Materials Horizons
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2025
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IF 10.7
Jian-Hui Zheng,Chang-Long Tan,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Harnessing the power of photoredox catalysis for the selective C(sp3)−H activation and oxidation of alkyl aromatics represents a cutting-edge approach to transforming petroleum-derived feedstocks into value-added C(sp3)−C(sp3) coupled chemicals. Herein, we delve into the photocatalytic process that involves the selective dehydrocoupling of ethylbenzene (EB) to access 2,3-diphenylbutane (DPB) alongside H2, employing three sulfur source-varied ZnIn2S4 (denoted as ZIS-x) catalysts. ZIS-TAA, with thioacetamide (TAA) as sulfur source, exhibits exceptional photocatalytic efficiency for DPB and H2 production. The results show the deficiency of charge carrier recombination centers in defect-poor ZIS-TAA is conducive to the separation of photogenerated charge. Additionally, the larger specific surface area and more surface functional groups provide abundant sites for reactant adsorption and activation, facilitating redox process aided by an ideal band-edge structure. This work illustrates a simple and cost-effective paradigm for designing semiconductor-based photocatalysts with tailored surface properties to enhance the efficiency of target cooperative photoredox reaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Chengwen Zhang,Zihan Li,Chengbo Qian,Ziyang Ye,Feifan Yu,Yuyuan Yao
Developing porous iron-based catalysts with high metal loading for highly efficient removal of the organic pollutants has been a challenge in environmental catalysis. In this work, the preparation of porous iron–nitrogen-co-doped carbon catalyst (pNC-Fe) innovatively utilized zinc nitrate (Zn(NO 3 ) 2 ) as a pore-forming agent and adenine for metal anchoring. The resulting catalyst possessed a high Fe loading (18.49 wt%) and a high specific surface area (395.69 m 2 /g), which enhanced the adsorption and degradation of pNC-Fe. As a demonstration, the maximum adsorption capacity of pNC-Fe for CBZ (389.7 mg/g) surpassed nearly all recently reported CBZ adsorbents. Additionally, pNC-Fe possessed an excellent adsorption regeneration capability even after 5 cycles, enhancing its reusability. Surprisingly, pNC-Fe in PMS system removed almost 100 % of 50 μmol/L carbamazepine (CBZ) in 15 min and performed an excellent k obs (0.5895 min −1 ), outperforming the majority of metal-based catalysts. Interestingly, the adsorption of CBZ by pNC-Fe also remarkably facilitated the degradation of CBZ. Notably, different from the free radical mechanism of most reported work, the quenching experiments and EPR detection demonstrated that the main reactive oxygen species (ROS) of the pNC-Fe/PMS system was singlet oxygen ( 1 O 2 ), endowing pNC-Fe with potential environmental anti-interference capability (less affected by common anions and pH variations). This work provides a valuable insight for the design of porous iron-based catalysts for wastewater remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Bingxuan Ji,LeLe Cui,Zhenghua Zhang
Metal ion leaching and catalytic efficiency decline are inevitable in the Fe-based electro-Fenton (EF) process. Herein, a metal-free EF process was proposed utilizing a system with one anode and two cathodes including an air-diffusion cathode (ADC) and a commercial graphite felt cathode. In the presence of peroxymonosulfate (PMS), this system produced and activated H 2 O 2 while generating reactive oxygen species (ROS). The dual-cathode system demonstrated superior performance, achieving a carbamazepine (CBZ) removal rate constant of 0.0511 min −1 , which is 1.2 times higher than the single ADC cathode system (0.0424 min −1 ). Additionally, the CBZ removal efficiency was increased by 29% at pH = 3 and 21% at pH = 5, respectively. The dual-cathode system also resulted in a significant reduction in energy consumption (219 kWh/kg total organic carbon), which is only 65% and 36% of the energy used by the single ADC cathode system and electrochemical PMS activation system, respectively. In the dual-cathode system, 1 O 2 , •OH, and SO 4 • − were identified, with SO 4 • − might working as a medium to activate H 2 O 2 and generate more ROS. Furthermore, the tailed UV combination effectively removed nearly 100% of CBZ and discharged zero H 2 O 2 , reducing environmental impact. Overall, this work not only provides a green H 2 O 2 production and utilization strategy without metal catalysts but also offers an efficient and low residual oxidant pollutant remediation technology.
