of applications due to their excellent physical and chemical properties. However, traditional synthesis routes always require high temperatures over 923 K or have high equipment requirements. Here, we developed a liquid metal gallium (Ga)-mediated strategy using only a commercial vortex mixer and metal powders to synthesize HEAs near room temperature (303 K) with low power (7 W). A variety of HEAs were successfully prepared, and the yield can be expanded to over 10 g each time. The mechanistic investigation proved that Ga continued to flow under the mechanical force and exposed fresh surfaces to contact the metal, thereby promoting the process of metal dissolution in Ga and forming HEAs. These as-prepared HEAs can be used for catalysis in electrochemical oxygen evolution reactions with low overpotential and high durability. This strategy provides an innovative method for low-energy synthesis of HEAs at room temperature.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Haiquan Zhang,Fuge Wang,Susu He,Bozhou Cao,Qiadong Yao,Ning Wang
Smart phase change materials (PCMs) have been carefully engineered using cutting-edge manufacturing techniques to meet specific application requirements. A multifunctional phase change composite has been developed by combining polyethylene glycol (PEG2000) binary eutectic, sodium stearate (NaR) micro−/nano-medium, and iron powder as raw materials. The binary eutectic PCM provides the composite with plasticity at room temperature. The addition of an appropriate amount of sodium stearate enhances the dispersibility of high-density iron powder (7.86 g cm −3 ) within the PCM, without altering the intrinsic morphology of the binary eutectic (1.27 g cm −3 ) before or after melting. As a result, the functional composite exhibits several attractive properties, including morphology switchability under external forces, temperature, and magnetic fields, asymmetric transmission of electrical signals in temperature gradients, efficient photo-thermal conversion, and excellent thermal storage performance. This self-prepared functional composite holds great potential for applications in drug delivery, morphology control in confined spaces, temperature management in building materials and electronic components, as well as electrical signal transmission across varying temperatures.
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Kai He,Yuanfang Lai,Shuchen Wang,Li Gong,Feng He
Metal doping for improving the reactivity of zerovalent iron (ZVI) has been well studied, while Mn(II)-modified microscale ZVI (Mn-mZVI) has not yet been explored. Herein, ball-milled Mn-mZVI was fabricated and used for Cr(VI) removal. Characterization analysis showed that the structure, composition, and charge of mZVI changed after the Mn(II) modification. The comparative test showed that Mn-mZVI could remove 100% of Cr(VI) within 10 min, whereas mZVI removed negligible Cr(VI) within 60 min. The zeta-potential and electrochemical evidence verified that the enhanced electrostatic attraction and electron-transfer ability contributed to the superior Cr(VI) removal performance of Mn-mZVI. Moreover, the solution pH increase caused the decline of Cr(VI) removal, and the presence of NO3– inhibited Cr(VI) removal, whereas other coexisting ions showed little influence on the Cr(VI) removal performance of Mn-mZVI. Chemical and material characterization analyses revealed that Cr(VI) reduction by Mn-mZVI was the combined action of Fe(0) and generated Fe(II). In addition, the reusability of Mn-mZVI was not ideal due to the surface passivation and loss of Mn(II), but the reactivity could be reactivated by ball-milling the reacted Mn-mZVI again with Mn(II). Overall, this work provides a new mentality for mZVI modification and is important to develop promising mZVI-based materials for Cr(VI) pollution control.
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Water
·
2024
·
IF 4.8
Zhi Ye,Yunpeng Liu,Jiang Xu,Nan Xu,Juncai Dong,Haijun Chen,Dongrui Li,Lei Peng,Yuxi Gao,Jiating Zhao
The efficiency and stability of in situ remediation of Cr(VI) contamination in underground water and soil are still challenging. In this study, a green tea (GT) synthesized nano-zerovalent iron (nZVI) nanocomposite supported by diatomite (DE) (nZVI@GT/DE) via tea polyphenols was designed. The synergetic effect of DE support and tea polyphenols wrapping increased the Fe(II) component in nZVI@GT/DE and its transportability. Compared to nZVI@GT/Mont (supported by Mont with sandwich structure), nZVI@GT/DE exhibited a notably higher capacity (>100 mg g–1) for immobilizing Cr(VI) and a more pronounced ability to release iron ions in solution (corrosion parameter: K ≈ 1.046). This was attributed to the combined effect of the unwrapping process of tea polyphenols coverage and the distinctive columnar porous structure of DE, which increased the exposure of α-Fe0 core for enhanced Cr(VI) reduction during their cotransport in the water-saturated soil system. X-ray absorption fine structure and X-ray photoelectron spectroscopy analyses confirmed that nZVI@GT/DE released more Fe(II) ions to reduce Cr(VI) to bidentate binuclear Cr(OH)3 (vs FeOCr2O3) complexes. This study unraveled the molecular mechanism and highlighted the Cr speciation transformation and physiochemical property changes of nZVI@GT/DE during their cotransporting when applied in situ remediation in complex subsurface of Cr(VI)-contaminated groundwater and soil system.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）