Nature Synthesis
·
2025
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IF 20
Wang Ruizhao,Dai Jie,Zhao Long,Hu Zhiwei,Chen Chien-Te,Kuo Chang-Yang,Zhan Guangming,Shi Yanbiao,Wang Jiaxian,Zou Yunjie,Xu Mingkai,Zou Xingyue,Zheng Qian,Zhou Bing,Wang Kaiyuan,Zhao Rui,Zhang Yan,Shen Yunhao,Yao Yancai,Zhang Lizhi
Electrochemical O 2 activation offers a green approach for efficient synthesis of singlet oxygen ( 1 O 2 ). However, it is commonly determined by adsorption-dependent O 2 activation and transformation and can suffer from the sluggish desorption of surface-bound *OOH. Here we report an adsorption-independent O 2 activation pathway for 1 O 2 electrosynthesis via an O 2 mono-hydrogenation process on compressive-strained rutile TiO 2 (CSR-TiO 2 ). This CSR-TiO 2 achieved an 1 O 2 generation rate of 148.26 μmol l −1 min −1 with near 100% Faradaic efficiency, outperforming the strain-free counterpart (35.97 μmol l −1 min −1 ) and other previously reported materials. Such superior performance of CSR-TiO 2 stemmed from compressive strain, which can suppress the formation of reductive unsaturated sites for the O 2 adsorption and enhance the reductive ability of atomic hydrogen (H*), favouring the O 2 mono-hydrogenation pathway and bypassing the traditional surface-bound *OOH desorption pathway. The generated 1 O 2 could be utilized for the selective oxidation of thioanisole and its derivatives, offering a promising strategy for green organic synthesis.
研究领域:
材料科学
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电化学
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绿色合成
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jiangze Wang,Li Li,Jianglei Sun,Yuxi Shi,Kaixuan Duan,Di An,Ya Zhou,Tong Mu,Die Hu,Tingxin Qian,Chao Liu,Chao Deng,Huining Xiao,Yuqian Liu
Bacterial resistance arising from antibiotic misuse necessitates the development of effective non-antibiotic antimicrobial agents. Herein, we report the synthesis of nitrogen-doped lignin-based carbon quantum dots (N,L-CQDs) with precisely adjustable singlet oxygen ( 1 O 2 ) production efficiency for photodynamic antibacterial therapy. A one-pot hydrothermal method using alkali lignin and ethylenediamine was employed to fabricate a series of N,L-CQDs (N,L-CQDs 1–4 ) with controlled nitrogen-doping levels. Comprehensive characterization reveals that nitrogen-doping enhances graphitization, modifies surface states, and creates in-gap emission centers, leading to tunable optical properties. Crucially, the 1 O 2 quantum yield (QY) was found to be directly dependent on the doping degree, with an optimal value of 82.61%, ranking the top among the reported for carbon-based photosensitizers. Theoretical calculations attribute the maximal 1 O 2 QY to a minimized singlet-triplet energy gap (Δ E ST = 0.27 eV), which facilitates intersystem crossing (ISC). The optimized N,L-CQDs 3 demonstrate potent, light-activated bactericidal activity against both Escherichia coli ( E. coli ) and Staphylococcus aureus ( S. aureus ) via 1 O 2 -mediated oxidative damage. Furthermore, when incorporated into a hydrogel patch, N,L-CQDs 3 significantly accelerated the healing of infected full-thickness wounds in a murine model by eliminating bacteria, modulating inflammatory cytokines, and promoting collagen deposition. This study not only establishes a strategy for tuning the photodynamic efficacy of biomass-derived carbon dots but also underscores their significant potential as low-cost and efficient antibacterial agents for translational wound care.
