Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122789
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IF 7.5
Dancheng Zhu,Caiyun Zhang,Jiabin Shen,Chao Shen,Chuanhong Jin,Hao Xu
Sulfamethoxazole (SMX), a widely used sulfonamide antibiotic, is a persistent aquatic pollutant due to its resistance to conventional treatment. Here, a Cu-ZSM-5/Ti 3 C 2 composite catalyst was fabricated by electrostatic self-assembly for peroxymonosulfate (PMS) activation. Characterization by XRD, SEM, TEM, XPS, and zeta potential analysis confirmed the successful integration of the components. The catalyst achieved 97.59% removal of 10 mg/L SMX within 30 min. Quenching and EPR results indicated that 1 O 2 was the major reactive species. The enhanced performance under alkaline conditions was associated with the negatively charged composite surface (-38.8 mV at pH 9), the deprotonated state of SMX, and favorable interfacial interactions that may promote preferential oxidation of the isoxazole moiety. Control experiments using a physically mixed sample showed markedly lower activity, especially at pH 11, highlighting the importance of the intimate heterointerface created by self-assembly. The superior activity was attributed to the synergistic interaction between Cu species in Cu-ZSM-5 and Ti-based sites in Ti 3 C 2 . This work provides insight into designing selective PMS activation catalysts for antibiotic-contaminated water treatment.
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Exploration
·
2026
·
IF 30.4
Weiwei Wang,Chun Lu,Xiaoxiao Liu,Wenlong Yang,Jie Zhou,Chenyao Hu,Xin Li,Guangze Nie
Sonopiezo-mediated heterogeneous catalysis is a promising technology for efficient removal of organic pollutants from wastewater. Nevertheless, it is challenging in real water matrix with coexisting ions due to the rather-limited selectivity of reactive oxygen species if any. Herein, a sonopiezo-triggered singlet oxygen evolution system for selective removal of tetracycline hydrochloride (TCH) was rationally designed by SrTiO 3 -TiO 2 heterojunction with a TiO 2 -terminated SrTiO 3 S-scheme interfacial structure. SrTiO 3 -TiO 2 heterojunction exhibits a dramatically expanded piezoelectric constant ( d 33 ), which produces a synergistic effect on improving the separation and transfer efficiency of charge carrier for efficient TCH degradation. Moreover, SrTiO 3 -TiO 2 heterojunction presents a high sonopiezo-current, which attractively indicates that SrTiO 3 -TiO 2 heterojunction has a potential capacity of charge separation under sonopiezo initiation. Remarkably, the mechanism was identified as the continuous generating of singlet oxygen ( 1 O 2 ), in which the sonopiezo-generated electrons trigger the formation of superoxide anion radical (•O 2 − ) and its subsequent transformation to generate 1 O 2 by expending more sonopiezo-generated holes. These findings provided new insights towards developing nonradical system for effective and selective oxidation of electron-rich pollutants via sonopiezo-catalytic process.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2026
·
IF 16.8
Qian Wang,Xuelin Zhang,Xinyue Chi,Weijian Yuan,Dianpeng Qi,Jianfeng Wu
Isostructural Hf- and Zr-based PDI-MOFs reveal metal-node effects. • Hf nodes enhance spin-orbit coupling and intersystem crossing. • Hf nodes promote triplet excitons and singlet oxygen generation. • PDI-MOF(Hf) enables rapid and selective sulfide oxidation. Efficient singlet oxygen ( 1 O 2 )-mediated selective oxidation requires photocatalysts capable of promoting intersystem crossing and enriching triplet states. Metal-organic frameworks (MOFs) provide a multifunctional platform for photocatalytic detoxification, yet how metal nodes regulate excited-state dynamics and triplet exciton formation remains insufficiently understood. Herein, we construct two isostructural perylene diimide (PDI)-based MOFs to systematically elucidate node-dependent spin-orbit coupling effects. The Hf nodes promote spin-related excited-state evolution through a heavy-atom effect, favoring triplet-state formation and 1 O 2 generation. As a result, the Hf-based MOF PDI-MOF(Hf) exhibits outstanding performance in mustard gas simulant detoxification, achieving a half-life of ≈ 4 min while maintaining high selectivity, and exhibits wide-ranging applications in the selective oxidation of aromatic sulfides into sulfoxides. Phosphorescence and in-situ electron paramagnetic resonance spectroscopy measurements corroborate the enhanced triplet-state processes and dominant 1 O 2 -mediated pathway. This work establishes a clear correlation between heavy-atom node engineering and spin-dependent photophysics, providing a general strategy to overcome intersystem crossing limitations in organic chromophores and advancing the rational design of MOF photocatalysts for detoxification and selective oxidation. Download: Download high-res image (190KB) Download: Download full-size image
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NANOTECHNOLOGY
