ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yan Gu,Tiefeng Xu,Zhexin Zhu,Xiufang Chen,Wenxing Chen,Wangyang Lu
The local coordination structure of metal atoms in single-atom catalysts (SACs) greatly influences their catalytic performance. And for most SACs, single metal atoms were anchored on carbon materials with N or C coordination. However, the rational design of oxygen-containing SACs and analyzing its structure–performance relationship remain challenging. Herein, we used amino-rich compounds to tailor the metatungstate and fix the W atoms and finally obtained the oxygen-containing W-SACs. The structural evolution of tungsten and its coordination atoms were tracked by electrospray ionization high-definition mass spectrometry. Furthermore, aberration-corrected transmission electron microscopy, X-ray absorption fine-structure spectroscopy, and first-principles calculation results revealed that different from the traditional SACs, the WO2N2 moiety (W coordinated with two O atoms and two N atoms) may be the favored structure for W species. This special structure promoted the energy transfer for enhancing singlet oxygen generation. This work presents an efficient way to prepare more high-efficiency SACs by atomic-scale tailoring and structural evolution tracking at the molecular level.
研究领域:
催化化学
·
材料科学
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DYES AND PIGMENTS
·
2025
·
IF 4.2
Meng-yan Chai,Thayalan Rajeshkumar,Hui Su,Fu-jie Zhao,Zhi Wang,Wei-ping Yin,Song Jiang,Guo-xing Liu,Li-jie Liu,Xin Zheng,Li-xia Xie,Sheng-qiang Guo,Yu-qiang Xiang,Laurent Maron,Cao-yuan Niu
The poor aqueous solubility of porphyrins and metalloporphyrins has long impeded their applications in biological systems. In this study, we report the synthesis of a novel porphyrin derivative—ZnTSPP—achieved by introducing four sulfonic acid groups onto a single porphyrin molecule. The photophysical properties were comprehensively characterized via UV–Vis absorption and fluorescence emission spectroscopy in deionized water, phosphate-buffered saline (PBS), and fetal bovine serum (FBS). ZnTSPP exhibits intense absorption in both the Soret and Q bands and displays a reversible pH response. Density Functional Theory (DFT) calculations further corroborate the pH-dependent formation of J- and H-aggregates. Additionally, cellular imaging studies performed on pig kidney epithelial cells (LLC-PK1) demonstrate that ZnTSPP is not only pH-responsive but also an efficient singlet oxygen generator. These attributes position ZnTSPP as a promising agent for biomedical imaging and photodynamic therapy.
研究领域:
生物化学
·
分子生物学
·
医学影像学
✓ 已验证
DOI
高影响因子
CHEMICAL PHYSICS
·
2024
·
IF 2
Lu Li,Feng Qin,Yongda Wang,Zhiguo Zhang
The proportion of singlet oxygen ( R ) produced from the triplet state of porphyrin in aqueous solutions was investigated by substituting porphyrin molecules with the metalloporphyrin Platinum(II) meso -tetraphenylporphyrin (Pt-TPP). The feasibility of using platinum porphyrin as a substitute for porphyrin to study the photophysical properties in photodynamic therapy (PDT) was confirmed. The model of first-order decay in a water-methanol mixed solution encompasses potential deactivation processes of the excited triplet states and was built, which was confirmed by monitoring the change in the total transition rate of the T 1 state ( A 0 ) value at different water contents under anoxic environments, obtained through measuring the phosphorescence lifetime ( τ p ) of Pt-TPP. Combined with A 0 and the quenching rate constant of T 1 by O 2 ( k q ), the formula for R in relation to changes in oxygen can be deduced in pure water.