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Catalysts
·
2022
·Vol. 12
·期 11
·1327
·
IF 4.501
Yifei Qi,Xiaoyue Zhou,Zhenjie Li,Renli Yin,Junhao Qin,Huashou Li,Wanqian Guo,Adela Jing Li,Rongliang Qiu
Peroxymonosulfate (PMS) has been intensively used to enhance the photocatalytic activity of catalysts, which is adopted as an electron acceptor to inhibit the recombination of electrons and holes. However, the effect of holes generated by visible light (VL) on PMS activation is always overlooked. Herein, the VL/Bi2WO6/PMS process was constructed for the efficient removal of organics, in which the degradation rate of carbamazepine (CBZ) increased by over 33.0 times by the introduction of PMS into Bi2WO6under visible light. The radical quenching and determination experiments confirmed that the photogenerated holes could firstly oxidize PMS to form SO5•−and react with HSO5−to produce1O2, then inducing the formation of other reactive species to greatly enhance the performance of pollutant removal by the VL/Bi2WO6/PMS process. Density functional theory (DFT) predicted that sites with high Fukui index (f0) on CBZ were more susceptible to being attacked, resulting in hydroxylation, ring closure, and C=C bond cleavage of CBZ. Toxicity estimation indicated that photocatalysis degradation products from CBZ were less toxic compared to the parent compound. This study provides a potential avenue for improving photocatalytic efficiency and widening the application of photocatalytic technology in wastewater purification.Keywords:Bi2WO6;carbamazepine;peroxymonosulfate;photocatalysis;singlet oxygen
研究领域:
环境科学
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化学工程
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材料科学
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高影响因子
ACS Nano
·
2020
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IF 14.588
Deyang Li,Xiyu Li,Tianyu Zhao,Haichun Liu,Shenlong Jiang,Qun Zhang,Hans Ågren,Guanying Chen
Lead halide perovskites hold promise for photovoltaics, lasers, and light-emitting diode (LED) applications, being known as light-harvesting or -emitting materials. Here we show that colloidal lead halide CsPbCl3 perovskite quantum dots (PQDs), when incorporating divalent manganese (Mn2+) ions, are able to produce spin-paired singlet oxygen molecules with over-unit quantum yield (∼1.08) in air conditions. Our mechanistic studies and atomic-level density functional theory calculations endorse an energy-migration-mediated quantum cutting process favoring multiple singlet oxygen generation (MSOG), in which one exciton-activated bulk Mn2+ ion (∼2.0 eV) inside the nanocrystal migrates its energy among the Mn2+ sublattice to two surface Mn2+ defect states (∼1.0 eV), followed by nonradiative energy transfers to two surrounding oxygen molecules. Moreover, superhydrophobicization of MSOG PQDs through silica-mediated polystyrene encapsulation prevents them from disintegrating in aqueous medium, enabling photodegradation of methyl orange at a rate even higher than that of the canonical titanium oxide photocatalyst. The observation of ultraefficient singlet oxygen generation in PQDs has implications for fields ranging from photodynamic therapy to photocatalytic applications.
研究领域:
材料科学
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光化学
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环境科学
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医学
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Yongguang Bu,Hongchao Li,Wenjing Yu,Yifan Pan,Lijun Li,Yanfeng Wang,Liangtao Pu,Jie Ding,Guandao Gao,Bingcai Pan
Oxygen vacancies (OVs) play a crucial role in the catalytic activity of metal-based catalysts; however, their activation mechanism toward peroxydisulfate (PDS) still lacks reasonable explanation. In this study, by taking bismuth bromide (BiOBr) as an example, we report an OV-mediated PDS activation process for degradation of bisphenol A (BPA) employing singlet oxygen (1O2) as the main reactive species under alkaline conditions. The experimental results show that the removal efficiency of BPA is proportional to the number of OVs and is highly related to the dosage of PDS and the catalyst. The surface OVs of BiOBr provide ideal sites for the inclusion of hydroxyl ions (HO–) to form BiIII–OH species, which are regarded as the major active sites for the adsorption and activation of PDS. Unexpectedly, the activation of PDS occurs through a nonradical mechanism mediated by 1O2, which is generated via multistep reactions, involving the formation of an intermediate superoxide radical (O2•–) and the redox cycle of Bi(III)/Bi(IV). This work is dedicated to the in-depth mechanism study into PDS activation over OV-rich BiOBr samples and provides a novel perspective for the activation of peroxides by defective materials in the absence of additional energy supply or aqueous transition metal ions.
