APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Yi Tian,Ping Yang,Xiao Zhang
The development of self-colorimetric probes for Fe 3+ detection without external reference remains a significant challenge, despite its critical importance in environmental monitoring and disease diagnosis. In this paper, bright red-emitting carbon dots (r-CDs) with photoluminescence (PL) quantum yield of 35.8 % were synthesized via a one-step solvothermal strategy. The abundant surface hydroxyl/carboxyl groups of r-CDs enabled specific Fe 3+ ion coordination resulted in a novel PL phenomenon, in which the red emitting (650 nm) of the r-CDs changed into green-emitting (500 nm) because of new fluorescent centers formation. pH stability test confirmed the robustness of r-CDs forFe 3+ sensing in a pH region of 2–13.This phenomenon is ascribed to a dual-mode self-colorimetric sensing platform, achieving a detection limit of 10.7 nM and a wide linear range of 0–700 μM in solution. Experimental result confirmed that Fe 3+ coordination triggered electron transfer and lead to new emitting center generation. This bright green emitting was also observed once r-CDs were added a SiO 2 gel with Fe ions, suggesting a significant application in solid-state moist environmental. This novel PL phenomenon is crucial for the preparation and application of CDs.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Chiyu Wen,Chao Wang,Defang Liu,Zhuo Cheng,Jing Zhao,Hongli Zhang,Jun Wang,Guoxiang Zhu,Yongfa Zhu
Nitro-aromatic compounds constitute predominant explosive materials extensively utilized in military applications and industrial blasting operations. However, the manufacturing, consumption, and decommissioning of these explosives generate significant quantities of wastewater exhibiting both ecotoxicological hazards and explosive potential. Herein, an amino-functionalized MIL-100(Fe) (AFM) catalyst demonstrating simultaneously enhanced explosive capture and degradation is developed. The synergistic interplay of electrostatic attraction and hydrogen bonding between the amino groups of AFM and nitro groups of nitro-aromatic explosive confer exceptional binding affinity. The optimized AFM exhibits a remarkable 2,4,6-trinitrotoluene (TNT) adsorption of 14.93 mg/g, which is 3.6 times of unmodified MIL-100(Fe). In photo-Fenton reactions, the optimized AFM completely degrades TNT within 30 min, and achieves a mineralization efficiency as high as 96.7 %. Moreover, the AFM exhibits excellent stability, retaining a high TNT degradation efficiency of 97.7 % after five consecutive cycles. The currently designed AFM catalyst possessing fascinating explosive affinity and high explosive mineralization efficiency is expected to advance sustainable remediation of high-risk explosive wastewater.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Tiefeng Xu,Chenyu Li,Ke Xiang,Yingxin Lu,Wangyang Lu
The photocatalytic removal of organic pollutants from wastewater has gained significant attention in recent years due to its environmental benefits and cost-effectiveness. In this study, a pyrolytic iron phthalocyanine/graphitic carbon nitride (FePc/g-C 3 N 4 ) composite photocatalyst was synthesized using ball milling and thermal cracking, and its performance in photocatalytic degradation along with the underlying mechanisms was investigated. Under solar light irradiation, the pyrolytic FePc/g-C 3 N 4 photocatalyst achieved complete carbamazepine (CBZ) degradation within 12 min by activating peroxymonosulfate (PMS), demonstrating a 29 % enhancement in degradation efficiency compared to the unpyrolytic FePc/g-C 3 N 4 . Additionally, the stability of the catalyst improved significantly post-pyrolysis, maintaining over 98 % degradation efficiency across nine cycles. The thermal treatment disrupted the phthalocyanine structure, modifying the coordination environment of the central Fe atom and facilitating the transfer of photogenerated charge carriers. This research provides valuable insights for designing stable single-atom iron-based composite photocatalysts.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2025
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IF 7.8
Huan He,Yixin Liu,Qiuyun Chai,Xiaofang Ma,Chaochao Lai,Ziwei Guo,Guoli Dong,Bin Huang,Xuejun Pan