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Journal of Water Process Engineering
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2025
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IF 6.7
Jing Zhang,Zhi Song,Boxia Liu,Dongxu Han,Xiayan Zhang,Jialu Liu,Yeqiong Huang,Chuhan Xing
Prussian blue analogues (PBAs) show potential in pollutant degradation, but are often limited by crystal structure regulation and insufficient exposure of active sites. In this study, Bi doping was used to synergistically optimize the crystal structure and electronic environment of CuFe-PBA and construct an efficient CuFe-Bi-3 catalyst for peroxymonosulfate (PMS) activated degradation of tetracycline (TC). The introduction of Bi induces crystal plane reconstruction, enhances the Cu 2+ /Cu + and Fe 3+ /Fe 2+ cycles, and increases the exposure of active sites. The TC degradation rate of CuFe-Bi-3 increased from 72.2 % to 92.1 % within 80 min, and the reaction rate constant increased from 0.01133 to 0.02631 min −1 . Mechanistic studies have shown that Bi regulation promotes the directional generation and utilization of 1 O 2 , constructing a synergistic oxidation pathway dominated by non-free radicals. A comprehensive comparison of EPR signals for various reactive oxygen species showed that the 1 O 2 signal was the strongest, significantly higher than O 2 •- , •OH and SO 4 •- . The system has good stability in various water qualities and a wide pH range, and toxicity assessment also shows that it can effectively reduce the toxicity of degradation products. This study provides theoretical support and application reference for the structure-electronic regulation of PBAs catalysts and Bi doping to construct an environmentally friendly and efficient PMS activation system in a complex water environment.
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INTERNATIONAL BIODETERIORATION & BIODEGRADATION
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2025
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IF 4.1
Zizhuo Li,Jinya Wei,Jitao Li,Yaling Yang,Dezhi Yang,Yuzhu Song
Herein, we rationally designed a novel and forceful ciprofloxacin (CIP) grafted zinc-doped-carbon dots (CIP@Zn/CDs) as an efficient artificial nanozyme against Escherichia coli ( E. coli ), multi-drug-resistant E. coli (AREC), and E. coli biofilms through the peroxidase (POD)-like catalytic activity and the synergistic antibacterial activity of CIP and Zn 2+ . On the one hand, extracellular DNA (eDNA) cleave by high levels of hydroxyl radicals (•OH) catalyzed by the POD-like catalytic activity of CIP@Zn/CDs. On the other hand, CIP@Zn/CDs with positive surface potential, elimination abilities against E. coli via electrostatic interaction, changing the cell membrane permeability and eventually leading to E. coli death within E. coli biofilms. Furthermore, the ultrasmall size of CIP@Zn/CDs possesses good biocompatibility favoring clinical translation. This work provides potential to develop CD-based techniques for applications in the field of selective antibacterial agents towards Gram-negative bacteria.
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FOOD CHEMISTRY
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2025
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IF 9.8
Jun Li,Yanli Li,Yuhan Shi,Zhangqi Li,Chunyu Deng,Guoqi Zhang,Qian Zhou,Zhouyu Wang,Xiaoqi Yu
Constantly escalating oxidative stress greatly increases the daily demand, and total antioxidant capacity (TAC) have become an important indicator. Therefore, the development of effective methods for TAC evaluation remains to be a research hotspot. Herein, a fluorescence/colorimetric sensor based on Fe-adsorbing carbon dots nanozymes (Fe-CDs) was constructed through a rational design. Fe-adsorbing step quenched the fluorescence of carbon dots and restored it by adding antioxidants to achieve fluorescence detection. Furthermore, it endowed Fe-CDs with peroxidase (POD) activity necessary for achieving colorimetric detection. A dual-mode fluorescence/colorimetric sensor array based on Fe-CDs was further constructed to selectively recognize 7 antioxidants and accurately evaluate TAC in 5 actual samples. In addition, Fe-CDs demonstrated excellent accuracy and anti-interference performance in detecting ascorbic acid TAC in fruit juice based on fluorescence/colorimetric methods, with detection limits of 2.1 and 0.4 μM as well as linear ranges of 4–40 and 6.3–150 μM, respectively. Moreover, Fe-CDs indeed guided changes in glutathione content through fluorescence imaging at the cellular level
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Materials Today Chemistry
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2024
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IF 6.7
Zhizhu Yue,Yonghe Yu,Tianjun Hu,Ying Wang,Lulu Cao,Yanxia Zhang,Yuhong Chang,Linjuan Pei,Jianfeng Jia
The development of economical multiphase photocatalysts is a significant challenge in achieving large-scale industrialization. Rational catalyst design can help in achieving efficient, energy-saving, and green catalytic reactions, making it more feasible to screen potential catalyst candidates. In this paper, we have successfully developed a high-efficiency photocatalyst Cu-doped Cu 2 WO 4 (OH) 2 (CWOH-y, where y represents the molar ratio of copper tungsten source), which can catalyze the aerobic coupling reaction of amines to produce corresponding imines under visible light irradiation. N-benzylidenebenzylamine is synthesized under visible light at 25 °C with an 89 % yield. Under natural light at around 35 °C (mean light intensity of 50 mW/cm 2 ), 94 % of the benzylamine is converted, and 97 % of the product is N-benzylidenebenzylamine. The catalyst exhibits high efficiency due to the synergistic effect of doped Cu, Cu 2 WO 4 (OH) 2 , and visible light. This combination generates a significant amount of superoxide free radicals and singlet oxygen when exposed to visible light. Furthermore, the catalyst demonstrates universality and stability with a wide range of amine derivatives. This study introduces a new environmentally friendly photocatalytic pathway for the synthesis of imines and emphasizes the potential applications of Cu 2 WO 4 (OH) 2 .