·
2018
·Vol. 29
·期 25
·255101
·
IF 3.404
Xin Zhang,Qi Yan,Di Naer Mulatihan,Jundong Zhu,Aiping Fan,Zheng Wang,Yanjun Zhao
The efficacy of nanoparticulate photodynamic therapy is often compromised by the short life time and limited diffusion radius of singlet oxygen as well as uncontrolled intracellular distribution of photosensitizer. It was hypothesized that rapid photosensitizer release upon nanoparticle internalization and its preferred accumulation in mitochondria would address the above problems. Hence, the aim of this study was to engineer a multifunctional micellar nanosystem featured with singlet oxygen-responsive cargo release and mitochondria-targeting. An imidazole-bearing amphiphilic copolymer was employed as the micelle building block to encapsulate triphenylphosphonium-pyropheophorbide a (TPP-PPa) conjugate or PPa. Upon laser irradiation, the singlet oxygen produced by TPP-PPa/PPa oxidized the imidazole moiety to produce hydrophilic urea, leading to micelle disassembly and rapid cargo release. The co-localization analysis showed that the TPP moiety significantly enhanced the photosensitizer uptake by mitochondria, improved mitochondria depolarization upon irradiation, and hence boosted the cytotoxicity in 4T1 cells. The targeting strategy also dramatically reduced the intracellular ATP concentration as a consequence of mitochondria injury. The mitochondria damage was accompanied with the activation of the apoptosis signals (caspase 3 and caspase 9), whose level was directly correlated to the apoptosis extent. The current work provides a facile and robust means to enhance the efficacy of photodynamic therapy.
研究领域:
药学
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纳米技术
·
癌症治疗
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Peng Jin,Niao Fu,Ruining Bai,Qingzhi Liu,Yujiao Liu,Mei Chen,Jieli He
Eutrophication-driven cyanobacterial blooms release microcystin-LR (MC-LR), a potent hepatotoxin, posing severe environmental and public health risks. Effective, safe MC-LR degradation is critical for water remediation. Herein, we propose a rationally designed unique donor–acceptor–acceptor (D-A1-A2) structural strategy to synthesize a covalent organic framework (COF-TFP-TAPT-Me) for visible-light-driven, controllable 1 O₂-mediated MC-LR photocatalysis. Structural/optoelectronic characterization confirmed triazine-based A2 (Melem) incorporation narrowed the parent D-A1 COF's band gap to 1.15 eV (vs. 1.38 eV) and enhanced charge separation via forming continuous π-conjugation, ordered π-π stacking, and a multi-level energy structure that promotes directional electron transfer (1.6-fold higher photocurrent than the parent COF). COF-TFP-TAPT-Me nearly completely degraded MC-LR in 25 min, with a pseudo-first-order rate constant 1.66-fold higher than the parent COF and outperforming benchmarks like P25 and PCN. Mechanistically, its D-A1-A2 configuration effectively enables highly selective and dominant 1 O₂ generation in metal-free COFs (in contrast to mixed ROS in the parent COF) via photosensitized energy transfer, selectively attacking MC-LR's Adda chain (UPLC–MS verified). The catalyst retains >95 % activity after 5 cycles, is stable in natural water, and shows >80 % cell viability in cytotoxicity assays. This work highlights a novel D-A1-A2 framework for regulating 1 O₂-dominated degradation, offering a trinity of high efficiency, stability, and low toxicity strategy for water purification.
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
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有机框架
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Xiaoyu Qiu,Linting Zou,Jianmei Cen,Xingnian Duan
In this research, Mo-oxides complexes combined with Co(OH) 2 grown on three-dimensional (3D) nickel foam (Mo-Co(OH) 2 /NF) were developed as a peroxymonosulfate (PMS) activator enabling a pathway transition from radical to non-radical for efficient degradation of organic pollutants. The incorporation of high-valence Mo species promoted the formation of sheet structure and facilitated the Co(II)/Co(III) ratio, while Co served as the primary active site for PMS activation. Consequently, complete removal of 40 mg/L Rhodamine B (RhB) in optimized conditions (catalyst = 1.5 cm 2 , 0.4 g/L PMS dosage, reaction temperature = 25 °C) was achieved within 2 min. In addition, excellent adaptability was exhibited over a wide pH (3.0–9.0) and versatility (99 %, 80.94 % and 91.54 % for MB, LFX, and TC, respectively) in Mo-Co(OH) 2 /NF + PMS system. Impressively, radical scavenging experiments and electron spin resonance (ESR) analyses revealed that the degradation process was mainly dominated by the conversion of O 2 •– to non-radical 1 O 2 . Hence, this work demonstrates the potential of high-valent metal-oxides complexes integrated with Co(OH) 2 as effective PMS activators for non-radical degradation of dye and other refractory antibiotics, significantly broadening their applications in environmental remediation.
