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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Calcium-rich biochar-enhanced Cu-Al2O3 fenton-like catalyst with dual reaction centers for efficient decomplexation of Ni-EDTA

Shuyu Qi,Zilong Zhao,Yingqing Ou,Lu Liu,Yatao Ren,Wenyi Dong,Hongjie Wang,Zigong Ning

In this study, a calcium-rich biochar (CRB)-enhanced dual reaction center (DRC) Fenton-like catalyst, Cu-Al 2 O 3 -CRB, was synthesized for the decomplexation of a typical heavy metal complex pollutant, Ni-ethylenediaminetetraacetic acid (Ni-EDTA), in industrial wastewater. After a 90-minute reaction, the removal rate of Ni(II) could reach 95.2%, regardless of the initial solution pH. Various characterization analyses confirmed the formation of electron-rich Cu regions and electron-deficient Al and C regions in the Cu-Al 2 O 3 -CRB catalyst. The catalytic oxidation experiments, chronoamperometry tests, and reactive oxygen species (ROSs) detection further revealed the roles of biochar and CaCO 3 on the catalytic behavior of Cu-Al 2 O 3 -CRB catalyst. The presence of biochar not only enhanced the loading of Cu species but also introduced additional electron transfer channels, while CaCO 3 further interacted with biochar/Cu species to amplify the electron cloud density surrounding Cu. The improvement of electronic polarization facilitated the activation of H 2 O 2 and the generation of •O 2 – , 1 O 2 and •OH. Contrary to conventional interfacial reactions, the weak adsorption between Cu-Al 2 O 3 -CRB and Ni-EDTA due to the electrostatic repulsion, led to the decomplexation reactions primarily occurring in the solution phase, rather than on the catalyst surface. This study sheds light on the potential of Cu-Al 2 O 3 -CRB as a DRC catalyst and emphasizes the significance of contaminant properties when using this kind of catalysts.

研究领域: 环境科学 · 催化化学
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Desalination and Water Treatment · 2024 · IF 1

Ca-doped g-C3N4 was prepared by two-step calcination for efficient photodegradation of methylene blue

Chaoliang Wang,Xiaoyang Zhao,Yongjun Li,Dehu Yang,Fuyang Liu,Feng Liu,Li Li,Ping Ke

A series of simple and low-cost Ca-doped g-C 3 N 4 (Ca/CN-X) photocatalysts were fabricated through a two-step calcination method for photodegradation of methylene blue (MB) simulated dyeing wastewater. The results showed that the photodegradation efficiency of Ca/CN-15 % on MB removal under visible light was 97.7 %, and the degradation rate constant was 4 times that of CN, showing the best photocatalytic performance. This was attributed to the fact that the doping of Ca expanded the absorption band edge, reduced the band gap, and suppressed the photogenerated electron-hole recombination, thereby increasing its corresponding photocatalytic activity. A possible photodegradation mechanism was explored, and it was found that h + was the main active species during the process. The above indicated that Ca/CN-X can be regarded as a promising catalyst for dyeing wastewater treatment.

CAS / MDL: 3317-61-1
研究领域: 材料科学 · 环境科学
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CHEMOSPHERE · 2024 · IF 8.1

Boron nitride quantum dots supported hollow NH2-MIL-125 drive photo-Fenton-PMS system for photocatalytic tetracycline degradation: Contribution of tannic acid etching