研究领域:
生物化学
·
医学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Ting Zhang,Yaobin Ding,Heqing Tang
An efficient singlet oxygen generation system was first developed by using Bi(V)/Bi(III) composites for degrading organic pollutants . The composites were prepared by hydrolyzing NaBiO 3 in HCl solutions. As monitored by various techniques, it was found that the morphology and composition of the composites were able to be tuned by changing the molar ratio of HCl to NaBiO 3 in the preparation process, which was optimized at 2.0. Due to the efficient generation of singlet oxygen, the use of the composite (0.75 g L −1 ) resulted in almost complete degradation of bisphenol A (0.2 mmol L −1 ) in 20 min, with a pseudo-first-order kinetic constant of 0.14 min −1 . The dominant reactive species in the degradation system were confirmed to be singlet oxygen, which was generated from the release of the lattice oxygen in the composite. The good performances of the concerned singlet oxygen generation system are general for degrading different organic pollutants.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 12
·8913-8920
·
IF 3.3
Zhen Chi,Jia Xu,Shida Luo,Xia Ran,Xiaojuan Wang,Pingan Liu,Yulu He,Yanmin Kuang,Lijun Guo
Triplet energy transfer (TET) from semiconductor quantum dots (QDs) to molecular triplets has potential applications in photon up-conversion and singlet oxygen generation. Here, we have constructed a complex consisting of CdTe QDs as the donor and 9-anthracenecarboxylic acid (ACA) as the triplet acceptor, and studied the TET pathways and enhanced singlet oxygen generation properties. The results from steady-state and time-resolved spectroscopy demonstrate efficient TET with a total efficiency of over 80% from photoexcited CdTe QDs to ACA. Dynamical analysis clearly indicates two distinctive TET channels – hot electron exchange and thermalized electron exchange – mediating the TET process in the CdTe QDs–ACA complex. The TET efficiencies from hot electron exchange at high energetic levels and thermalized electron exchange on the lowest exciton state can reach ∼27% and ∼85%, respectively, following 530 nm excitation. This efficient TET endows the CdTe QDs–ACA complex with a good capability of generating singlet oxygen species with a yield of up to ∼59%. These findings contribute further insights to the mechanisms of interfacial TET processes and are significant in designing efficient TET systems based on semiconductor nanoparticles and triplet molecules.
研究领域:
材料科学
·
光化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Environmental Science-Nano
·
2023
·Vol. 10
·期 5
·1428-1440
·
IF 7.3
Xixi Chen,Yanjun Li,Wanyi Fu,Shuanghong Tian,Yulong Yang,Kai Yang,Xuanbo Xu,Xihui Zhang
The importance of nonradical Fenton-like catalysis in environmental fields has motivated research for effective singlet oxygen (1O2) production, but realizing the accurate design and regulation of active sites for manipulating oriented 1O2 generation is still highly challenging. In this study, α-, β-, and γ-MnO2 catalysts with different oxygen vacancy (OV) abundance were fabricated to activate H2O2 to generate 1O2 for the degradation of oxytetracycline (OTC). The OV-rich α-MnO2 had a high OTC removal efficiency (>93.5%) at the pH range from 4.0 to 11.0. Moreover, α-MnO2 exhibited great applicability for a real water matrix, and the total removal of various kinds of emerging contaminants from hospital wastewater reached up to 97.4%. The excellent performances of α-MnO2 were attributed to the rich contents of OVs that induced the oriented generation of 1O2. Theoretical density functional theory (DFT) calculations validated that the OV-rich α-MnO2 had the highest H2O2 adsorption ability (−1.39 eV) and the lowest energy barrier (0.41 eV) for the dissociation of *OH to form the *O intermediate, which promoted the oriented formation of 1O2. This work provides a strategy of manipulating the oriented generation of 1O2 towards water decontamination via regulating the abundance of oxygen vacancies in α-MnO2 nanocatalysts.