Conventional plastic waste management through landfilling and incineration not only consumes vast land resources but also emits hazardous compounds, severely endangering ecosystems. An emergent and promising solution is the conversion of this waste into functional carbon-based materials for water purification, enabling sustainable reuse. Herein, four kinds of plastics were pyrolyzed to char doped with Fe and Ca for peroxymonosulfate (PMS) activation to degrade bisphenol A (BPA). The doped char exhibited highly effective adsorption and catalytic capabilities for BPA removal. Fe-doping enhanced the adsorptive removal of BPA by increasing the specific surface area and adsorption sites of the char. The Fe/Ca co-doped catalyst achieved 94.1 % BPA removal within 10 min, while the Ca components effectively reduced post-reaction SO 4 2- accumulation, mitigating secondary ionic pollution. Quenching experiments and EPR analyses confirmed the generation of SO 4 – ·, ·OH, ·O 2 – and 1 O 2 , indicating the coexistence of radical and non-radical oxidation pathways. Moreover, the waste-plastic-derived char with Fe/Ca also exhibited a high BPA removal efficiency of 81.2 %, and the residual toxicity of BPA was markedly reduced after degradation. This study proposes a novel strategy that synergistically combines resource recycling with pollutant removal.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Shu-Hu Yin,Xiao-Yang Cheng,Yu Han,Ting Zhu,Zhong-Wei Yu,Rui Huang,Jun Xu,Yan-Xia Jiang,Shi-Gang Sun
Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions (ORR), yet their moderate intrinsic activity and susceptibility to reactive oxygen species (ROS)-induced degradation hinder practical implementation. Herein, we fabricate a Ru-Fe dual-site catalyst (RuFe-N-C) through a two-step pyrolysis strategy. Structural characterization reveals atomic-scale proximity between Ru single atoms and Fe-N 4 moieties, exhibiting a projected distance of ~1.7 Å. This configuration induces Fe–N bond elongation accompanied by 2.5% lattice distortion. The optimized RuFe-N-C catalyst exhibits high ORR performance, with a half-wave potential ( E 1/2 ) of 0.840 V and peak power density ( P max ) of 938 mW cm –2 under 150 kPa absolute H 2 -O 2 . These metrics signify substantial enhancements relative to conventional Fe-N-C benchmarks (+21 mV in E 1/2 and +42% in P max ). Moreover, the catalyst maintains outstanding stability, showing merely 17 mV E 1/2 decay after 10000 accelerated durability test (ADT) cycles. Experimental analyses reveal a bifunctional mechanism: (1) Adjacent Ru sites substantially enhance the intrinsic ORR activity of Fe-N 4 moieties, delivering a notable turnover frequency (TOF = 17.86 e site –1 s –1 at 0.85 V vs. RHE) that exceeds state-of-the-art Fe-N-C benchmarks by 1–2 orders of magnitude (< 1 e site –1 s –1 ); (2) Ru centers function as electron relays that facilitate ROS scavenging, thus suppressing degradation. This work establishes a paradigm for engineering bimetallic single-atom catalysts through synergistic electronic modulation to concurrently enhance activity and stability.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2025
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IF 2.9
Jiaqi Li,Yidan Zhang,Pingyu Luo,Chun Li,Fanming Zeng,Tiantian Sun,Hanhui Lei,Xiaoteng Liu,Chunbo Liu
Persulphate-based advanced oxidation technology efficiently and cost-effectively removes organic dyes from water but designing stable photocatalytic systems and understanding their reaction mechanisms remain key challenges. Metal–organic frameworks (MOFs) have attracted considerable research attention for degrading organic pollutants owing to their high porosity, tunable structure, and ease of modification. In this study, a series of M-MOF-74 (M = Co, Fe, Ni) photocatalysts are synthesized by a hydrothermal method for methylene blue (MB) degradation. Among them, the Co-MOF-74 photocatalytic synergetic peroxymonosulfate system exhibits high catalytic activity after 30 min of visible light irradiation. MB degradation efficiency reaches 94.8%, and the reaction rate constant is 0.210 min−1, which is approximately 19.44 times higher than the reaction rate constant of the original Co-MOF-74. Compared with Fe-MOF-74 and Ni-MOF-74, Co-MOF-74 exhibits better photocatalytic performance due to the dynamic changes in the valence state of cobalt, which more effectively facilitate the activation of PMS. In addition, this study analyses the possible degradation pathways of MB in water and toxicological evaluations of intermediate products, providing new insights for the effective removal of dyes in water.