Jun Guo,Jun Hou,Zijun Yang,Jun Xia,Jun Wu,Guoxiang You,Lingzhan Miao

NH 2 -MIL-125(Ti) materials had great potential for photocatalytic applications but had low activity due to exciton effect and narrow absorption range of visible light. The surface oxygen-containing negative functional groups of boron nitride quantum dots (BNQDs) could overcome these defects, but due to the low load capacity, a higher specific surface area of the substrate was usually required. In this paper, a hollow Ti-MOF material was developed by etching technology. The hollow structure formed by tannic acid etching broadened the absorption range of visable light and provided more alternative surfaces for loading BNQDs. The 85.2% of high tetracycline (TC) removal efficiency for the best sample (BNQDs-5@20-Ti-MOF + PMS) was obtained, which was about 56.8 and 1.9 times of the 20-Ti-MOF and BNQDs-5@20-Ti-MOF, respectively. BNQDs-5@20-Ti-MOF + PMS system showed a great TC degradation efficiency in a wide pH range (pH = 5–9). In addition, reaction temperature and the inorganic ions did not show significant inhibition effect for TC removal. Both free radical and non-free radical pathways were involved in the TC degration by BNQDs-5@20-Ti-MOF + PMS system, among which O 2 •− and 1 O 2 played the key roles. Interestingly, multiple 1 O 2 production paths contributed to the high efficiency and stability of BNQDs-5@20-Ti-MOF + PMS system. This study revealed a reasonable combination of Ti-MOF and BNQDs, which provided a new efficient photocatalyst for environmental remediation.

研究领域: 环境科学 · 材料科学
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Journal of Materials Chemistry C · 2025 · IF 5.1

Boosting photoelectricity based on self-supported flexible metal–organic framework arrays for photo-Fenton-like degradation of organic pollutants

Shenghao Wang,Yajuan Wang,Linbo Cao,Jiasheng Zhang,Yuqing Liu,Bo Wang,Mingmin Li

Utilisation of highly efficient catalysts for photo-Fenton-like reactions, although challenging, is urgently desired to alleviate the serious global burden caused by organic pollutants. In this work, an example of two-dimensional (2D) porphyrin (TCPP) MOF arrays vertically grown on a copper foam (CF) was synthesized under hydrothermal conditions. The honeycomb-like structure offers a large surface area and capacious porous space for fast mass transfer and enrichment of organic pollutants. The highly dispersed active site (M–N4) of nanosheet arrays promotes the utilization of visible light to generate and separate photoelectrons and holes. In addition, the photocatalytic efficiency was further strengthened by the introduction of bimetallic sites. The macro-integrated structure can be conveniently recovered for cyclic catalysis, thus reducing costs and avoiding secondary pollution. These features together permit the self-supported 2D TCPP-MOF array's remarkable performance in persistent mineralization of various organic pollutants with different surface charges owing to the production of reactive oxygen species (ROS). This study provides a general method to rationally design and optimize photo-Fenton-like catalytic performance based on 2D MOFs for water remediation.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Boosting oxygen storage capacity of Fe-Cu bimetallic catalysts through sulfide modification for efficient and selective molecular oxygen activation

Yan Sun,Zhicheng Wang,Xiaohui Wu,Wen-Da Oh,Mingjie Huang,Tao Zhou

Molecular oxygen (O 2 ), a reactive oxygen species precursor, has great potential for water purification, but its spin-forbidden resistance hinders its direct involvement in the redox reactions of organic compounds under mild ambient conditions. In this study, a facile strategy was employed to synthesize sulfide-modified Fe-Cu bimetallic catalysts (FeCu-S) to enhance the activation efficiency of O 2 . The results showed that the FeCu-S material exhibited a tenfold increase in O 2 activation compared to that of the control group, primarily attributed to the increased specific surface area of the catalysts with an optimized Fe/Cu site distribution and promoted generation of Cu-containing crystalline phases (e. g., CuFeS 2 and CuO) to significantly enhanced the oxygen storage capacity. Moreover, such Cu-containing crystalline phases strengthened surface electron transfer, thus remarkably promoting the selective generation of singlet oxygen ( 1 O 2 ) for sulfamethoxazole (SMX) degradation. The FeCu-S/O 2 system maintained high activity after the fifth recycle with stable reaction pH and negligible leaching of Cu and Fe ions, also exhibited great performance in the advanced treatment of the real biological effluent and ultrafiltration effluent from landfill leachate, confirming its great potential for practical water purification applications.