研究领域:
环境科学
·
催化化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
Small Methods
·
2021
·Vol. 5
·期 7
·2100423
·
IF 14.188
Mingzhe Shao,Dapeng Liu,Baolin Yan,Xilan Feng,Xiaojuan Zhang,Yu Zhang
Inorganic nanomaterials have attracted much attention as enzyme mimics because of simple and stable spatial conformation of those artificially synthesized nanocatalysts. Cu 2 O, as an important kind of narrow band gap semiconductor, is identified as effective as visible-light-driven photocatalysts, which can catalyze decomposition of H 2 O 2 into reactive oxygen species. Moreover, after forming Cu x O/CeO 2 hybrids, the strongly coupled interface between the two components will further improve their catalytic performance. In this paper, the authors try to construct FTO/TiO 2 /Cu x O/CeO 2 (1 < x < 2) nanohybrids with such a kind of active interface via a layer-by-layer electrodeposition strategy by aid of the following surface etching process. It is found that FTO/TiO 2 /Cu x O/CeO 2 exhibits good peroxidase mimic activity in the dark but much better performance under visible light irradiation (λ ≥ 420 nm) during catalytic oxidation of 3,3′,5,5′-tetramethylbenzidine substrates in the presence of H 2 O 2 . Detailed characterizations disclose that the construction of TiO 2 /Cu 2 O pn-heterojunctions do effectively accelerate separation of photogenerated carriers, and the formation of a highly active Cu x O/CeO 2 interface is synergistically favorable for selectively generating singlet oxygen to boost the catalytic performance of FTO/TiO 2 /Cu x O/CeO 2 .
研究领域:
材料科学
·
催化化学
·
纳米技术
✓ 已验证
DOI
PubMed
高影响因子
DYES AND PIGMENTS
·
2021
·
IF 4.889
Hao Liu,Juanjuan Yin,Enyun Xing,Yingying Du,Yu Su,Yaqing Feng,Shuxian Meng
Cyanine dyes are widely used in the field of tumor phototherapy due to their excellent photophysical properties. To explore the heavy atoms effects on the photothermal and photodynamic performance of phototherapeutic agents, chlorine, bromine, and iodine were introduced to synthesize a series of cyanine dyes (IR6, IR7, and IR8). We have found that all halogenated cyanine dyes exhibited high excitation wavelength (around 800 nm) and low dark toxicity. Among them, IR8 behaved the best singlet oxygen production ability in the three dyes. For photothermal performance, IR8 exhibited the best photothermal conversion rate (46.6%), photothermal stability, and excellent therapy efficiency (half-maximal inhibitory concentration, IC 50 = 16.2 μg/mL). IR7 behaved a greater enhancement of the photothermal conversion rate (43.4%) than IR6 (42.3%). In conclusion, the heavy atoms effects on the photothermal and photodynamic properties of cyanine dyes are positively correlated with the increase of the atomic number of the halogen atom, and the iodine atom may be the most worthy of consideration in the all halogen atoms.
研究领域:
肿瘤学
·
生物医学工程
·
药理学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Rui Zhang,Yan Guan,Zhiyan Zhu,Hongying Lv,Futian Li,Shuqing Sun,Juan Li
The tissue penetration depth of light and the singlet oxygen (1O2) generation efficiency of photosensitizers (PSs) are the two main factors that determine the effectiveness of photodynamic therapy for tumors. Herein, we report a novel strategy to prepare a multifunctional upconversion photosensitizer (UCPS) based on the host/guest nanoarchitecture. By a simple reprecipitation method, host/guest tetracene/pentacene nanorods (Tc/Pc NRs) were synthesized for enhancing triplet–triplet annihilation-upconversion (TTA-UC) or two-photon excited emission and 1O2 generation efficiency upon 650 or 808 nm excitation. Tc/Pc NRs had higher 1O2 quantum yield (74%) than Tc NRs (28%) upon 650 nm laser irradiation. The proposed mechanism is that doping Pc molecules into Tc NRs induces intermediate states between S0 and S1, shortening the energy gap for 1O2 generation and resulting in TTA-UC emission. Equally important, with 808 nm fs laser excitation, Tc/Pc NRs showed an enhanced 1O2 generation efficiency and two-photon absorption cross section (σ) compared with Tc NRs. In addition, when the tumors in mice were exposed to Tc/Pc NRs with 650 or 808 nm wavelength irradiation, the tumor inhibition rates achieved 99 and 95%, respectively. This work opens new perspectives for exploring novel nano-UCPSs for biomedical applications.