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WATER AND ENVIRONMENT JOURNAL
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2025
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IF 1.8
Soghra Yaghoobi-Rahni,Habibollah Younesi,Hassan Karimi-Maleh,Nader Bahramifar,Rasoul Malekfar,Hua Yang
This research examined the characteristics and performance of a Bi 2 WO 6 (BWO) based composite manufactured in a simple way for the degradation of amoxicillin (AMX) under 50-watt LED-COB visible light. Various techniques such as SEM/EDS, TEM, XRD, FTIR, BET, TGA, XPS and EPR were used to characterize the BWO composite. The impact of photocatalyst dosage, initial pH and AMX concentration on the catalytic decomposition of AMX was studied. Based on the EPR signals, • OH and • O 2 − are effective factors in the degradation of AMX. The findings indicated that the effectiveness of AMX degradation was influenced by pH, with optimal performance achieved at pH 3, a concentration of 20 mg/L AMX, a catalyst dose of 0.2 g/L and a temperature of 25°C, resulting in a 92.5% removal rate. The investigation also showed that the photocatalytic breakdown of AMX followed the Langmuir–Hinshelwood equation. Additionally, the photodegradation efficiency of AMX increased with temperature, reaching over 98% at 40°C and 50°C. At pH 3, the BWO composite's reusability for the degradation of AMX decreases with five reaction cycles from 98.00% in the first cycle to 78.00% in the fifth, without washing or thermal treatment. Using LC–MS/MS analysis, the breakdown mechanism and potential degradation products of AMX were investigated. This study presents a single-step hydrothermal approach for fabricating Bi 2 WO 6 /Bi 2 O 3 heterojunctions, marking a significant advancement in the development of sustainable and eco-friendly photocatalytic materials for the removal of antibiotics and organic contaminants from water. Summary Oxygen-deficient Bi 2 WO 6 made hydrothermally exhibits good photocatalytic activity in visible light Measurement of free radicals using EPR spectroscopy during amoxicillin degradation Amoxicillin removal efficiency reached 98.76% after exposure to visible light The prepared Bi 2 WO 6 can be reused for up to five cycles while maintaining high stability
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ANALYTICAL CHEMISTRY
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2025
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IF 6.7
Liu Qu,Hong-Yuan Chen,Jun Hu,Jing-Juan Xu
The capture and identification of reactive intermediates, especially the short-lived radical species, play essential roles in elucidating the reaction mechanisms in nanozyme catalysis. To permit the direct characterization of the short-lived intermediates at the solid–liquid catalytic interface with electrospray ionization mass spectrometry (ESI-MS), this work develops a tip-based dual-function nanozyme microreactor/ion emitter. This innovative device was fabricated by decorating a thin-layer nanozyme deposit (e.g., the iron oxide-based nanozyme with peroxidase-like activity) into the inner surface of a microsized glass capillary. Unlike the conventional bottom-up wet-chemistry approaches, the immobilization of the nanozyme was proceeded via a top-down and thermal oxidation method. This procedure enables a clog-free production of the desired thin-layer nanozyme into the front tip of a tapered capillary, with a length of only a few microns. By employing a nanozyme-decorated ion emitter, we achieved the direct detection of various radical intermediates in the peroxidase-like nanozyme-catalyzed chromogenic reactions. Beyond the classical chromogenic reactions, the practicability of the integrative device was further characterized by probing a widely employed fluorogenic reaction, i.e., the deacetylation conversion of Amplex Red (AR) to resorufin. Notably, a radical intermediate (i.e., AR•+) was successfully detected, providing direct evidence supporting the previously speculated radical-mediated reaction mechanism. This work established an effective and convenient method to implement cutting-edge nanozyme catalysis with powerful in situ mass spectrometry. We believe it holds promise for broader application to the in-depth explorations of diverse nanozyme-catalyzed reactions.