研究领域: 环境科学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Boosting molecular oxygen activation through synergistic interaction of boron-doped biochar and ascorbic acid: Key role of BC2O and BC3

Qingyang Dai,Kecheng Zhu,Yongliang Xu,Yixuan Liu,Yuanren Jiang,Chenghe Yan,Chi Zhang,Hanzhong Jia

Ambiguous interpretations regarding the underlying mechanism of molecular oxygen (O 2 ) activation by the carbonaceous material/reductant system, especially in terms of the catalytic active site, have impeded the optimization and broader application of the system in environmental remediation. Here, we thoroughly investigated the role of boron-doped biochar (BBC) active sites in O 2 activation and optimized the ascorbic acid (AA) dosing strategy to improve the hydroxyl radical (•OH) production rate and pollutant removal. The introduction of boron facilitated O 2 activation through the successive one-electron transfer to generate •OH that predominantly occurred and accumulated on BBC surface, where •OH yield was nearly 5-fold and 9-fold higher than that in N-doped biochar/AA and zero-valence iron (ZVI) system, respectively. This results in better degradation performance of BBC/AA system for organic pollutants absorbed on the BBC surface and robust resistance to commonly occurring water anions and negatively charged organic matter. Moreover, the stepwise addition of low-concentration AA (0.5 mM) promoted the BPA removal (over 90 %) by maximizing the effective availability of AA and •OH. Characterization, galvanic oxidation process, and theory calculation results revealed that BC 2 O acted as the primary electron-accepting group to receive the electrons from AA, while BC 3 acted as both an electron-donating group and an O 2 adsorption site on BBC, which together facilitated O 2 activation and •OH production on the BBC surface. These findings provide a comprehensive understanding of O 2 activation within the BBC/AA system, highlighting its potential as a sustainable and effective approach for advanced environmental remediation applications.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Boosted photo-Fenton-like process for selective degradation of emerging contaminants by dehydrated Fe-based metal–organic framework with thermodynamically-favorable center metal electron density and confinement effect

Wei Guo,Xiaoyan Zhang,Ke Wang,Xueyi Zou,Guoshen Zeng,Jiapeng Zhong,FengHui Tian,Chuanhao Li

The Heterogeneous Fenton reaction has long stood out as a highly effective technology for water purification. However, it is nowadays facing challenges such as low selectivity, sluggish Fe(III) reduction, and limited H 2 O 2 conversion efficiency. Herein, dehydrated MIL-100(Fe)-250 was synthesized through thermal treatment, demonstrating superior efficiency in removing emerging contaminants, with a three-fold efficiency higher than undehydrated sample. The dehydrated MIL-100(Fe)-250 exhibited selective acceleration in the removal of quinolones and phenolic organics, rendering the system resistant to interference from coexisting matter. Through in-situ diffuse reflectance infrared Fourier-transform spectroscopy and density functional theory calculation, it was manifested that dehydration process regulates the steric hindrance and local electron density of Fe ions. This adjustment enhances charge transfer, thereby facilitating Fe(III) reduction and promoting the H 2 O 2 activation and conversion efficiency. Moreover, the quasi-steady-state concentrations of hydroxyl radical in MIL-100(Fe)-250 were found to be 2.2 times higher than that those in undehydrated sample. Impressively, the dehydrated MIL-100(Fe)-250 displayed adaptability across a broad pH range of 5.0–9.0. The present study underscores the significant potential of porous MIL-100(Fe)-250 with spatial confinement, which imparts a clear size exclusion effect. As a result, this catalyst emerges as a promising candidate for eliminating contaminants in real water matrices, offering a viable strategy for water pollution control.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Biomass-derived in-situ carbonized ferrous sulfide for Fenton oxidation of phenol in wastewater: mechanisms, pathways, and applications