研究领域:
环境科学
·
催化化学
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DOI
PubMed
高影响因子
CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Lingling Kang,Cong Chao,Chenchen Xiong,Shuang Yu,Changtao Xiao,Changsheng Zhao,Shisheng Cui,Jiguang Li,Jing Li,Jianbing Shi,Bin Tong,Zhuo Wang,Yin Song,Weiqian Zhao,Zhengxu Cai,Yuping Dong
Exciton dynamics exert a pivotal role in the photodynamic efficiency of photosensitizers, however, strategies for modulating exciton dynamics to motivate electron transfer in exciton-involved photoreactions remain largely unexplored. Herein, we employed a cutting-edge microfluidic platform combined with computational fluid dynamics to encapsulate a commercial type II PS [rose Bengal (RB)] within a rigid host matrix. This encapsulation yielded host/RB nanoparticles (NPs) with a uniform structure and controllable size. The photoexcited dynamics of these host/RB NPs were characterized using time-resolved spectroscopy, and the results revealed that encapsulation not only extended the triplet exciton lifetime of RB, but also created an optimized environment to motivate electron transfer between RB molecules. These findings rationalize the observed remarkable 20-fold reduction in type II photoreaction and a 3-fold promotion in type I photoreaction for host/RB NPs. Due to the dramatic generation of HO• and O2•–, host/RB NPs demonstrated excellent ability for the in vitro eradication of Staphylococcus aureus and Escherichia coli biofilms and the in vivo treatment of S. aureus-infected wounds under hypoxia, with a minimum killing concentration of 10–7 M. This work sheds light on the motivation of exciton transfer to develop type I PS with enhanced photodynamic properties.
研究领域:
材料科学
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光动力学
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纳米技术
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生物医学工程
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微生物学
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Ximan Wang,Yanshu Chen,Dehui Bian,Sigen A,Wenyue Zhao,Yunfeng Wu,Siqi Bao,Yingchen Duan
Novel Yb-BiOI/Ce-MgAl-LDH S-scheme heterojunction boosts photo-Fenton degradation. • Substrate molecular orbitals govern the selective 1 O 2 -dominated degradation. • S-scheme heterojunction achieves 100% TC-HCl degradation within 20 min. • The system demonstrates excellent environmental adaptability and stability. • Photocatalytic mechanism elucidated via experiments and DFT calculations. Developing highly selective catalytic systems remains a grand challenge in advanced water remediation. A novel S-scheme Yb-BiOI/Ce-MgAl-LDH heterojunction was rationally designed to synergistically boost photo-Fenton degradation via targeted singlet oxygen ( 1 O 2 ) generation. Unambiguously validated by in situ XPS and density functional theory (DFT) calculations, the S-scheme charge-transfer pathway efficiently accelerated spatial carrier separation while preserving maximum redox potentials. Consequently, the composite rapidly degraded the parent tetracycline hydrochloride within 20 min and achieved a mineralization efficiency of 52.5%, exhibiting outstanding degradation performance. Crucially, mechanism studies and density functional theory analyses have demonstrated that this highly selective reaction process, driven primarily by 1 O 2 as the dominant reactive oxygen species, is essentially determined by the energy levels of the specific molecular orbitals of the substrate. Pathway elucidation, coupled with in silico predictions and empirical phytotoxicity bioassays, comprehensively confirmed the substantial reduction in intermediate ecotoxicity. Ultimately, the scientific value of this work lies in providing deep mechanistic insights into S-scheme-driven selective oxidation, offering a robust and sustainable paradigm for designing targeted detoxification systems in wastewater treatment. Download: Download high-res image (262KB) Download: Download full-size image