研究领域:
纳米催化
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分析化学
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质谱学
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材料科学
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反应机理研究
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Journal of the American Chemical Society
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2025
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IF 15.6
Qian Zheng,Hengyue Xu,Yancai Yao,Jie Dai,Guangming Zhan,Jiaxian Wang,Bing Zhou,Ruizhao Wang,Kaiyuan Wang,Rui Zhao,Bo Yang,Lizhi Zhang
Reverse hydrogen spillover (RHS) from the surface oxygen of titanium oxide to single-atom catalytic centers enables efficient electrochemical hydrogenation via atomic hydrogen (H*) transfer, a process critically dependent on the coordination environment and electronic structure of the active site. In this study, we reveal that a four-oxygen-coordinated Rh single-atom electrode (Rh1O4) exhibits superior RHS capability during water electrolysis of titanium foam compared to its five- or three-coordinated counterparts (Rh1O5 or Rh1O3). The Rh–O coordination number directly modulates the relative position of the Rh d-band center to the Fermi level, thereby regulating H* adsorption on Rh and the RHS efficiency between titanium oxide’s surface oxygen and the Rh single atom on the titanium foam electrode. Remarkably, the four-coordinated Rh1O4 configuration achieves an optimized hydrogen adsorption Gibbs free energy (ΔGH*) of +0.08 eV, approaching that of the coordinating oxygen atoms (−0.47 eV), which drastically reduces the RHS energy barrier to +0.55 eV, significantly lower than those of Rh1O5 and Rh1O3. This structural optimization translates to exceptional electrochemical hydrogenation performance, exemplified by a 4-chlorophenol degradation rate constant of 4.65 h–1, surpassing Rh1O5 (1.18 h–1) and Rh1O3 (0.16 h–1) by 4- and 29-folds, respectively. Our findings highlight the pivotal role of single-atom coordination engineering in tailoring atomic-level hydrogen transfer dynamics and provide a strategic framework for designing high-performance single-atom electrocatalysts for sustainable electrochemical hydrogenation applications.
研究领域:
电催化
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环境修复
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材料科学
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单原子催化
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可持续化学
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Journal of Water Process Engineering
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2025
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IF 6.7
Yongxiu Song,Shifei Kang,Mingzhu Huang,Youduo Wu,Yuyang Lv,Chuang Xue
The generation of hydroperoxyl radical ( OOH) radicals is an important issue and has significant value in the highly selective removal of pollutants in complex water environment. However, the metal active center catalysts frequently encounter the limited surface site type and energy level mismatch, making it difficult to maintain a stable supply of OOH. Therefore, a novel photocatalytic self-Fenton system based on metal-free g-C 3 N 4 /chitosan (g-C 3 N 4 /CS) catalyst was developed to achieve excellent efficiency in the removal of tetracycline, bisphenol A and 2,4-dichlorophenol across a broad pH range (3.14–9.04), superior the conventional Fenton system which only works at pH 3–5. Chitosan modification enhanced the charge separation and transfer efficiency of the S-scheme charge transfer pathway, optimized the formation of OOH, O 2 − , h + , enhancing the selective generation and stable supply of OOH radical with a high ratio of 33 %, led to the efficiency removal of pollutants. Further mechanistic analysis demonstrated the unique dominance of the desired OOH radicals. g-C 3 N 4 /CS catalyst exhibited excellent stability and reusability by the cycling experiments, suggesting durable OOH supplying. This work offers novel insights into g-C 3 N 4 based metal-free catalyst with special radical features through chitosan modification, demonstrating the potential for industrial applications of OOH dominated g-C 3 N 4 /CS self-Fenton system in wastewater treatment.
研究领域:
环境科学
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材料化学
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光催化
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水处理技术
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高级氧化工艺
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Yuqi Sun,Amatjan Sawut,Rena Simayi,Xixi Huang
Though advanced oxidation technologies show promise for water purification, they face challenges. Photocatalysts struggle with recoverability and environmental adaptability, while the Fenton process is limited by the finite cycling of Fe species, low H 2 O 2 utilization, and strict acidic pH requirements. Based on the above issues, this paper developed a novel FeOCl-loaded hydroxypropyl methylcellulose/polyacrylamide (HPMC/PAM) composite hydrogel (FeOCl/HPMC/PAM) is developed as an efficient photo-Fenton-like catalyst. The FeOCl/HPMC/PAM composite system exhibits complex degradation kinetics (zero-order reaction with 5–50 μL hydrogen peroxide solution, first-order reaction with 100 μL hydrogen peroxide solution) and demonstrates highly efficient degradation performance across a broad pH range (1–7). Under pH= 7, it achieves 93.47 % methylene blue (MB) degradation within 60 min via an adsorption-degradation synergistic mechanism. After six cycles, it retains 75 % activity, showing favorable reusability. The cyclic stability test shows that it still retains 75 % of the degradation efficiency after 6 consecutive cycles, confirming its reliable reusability. Meanwhile, the iron leaching rate of the composite material during the reaction is only 0.061 mg/L, confirming its structural stability and environmental safety. With low cost, easy recovery, and wide pH adaptability, this composite hydrogel exhibits potential as a commercially viable system for organic pollutant removal from real water matrices.
研究领域:
环境科学
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材料化学
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水处理技术
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催化化学
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高分子科学
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危险品化学品经营许可证（带存储）