Fangfang Ye,Xiaoying Jin,Zuliang Chen

Innovative iron-based nanoparticles (NPs) made from biomass provide sustainable solutions for environmental cleanup, integrating better environmental management with resource recycling. This study introduces biomass-derived carbon-coated iron sulfide (FeS@CMP) as an efficient Fenton catalyst for phenol oxidation, addressing challenges associated with FeS NPs in advanced oxidation processes (AOPs), for example deactivation and aggregation. Firstly, advanced characterization reveals its porous structure, high surface area, and abundant active sites, compared to carbonized biomass precursor (CMP), while FeS@CMP demonstrates superior physical and chemical stability. Secondly, FeS@CMP achieves remarkable efficiency in activating hydrogen peroxide (H 2 O 2 ) for phenol removal (94.08%), which is much greater than that of CMP (40.70%). Further, mechanistic analysis identifies a synergistic electron transfer process involving multiple ROS, including •OH, SO 4 -•, and 1 O 2 , driving effective phenol degradation. Thirdly, using Density Functional Theory (DFT) calculations and Liquid Chromatography-Mass Spectrometry (LC-MS), a specific degradation pathway for phenol is proposed. Finally, toxicity assessments reveal a marked decline in toxicity of degradation products and excellent reusability over multiple cycles. FeS@CMP also effectively degrades contaminants in real wastewater. This study converts waste into high-performance biomass-based catalysts, advancing sustainable development and offering an eco-friendly method for phenol removal, enhancing low-impact AOP technologies.

研究领域: 环境科学 · 材料科学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Bioinspired Ultra-Stretchable and Highly Sensitive Structural Color Electronic Skins

Yuanyuan Shang,Chao Huang,Zhou Li,Xuemin Du

Organisms possess remarkably adaptive ability to complex environments. For example, chameleons can alter their skin color to adapt to varying environments, which has inspired significant advances in bioinspired soft electronic skins (E-skins), and their wide applications in wearable sensors, intelligent robots, and health monitoring. However, current bioinspired E-skins face challenges in ultra-stretchability, high sensitivity, and long-term stability owing to the intrinsic limitations associated with their mismatched interface between soft matrix and hard conductive fillers, hindering their practical applications. Here, it is reported that bioinspired structural color electronic skins (SC E-skins) that consist of liquid metal particles (LMPs), periodical ordered colloidal crystal arrays, and ultra-stretchable hydrogel, imparting synergistic and durable electrical–optical sensing capabilities. Such SC E-skins demonstrate outstanding performances including superior flexibility (elongation at break > 1100%), high sensitivity (gauge factor = 3.26), fast synergetic electric–optical response time (≈100 ms), outstanding durability (over 1500 cycles), and high accuracy (R 2 > 99.5%). These bioinspired SC E-skins with excellent capability of converting mechanical signals into synergetic electrical–optical outputs hold great promise for smart wearable devices, affording a new horizon in developing advanced health monitoring technologies.

CAS / MDL: 3317-61-1
研究领域: 材料科学 · 生物医学工程 · 传感器技术
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Bio-inspired nanozymes with smartphone-assisted sensor platform for colorimetric detection of ascorbic acid in fruits and supplements

Jun Li,Zue Hu,Yi Peng,Hui Yang,Qian Zhou,Nan Wang,Xianggui Chen,Xiaoqi Yu

Nanozymes have become one of the key applications in the analysis and sensing of food. However, nanozymes presented have shortcomings that limit their further application, such as complex raw material sources, and high condition requirements for synthesis. Cu-GSSG nanozymes under green preparation conditions were synthesized inspired by the detoxification process of glutathione in living organisms. Cu-GSSG nanozymes were further loaded onto filter paper to construct a smartphone-assisted colorimetric sensor test strip for ascorbic acid (AA) detection. As the excellent peroxidase-like enzymes, Cu-GSSG nanozymes showed low AA detection limit of 2.9 μM with a wide linear range of 10–300 μM. Cu-GSSG nanozymes exhibited excellent anti-interference, accuracy, and biocompatibility performances for reliable detection AA in prickly pear juice and 10 supplements. The intelligent colorimetric sensor platform based on the bio-inspired Cu-GSSG nanozymes showed the great potential in rapid detection and large-scale screening of AA in fruits and supplements.