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Small
·
2026
·
IF 11.8
Chaoyuan Deng,Jiarui Li,Xiaomeng Liu,Shichen Gao,Xunrui Cheng,Dandan Huang,Zhi Zhu,Jiahao Mei,Bo Sheng
The conversion of peroxymonosulfate (PMS) to singlet oxygen ( 1 O 2 ) mediated by Fe-based nanoparticles is significant for environmental remediation. However, the selectivity of this process is often compromised by the apparent valence change of Fe during conventional redox activation. Herein, we report an unconventional PMS activation pathway catalyzed by iron carbide (Fe 2 C), which enables discriminative regulation of 1 O 2 generation from PMS decomposition. Unlike inert Fe 3 O 4 and Fe 2 O 3 catalysts, the surficial Fe 2+ and Fe 3+ sites bridged by carbon atoms in Fe 2 C are identified as the effective catalytic centers. These Fe–C sites achieve PMS activation via built-in electric fields and sustain long-term catalytic activity, thereby bypassing the pathway of full electron transfer that sacrifices low-valent Fe. Consequently, Fe 2 C exhibits a 661.3-fold higher efficiency in levofloxacin removal than Fe 3 O 4 and Fe 2 O 3 . Moreover, the non-radical degradation pathway via 1 O 2 oxidation achieves nearly 100% selectivity, facilitating the complete removal of various pollutants within 5 min. By rationally incorporating covalent coordination into the design of Fenton-like catalysts, this work overcomes the inherent trade-off between activity and durability. Thus, effective water purification is achieved through selective, nonradical reaction pathways.
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PubMed
高影响因子
Redox Biology
·
2026
·
IF 16.2
Yunshen Chen,Gaogao He,Wei Zhang,Jiajie Li,Xiaoxi Li,Sijun Dong,Qinglian Liu,Lei Zhou
By responding to stimuli of diverse physics and chemical nature, transient receptor potential (TRP) channels fulfill important physiological functions in both excitable and non-excitable cells. Capsaicin (CAP) from chili peppers and allyl isothiocyanate (AITC) from mustard are natural and potent agonists for TRPV1 and TRPA1, respectively. Upon exposure to hydrogen peroxide (H 2 O 2 ), the central molecule in redox signaling pathways, TRPA1 shows robust activation and much higher sensitivity than TRPV1. Singlet oxygen ( 1 O 2 ), the molecular oxygen in electrically excited states, is the least studied reactive oxygen species (ROS). Here we report that both TRPV1 and TRPA1 are sensitive to the modification by 1 O 2 , but they exhibit drastically different responses. 1 O 2 generated by excited photosensitizers enhances the function of TRPV1 by accelerating its opening kinetics, increasing the current amplitude, and left-shifting the voltage-dependent activation curve towards physiological membrane potentials. A histidine residue located in the N-terminal ankyrin repeat domain of TRPV1 is identified to be important in 1 O 2 modification process. In contrast, as reported by imaging of cytosolic calcium, 1 O 2 modification of TRPA1 leads to a transient increase and then permanent inhibition of channel activity, and eventually obliterates TRPA1's response to AITC but not carvacrol – electrophilic and non-electrophilic agonists for TRPA1, respectively. Conversely, hTRPA1 is much more sensitive to H 2 O 2 , with the EC50 for channel activation about five times lower than that of hTRPV1, and the responses by two channels to H 2 O 2 mainly involves intracellular cysteine residues. The physiological significance of the distinct responses of TRPV1 and TRPA1 to two representative ROS, 1 O 2 and H 2 O 2 , warrants further investigation.