研究领域:
环境科学
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材料科学
·
化学工程
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Fangfang Gao,Guanyun Zhang,Dexin Wang,Juan Wang,Linping Liu,Yuting Li,Lixia Xuan,Junshuo Nie,Haoru Song,Guo Wang,Yifeng Wang
In photocatalysis, the nature of reactive oxygen species plays a pivotal role in determining product selectivity. Yet, selective generation of singlet oxygen (1O2) is particularly desirable for achieving targeted photooxidations. Herein, two new nanosized titanium-oxide clusters (TOCs) doped with Ce, Ti14Ce2 and Ti4Ce2, were synthesized and explored in the selective photocatalytic oxidation of benzyl alcohols to benzaldehydes under mild conditions. Interestingly, the titanium-oxide core of Ti14Ce2 is recognized as a fragment of anatase TiO2, positioning Ti14Ce2 as a molecular model for Ce-doped TiO2 nanoparticles. Ce-doping effectively reduces the bandgap energy of the clusters, enabling visible-light absorption and enhancing their photocatalytic properties. Moreover, it promotes efficient energy transfer to O2 for 1O2 generation by increasing spin–orbit coupling. Both clusters exhibited high activity and selectivity in the oxidation of benzyl alcohols to benzaldehydes under visible-light irradiation. Our findings not only expand the TOC family with novel Ce-doped members but also offer insights into designing photocatalysts at the atomic level to enhance 1O2 generation for selective photo-oxidations.
研究领域:
材料科学
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光催化
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无机化学
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纳米技术
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物理化学
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高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yi Han,Mengxin Guo,Hongcheng Gao,Changyong Zhang,Keping Lu,Dejin Wang,Hongyu Xia,Zheng Peng
Sonophotocatalysis (SPC) has been designed as an emerging treatment technology to degrade organic pollutants in wastewater. Reed and Red mud waste were utilized to synthesize a novel heterojunction catalyst (RSRM50-1100) through co-pyrolysis processes. Several characterization tests and density functional theory (DFT) calculations confirmed that the FeAl 2 O 4 /Fe 3 O 4 /BC heterojunction was present in RSRM50-1100, and the spontaneous electron transfer occurred from FeAl 2 O 4 to Fe 3 O 4 within the heterojunction. Meanwhile, RSRM50-1100 exhibited excellent degradation and photoelectric properties in SPC system. Furthermore, a series of free radical identification experiments confirmed that 1 O 2 was dominant in the SPC system of RSRM50-1100. The generation of 1 O 2 stemmed from the reaction of h + / · O 2 − and •OH/ · O 2 − , with the •OH/ · O 2 − reaction dominating. These findings not only showed that a novel photocatalyst RSRM50-1100 had an excellent performance for mitigating water pollution, but also proposed a promising strategy for disposing solid wastes.
研究领域:
环境科学
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催化
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材料科学
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水污染控制
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化学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Xue Zhao,Xue Li,Zhu Zhu,Wanbiao Hu,Haibo Zhang,Jian Xu,Xun Hu,Yingtang Zhou,Ming Xu,Hucai Zhang,Guangzhi Hu
Effective removal of pollutants that affect human health and ecosystem stability is a crucial challenge. Here, the structural confinement engineering strategy realizes the effective anchoring of atomically dispersed Co in the B-doped-CN network (BCN) (BCN/CoN[2 +2]). The advanced oxidation process (AOP) involved BCN/CoN[2 + 2] has realized the rapid and complete degradation to tetracycline (TCL), the removal of approximately 80% and 100% of tetracycline was achieved in 5 min and 30 min, respectively. The AOP with BCN/CoN[2 + 2] can degrade TCL over a wide pH; in addition, BCN/CoN[2 + 2] has the ability to efficiently degrade common pollutants, and its catalytic activity did not decay even if it was used repeated five times. Electron paramagnetic resonance (EPR) spectroscopy shows that BCN/CoN[2 + 2] drives the complete conversion of peroxymonosulfate (PMS) to 1 O 2 , and density functional theory calculations demonstrate that the base for the conversion of PMS to 1 O 2 is from the isolated state of the active site Co.