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LAB ON A CHIP
·
2025
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IF 5.4
Jie Chen,Penghui Li,Ran An,Aishan Cai,Kaiqi Wang,Zheyu Zhang,Tao Wang,Yuandu Hu
Although shape-controllable alginate-based microgels via droplet microfluidics have been widely investigated, studies have mostly focused on tuning the designs of microfluidic devices and parameters of the crosslinking media, and very little attention has been paid to studying the effect of droplets' compositions on the morphologies of the resulting microgels. In the present study, droplets of aqueous solutions of sodium alginate (SA) with different additives (i.e., 10 wt% dextran, PEG, or glycerol) have been produced from microfluidics and collected in solutions with different concentrations of glycerol (0–70 wt%) and FeCl3 (2–10 wt%). The effect of droplet compositions on the morphologies of resulting Fe-alginate microgels has been systematically investigated. The results showed that the morphologies of the microgels were remarkably influenced by the interactions between the droplets and the collecting solutions, leading to the formation of microgels with different shapes. Additionally, microgels prepared under specific conditions exhibited certain deformation patterns. For example, dimpled microgels with large cavities exhibited an increase in cavity size in collecting solutions with higher concentrations of glycerol and FeCl3 (the value of d/D rose from 0.3 to 0.5, D and d represent the outer contour dimension and the cavity diameter of the microgel). Similarly, red blood cell-like microgels showed an increase in concavity depth as the concentrations of glycerol and FeCl3 increased (the value of D/L rose from 1.7 to 3.7, D represents the horizontal length of the microgel, and L indicates the vertical depth of the concave). The dimple-like microgels were uniquely advantageous in terms of rapid and efficient payload release (up to 98% release in 5 hours, 16.68 μg of total release), significantly superior to the spherical microgels (82% release in 5 h, 12.54 μg of total release). These findings establish a framework for morphological engineering of microgels, offering promising opportunities for applications in payload delivery systems requiring rapid and controlled release profiles.
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FUEL
·
2025
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IF 7.5
Lina Dai,Qiang Li,Xianglan Dong,Enqi Zhang,Yufeng Hu,Xin Guo,Yanduo Liu
Photocatalysis exhibits great potential for applications in solving energy and environmental problems, and has received widespread attention. This article constructs a new type of Mn-Fe Prussian blue analogues S-scheme mechanism photocatalytic material. The material is composed of oxidized photocatalysts (Ag 2 MoO 4 ) and reduced photocatalysts (Mn-Fe PBAs). The composite photocatalyst constructed in this way shows advantages such as a wide spectral response range, high charge carrier separation efficiency, and strong oxidation–reduction ability, which can significantly enhance photocatalytic efficiency. By studying the construction method and CO 2 reduction performance of the photocatalyst, the structure-performance relationship can be clarified. The CO production rate is 43.3 μmol/g/h, and the selectivity can reach 94.9 %, which is far superior to the current mainstream photocatalytic system. The electron transfer kinetics and S-scheme charge separation mechanism between the Mn-Fe PBAs and Ag 2 MoO 4 interfaces are explained by steady-state surface photovoltage spectroscopy (SS-SPS) and near ambient pressure XPS (NAP-XPS). In-situ DRIFTS techniques are used to monitor the changes of transition intermediates, and combined with theoretical calculations, the activation mechanism of CO 2 by the Mn-Fe catalytic site is deeply revealed at the atomic level. This study provides new theoretical guidance and profound insights for the construction of Prussian blue analogues photocatalysts.
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Matter
·
2024
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IF 17.3
Lingfeng Li,Jiaming Zhu,Fanpeng Kong,Yijie Wang,Cong Kang,Ming Xu,Chunyu Du,Geping Yin
Elucidating how the local strain environment of single atoms affects their impact on a sluggish acidic oxygen reduction reaction (ORR) is important for the design and construction of highly active electrocatalysts. Here, we report that the atomic strain geometry of Fe single sites is exclusively regulated by the communicative effects of dual atoms. Theoretical analysis reveals that Fe-Ru dual atoms in a moderate strain environment achieve the lowest Gibbs free energy barrier during an ORR. Impressively, FeRu-N-C with an FeRuN 8 moiety exhibits the highest acidic ORR performance, with a half-wave potential ( E 1/2 ) of 0.860 V and only a 17-mV loss in E 1/2 after 50,000 potential cycles. Operando characterization and electronic configuration analysis demonstrate that moderately strained Fe sites promote hydrogenation desorption of (oxy-)hydroxyl by enabling more electrons to occupy antibonding orbitals. This study describes a promising way of investigating high-performance single-atom-based catalysts by tailoring the atomic strain environment.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120613