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PubMed
高影响因子
JOURNAL OF THE INDIAN CHEMICAL SOCIETY
·
2025
·Vol. 103
·期 1
·102321
·
IF 3.4
Juan Wang
Environmental discharge of antibiotics and dyes poses serious threats to human survival and development. In this study, sheet‐like ZnTi‐layered double hydroxide (ZnTi‐LDH) photocatalysts were rapidly synthesized via hydrothermal method at varying reaction temperatures. With increasing hydrothermal temperature, the formation of ZnTi‐LDH became more pronounced, and its photocatalytic performance was assessed using tetracycline hydrochloride (TCH) and Congo red (CR) as model contaminants. The photocatalytic performance of ZnTi-LDH prepared at 210 °C after 60 min of light exposure was optimal, with degradation degree of TCH and CR reaching 84.20 % and 62.75 %, respectively. Similarly, the corresponding first-order reaction rate constants are also the highest, at 0.021 min −1 and 0.010 min −1 , respectively. Mott–Schottky analysis, optical property analysis and electrochemical property analysis combined were conducted to elucidate the photodegradation mechanisms of TCH and CR on ZnTi‐LDH. Reactive‐species trapping experiments confirmed that photogenerated electrons primarily generate superoxide radicals through electron transfer rather than forming singlet oxygen via energy transfer.
研究领域:
环境化学
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材料科学
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光催化
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污染物降解
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纳米材料
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2025
·
IF 3.7
Wanwan Wang,Lei Wang,Rensong Sun,Hao Wu,Ziang Liu,Xiao Qian,Jiayu Quan,Engin U. Akkaya
Graphical β-Galactosidase-triggered release of singlet oxygen is shown to target and selectively eliminate senescent cells. In addition, data obtained using tumor models reveal a significant suppression of tumor progression by targeted singlet oxygen release. Targeting senescent cells for cancer treatment is an important recent direction. In this work, we designed and synthesized a galactoside-functionalized pyridone endoperoxide. The endoperoxide in this form, releases singlet oxygen at a relatively slow rate, but when transformed by β-galactosidase activity, the pyridone endoperoxide releases singlet oxygen with a half-life of 30 minutes at 37 °C. We also studied this compound with a variety of cell lines with differential β-galactosidase expression levels. Cytotoxicity of the target compound is enhanced in high galactosidase-expressing SKOV-3 cells. In vivo tests with tumor models also showed significant suppression of tumor progression. Targeting singlet oxygen to senescent cells appears to be promising new approach for treating diseases concurrent with aging, including cancer.
研究领域:
生物化学
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肿瘤学
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药物化学
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DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Xudong Zhou,Yashi Zhong,Rui Bai,Wei Chen,Junpeng Li,Lifeng Lin,Xiaochun Tian,Feng Zhao
Per and polyfluoroalkyl substances (PFAS) present profound environmental and health hazards owing to their chemical persistence. Photocatalytic technology harnesses solar energy to generate reactive oxygen species for pollutant degradation. However, prevailing studies have emphasized hydroxyl radical mediated pathways. The short lifetime of hydroxyl radical and the stringent conditions required for its formation constrain the efficiency of this approach against recalcitrant PFAS such as perfluorooctanoic acid (PFOA). In this study, a ZnIn 2 S 4 photocatalyst enriched with sulfur vacancies is synthesized via a facile hydrothermal-calcination approach. The introduction of sulfur vacancies enhances visible light absorption and promotes efficient separation of photogenerated electron-hole pairs. Theoretical calculations further reveal that sulfur vacancies enhance the kinetics of oxygen evolution, oxygen adsorption capacity, and the efficiency of singlet oxygen ( 1 O 2 ) generation, reducing the activation barriers throughout the oxygen activation cascade. Combined electron paramagnetic resonance spectroscopy and radical quenching experiments confirm 1 O 2 as the dominant reactive oxygen species responsible for PFOA degradation, operating via a non-hydroxyl radical mechanism. The catalyst achieves over 93% degradation efficiency for 50 µg L −1 PFOA in surface water and aquaculture wastewater, demonstrating the application potential of sulfur vacancy-engineered photocatalytic systems for the effective remediation of trace emerging contaminants in actual environments.
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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污染物降解
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高影响因子
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