研究领域:
环境科学
·
材料科学
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Shiqi Liu,Zichen Zhang,Fei Huang,Yongze Liu,Li Feng,Jin Jiang,Liqiu Zhang,Fei Qi,Chao Liu
N-doped carbonaceous materials are promising efficient catalysts for peroxymonosulfate (PMS) activation. In this study, the high-efficient N-doped carbon materials were prepared by direct carbonization of polyaniline (PANI) at 700 °C–1000 °C. It was optimized that the CPANI-9 (carbonized polyaniline prepared at 900 °C) exhibited excellent catalytic performance to activate PMS for phenol degradation, which was efficient over a wide pH range (pH 3.5∼9). In the CPANI-9/PMS system, the PMS adsorption/activation was identified as the key step determining the reaction rate. The quenching experiments and electron paramagnetic resonance demonstrated that the non-radical pathway was dominant in phenol degradation and singlet oxygen ( 1 O 2 ) was the main active specie. Graphitic N, pyridinic N, defects and ketonic groups (C O) were identified as catalytic sites. Interestingly, only the presence of PO 4 3− greatly decreased the phenol degradation rate and PMS decomposition. The CPANI-9/PMS system could also degrade effectively various organic pollutants , indicating that it had potential practical application.
研究领域:
环境科学
·
化学工程
·
材料科学
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JOURNAL OF NANOBIOTECHNOLOGY
·
2026
·
IF 12.6
Hao Zhang,Xiaoyu Song,Leilei Zhao,Chenlong Wang,Shen Chen,Yinghui Wang,Li Zhang,Fangyi Xu,Hongjie Zhang,Qilong Wang,Chao Luo
Photodynamic therapy (PDT) holds significant potential for tumor treatment, yet its immunotherapeutic efficacy is severely constrained by the immunosuppressive tumor microenvironment (TME) marked by lactate accumulation, hypoxia, and glutathione (GSH) overexpression. To overcome these limitations, we engineered an injectable hydrogel system (FPH@A/C) that synergistically integrates oxygen-independent PDT, ferroptosis activation, and lactate metabolic reprogramming to remodel immunosuppressive TME and potentiate antitumor immunity. The hydrogel comprises singlet oxygen-preloaded iron-based nanoparticles (FPH), lithium carbonate (LC), and sodium alginate (ALG), rapidly crosslinking into a stable matrix when encountering physiological Ca²⁺ concentration for localized therapeutic delivery. Within TME, GSH-triggered FPH degradation releases Fe²⁺ and pre-stored singlet oxygen, enabling chemodynamic therapy (CDT) and photo-independent PDT to induce tumor ferroptosis. Simultaneously, LC reprograms lactate-a metabolic byproduct-into an energy substrate for CD8⁺ T cells, counteracting lactate-driven immunosuppression. Notably, combining FPH@A/C with immune checkpoint blockade (ICB) therapy demonstrates synergistic effects, robustly enhancing dendritic cell maturation and cytotoxic T lymphocyte infiltration. This multifunctional platform establishes a novel paradigm for colorectal cancer immunotherapy by concurrently addressing metabolic constraints and immune evasion mechanisms.
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高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2026
·
IF 7.8
Huanxuan Li,Chen Liu,Tao Rao,Zhong Zhou,Zhitong Yao,Wei Han,Jingang Huang,Shaodan Xu,Xiuyan Liu
Developing stable and efficient catalysts for peroxymonosulfate (PMS) activation is of critical significance for the remediation of antibiotic-contaminated wastewater, as conventional catalytic systems often suffer from insufficient activity, poor stability, or a narrow pH adaptation range. Herein, sulfur-doped metal-organic framework (MOF)-derived catalysts (Co-BDC@S) were successfully synthesized via a one-step pyrolysis of cobalt(II) 1,4-benzenedicarboxylate (Co-BDC) and sulfur powder. Systematic optimization of the synthesis parameters revealed that the Co-BDC@S-700–4 catalyst (where the subscripts "700" and "4" denote the calcination temperature and sulfur doping amount, respectively) exhibits superior PMS activation performance. Specifically, it achieves 97 % removal of ciprofloxacin (CIP, 20 mg/L) within 30 min, accompanied by an ultrahigh initial apparent rate constant of 0.268 min⁻¹ . The system has excellent pH tolerance (3–10) and maintains > 73 % efficiency after 5 cycles (Co leaching <1.0 mg/L), meeting wastewater discharge standards. Mechanistic studies confirm singlet oxygen (¹O₂) as the dominant reactive species, whose high steady-state concentration (5.24 ×10⁻¹² M) is attributed to the synergistic effect of Co₄S₃ and sulfur vacancies facilitating electron transfer and non-radical pathways. Furthermore, ultra-performance Liquid Chromatography Triple Time-of-Flight Mass Spectrometry (UPLC-Triple-TOF/MS) identified 22 transformation intermediates during CIP degradation, and ecological toxicity assessment via the ECOSAR model confirms their significantly reduced environmental risks. This work provides a stable, eco-friendly catalyst and valuable mechanistic insights for designing advanced oxidation systems.
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