·
IF 7.2
Xiao Feng,Qiqi Gan,Zhongliang Li,Yunhong Zhao,Tengfeng Xie,Dejun Wang,Yanhong Lin
Photocatalysis-coupled advanced oxidation rapidly mineralizes pollutants; here we engineer a Fe-CoS 2 /ZnIn 2 S 4 composite catalyst that activates peroxymonosulfate under visible light to eliminate tetracycline within minutes. The structure, morphology, composition, and optical properties of the photocatalyst were analyzed in detail. Fe-CoS 2 /ZnIn 2 S 4 exhibited markedly improved degradation performance, achieving 88 % TCH removal within 10 min and 94.6 % degradation efficiency within 30 min. The separation and transfer characteristics of photogenerated charges were investigated via surface photovoltage (SPV), transient photovoltage (TPV), photoluminescence (PL) spectroscopy, and UV–visible diffuse reflectance spectroscopy (UV-Vis DRS). Furthermore, the degradation of organic pollutants by sulfate radical-based advanced oxidation processes (SR-AOPs) assisted by photocatalysis was thoroughly studied. The test results demonstrate that the synergistic effects of metal nanoparticle loading and heterojunction construction enable the composite catalyst to achieve efficient photogenerated-carrier separation and rapid Co 3 + /Co 2+ cycling, thereby accelerating PMS activation and generating abundant radicals for pollutant removal. This study offers new insights for developing highly efficient PMS photo-activators for water treatment.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2025
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IF 4.9
Li Huanxuan,Wei Xueheng,Gao Xing,Liu Chen,Li Ning,Xu Chen,Huang Jingang,Liu Xiuyan,Xu Shaodan
The degradation of antibiotics remains a major and persistent challenge in wastewater treatment. This study reports the synthesis of three distinct catalysts from a zeolitic imidazolate framework-67 (ZIF-67) precursor through pyrolysis at 800 °C, namely ZIF-67(Fe)-800, ZIF-67(Co)-800, and ZIF-67(FeCo)-800. Comprehensive characterization (e.g., X-ray diffractometer and transmission electron microscopy analyses) confirmed their graphitic carbon matrix, specific metallic phases, and unique polyhedral morphologies. These catalysts were employed to activate peroxymonosulfate (PMS) for ciprofloxacin (CIP) degradation. Strikingly divergent catalytic performances were observed, with CIP degradation rate constants of 0.0027, 0.0731, and 0.0504 min –1 for ZIF-67(Fe)-800, ZIF-67(Co)-800, and ZIF-67(FeCo)-800, respectively. Furthermore, the bimetallic ZIF-67(FeCo)-800 demonstrated consistently inferior performance in activating both peroxydisulfate and sodium percarbonate compared to PMS, resulting in significantly lower CIP degradation rates of 52% and 87%, respectively. Mechanistic investigations using electron paramagnetic resonance and quenching tests revealed that hydroxyl radical ( · OH), sulfate radical (SO 4 •− ), and singlet oxygen ( 1 O 2 ) were the dominant reactive species in both the ZIF-67(Fe)-800/PMS and ZIF-67(Co)-800/PMS systems. In contrast, the ZIF-67(FeCo)-800/PMS system operated via a distinct pathway, primarily generating SO 4 •− , accompanied by · OH, 1 O 2 , and superoxide radicals (O 2 •− ). Notably, H 2 PO 4 − and HCO 3 − exhibited strong inhibitory effects on CIP degradation, while SO 4 2− and CH 3 COO − led to modest rate enhancements. Overall, this work provides a rational framework for designing MOF-derived catalysts and highlights their potential for application in advanced oxidation processes aimed at removing pharmaceutical pollutants.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Bin Zhu,Wei Zhang,Shihao Li,Naifeng Wen,Jingqiang Zheng,Chaohong Guan,Jie Li,Zhian Zhang
Li5FeO4 (LFO) is a leading candidate for cathode prelithiation due to its ability to engage in both anionic and cationic redox processes, offering substantial capacity potential. However, the practical implementation of LFO is hampered by incomplete delithiation and susceptibility to air-induced degradation, which together constrain its effectiveness in lithium compensation. In this study, we propose a lattice modulation strategy that incorporates cobalt substitution at the iron sites of LFO, resulting in the novel compound Li5.5Fe0.5Co0.5O4 (LFCO), which enhances both the anionic redox activity and the air stability of the material. We demonstrate that the incorporation of Co2+ ions facilitates the reversible oxidation of lattice oxygen species from O2– to intermediate O2n– and ultimately to O2, thereby augmenting the overall redox capacity. LFCO exhibits superior electrochemical performance with specific capacities of 860.1 mAh g–1 at 0.1C and 580.0 mAh g–1 at 1C, compared to 681.5 and 351.8 mAh g–1 for LFO. Furthermore, LFCO maintains a high capacity of 520.8 mAh g–1 after exposure to 20% relative humidity for 4 days. Integration of LFCO into graphite∥NCM811 pouch cells results in 89.6% capacity retention at 0.5C over 200 cycles, underscoring the potential of this material in developing next-generation energy-dense lithium-ion batteries.
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