研究领域:
生物医学工程
·
纳米医学
·
肿瘤学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yuxuan Bai,Ganbing Zhang,Mingwang Liu,Shenghuai Hou,Shuang Zheng,Shu Yang,Chengzhou Zhu,Hui Xu
The electronic state modulation of catalytic active sites governs the oxidation/reduction activation pathway of peroxymonosulfate (PMS), however, directional singlet oxygen ( 1 O 2 ) generation via establishing electron-depleted active center remains challenging. Herein, we propose an innovative axial coordination strategy to engineer atomically dispersed Co-N x moieties on MXene substrates, creating a Co SA -N 2 O 1 /MXene catalyst with precisely modulated electron-depleted sites. The tailored electronic configuration redirects 2,4-dichlorophenol degradation from radical-dominated pathway (Co SA -N 4 counterpart without axial O modulation) to 1 O 2 -driven mechanism with 90.5% contribution, achieving up to 5.1-fold activity enhancement, even outperforming most state-of-the-art Fenton-like systems. The charge density redistribution and greater density of states near Fermi level accelerate PMS activation to selective generation of 1 O 2 . It also demonstrates exceptional environment robustness and high stability for treating real lake water. Our findings advance atomic-level insights into PMS activation and establish a novel paradigm of axial coordination engineering for designing next-generation single-atom catalysts.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic and Nano-Metal Chemistry
·
2019
·
IF 0.685
Xue-Wen Liu,Jie Huang,Yu-Xuan Tang,Song-Bai Zhang,Ji-Lin Lu
Two new ruthenium complexes containing a new polyaza ligand were found to inhibit the DNA supercoiled relaxation mediated by topoisomerase I (topo I), cleave DNA under irradiation and interact with CT-DNA by intercalation. Both complexes exhibited fast singlet oxygen generation rate, and DNA photocleavage reaction should be initiated by 1O2. Furthermore, complex 2 showed higher photocleavage activity, topo I inhibition activity, and DNA affinity than complex 1. This work shows that two complexes can act as DNA binders with high affinity and good DNA photocleavers. Furthermore, complex 2 can act as a good topo I inhibitor.
研究领域:
化学
·
分子生物学
·
药理学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2022
·
IF 3.841
Xiangjun Mu,Wanqing Zhang,Changqing Yi,Mei-Jin Li,Fengfu Fu
As a biological thiol closely related to the incidence of gastric cancer, homocysteine (Hcy) has been reported to be detected in vivo and in vitro . The design of ratiometric photoluminescent probes often relies on the unique chemical structure of the molecular. In this paper, we designed and synthesized three aldehyde-containing iridium(III) complexes and characterized their structure and photophysical properties. They showed a good specificity for Hcy detection. The color of the solution gradually changed from red to pale yellow. The photoluminescent variation from red to green was observed by the naked eye after addition of Hcy to the solution of the Ir1 ([(CHO-pba) 2 Ir(bpy-2NH 2 )]PF 6 ), Ir2 ([(CF 3 -pba) 2 Ir(bpy-2NH 2 )]PF 6 ) and Ir3 ([(CH 3 -pba) 2 Ir(bpy-2NH 2 )]PF 6 ) with a large blue shift by 120, 63 and 106 nm, respectively. Based on the differences in their structures, it could be inferred that this type of ratiometric photoluminescent probe based on iridium(III) complexes with aldehyde was related to the strong electron-donating effect of the nitrogen-containing substituents on the bipyridine ligand in the structure, and the introduction of electron-donating groups on the 4-(2-pyridinyl)benzaldehyde (pba) ligand can enlarge the blue shift of the photoluminescent wavelength upon sensing of Hcy. On the other hand, iridium(III) complexes are currently recognized as a third-generation good photodynamic therapy photosensitizer. The photodynamic therapy properties of the three iridium(III) complexes in this article have also been evaluated. All of them have strong singlet oxygen generation ability and low cytotoxicity which are expected to be used in photodynamic therapy and Hcy detection.
研究领域:
分析化学
·
生物化学
·
分子生物学
·
治疗学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）