研究领域: 食品分析 · 生物医学工程 · 纳米技术
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JOURNAL OF CONTROLLED RELEASE · 2024 · IF 10.5

Biofilm-camouflaged Prussian blue synergistic mitochondrial mass enhancement for Alzheimer's disease based on Cu2+ chelation and photothermal therapy

Lianxin Li,Yu Xiong,Yuewen Zhang,Yujiao Yan,Ruixin Zhao,Fengmei Yang,Meng Xie

Alzheimer's disease (AD) is one of the most common neurodegenerative diseases characterized by cognitive and memory impairment. Metal ion imbalance and Mitochondrial dysfunction, leading to abnormal aggregation of β-amyloid protein (Aβ), are key factors in the pathogenesis of AD. Therefore, we designed a composite nanometer system of red blood cell (RBC) membranes-encapsulated Prussian blue nanoparticles (PB/RBC). Prussian blue nanoparticles (PBNPs) can chelate Cu 2+ and reduce reactive oxygen species (ROS). The RBC membranes are a kind of natural long-lasting circulating carrier. At the same time, through NIR irradiation, the excellent photothermal ability of PBNPs can also temporarily open the blood-brain barrier (BBB), enhance the transmission efficiency of PB/RBC across the BBB, and depolymerize the formed Aβ deposits, thereby achieving the optimal therapeutic effect. In vitro and in vivo studies demonstrated that PB/RBC could inhibit Cu 2+ -induced Aβ monomers aggregation, eliminate the deposition of Aβ plaques, improve the quality of mitochondria, restore the phagocytic function of microglia, alleviate neuroinflammation in APP/PS1 mice, and repair memory damage. In conclusion, our biofilm-camouflaged nano-delivery system provides significant neuroprotection by inhibiting Cu 2+ -induced Aβ monomers aggregation, photothermally depolymerizing Aβ fibrils and reducing the level of ROS, thus effectively ameliorating and treating AD.

研究领域: 神经科学 · 纳米技术 · 药学 · 生物医学工程
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

Bimetal-organic framework derived single-atom-like Co/Fe catalysts for peroxydisulfate activation: The dual amplification of radical and nonradical pathways

Fangxin Deng,Shoushu Wei,Xiangwei Zhang,Yanping Zhu,Qingze Chen,Zhiyi Deng,Runliang Zhu

A novel single-atom-like Co/Fe catalyst (i.e., Co/Fe-N-C) was synthesized by pyrolysis of a Zn/Co/Fe zeolitic imidazolate framework, and applied in peroxydisulfate (PDS) activation for removal of organic contaminants from wastewater. The isolated diatomic metal-nitrogen sites were detected by X-ray adsorption fine-structure. The degradation of four contaminants (i.e., phenol, bisphenol A, 2,4-dichlorophenol, and N-methyl-2-pyrrolidone) with a concentration of 100 mg/L could be degraded separately within 20 min by the Co/Fe-N-C system with 10 mmol/L of PDS, 0.5 g/L of catalyst dosage, and initial pH of 3. Besides, 79.2 % of phenol could be mineralized in 120 min, and the turn-over frequency value of the catalyst was calculated to be 27.17 min −1 , which was higher than the commonly reported homogeneous PS-AOPs. Moreover, the Co/Fe-N-C exhibited high stability (mineralization rate over 70 % after 5 cycles), a wide initial pH range (3−9), and high catalytic performance at 5–20 mmol/L of PDS concentrations. Based on the analysis of radical scavenging experiments and electron spin resonance spectra, the radical and non-radical pathways for PDS activation were proved in the system, and the contribution of phenol degradation by each pathway was clarified.

研究领域: 环境科学 · 催化化学
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