TRANSACTIONS OF TIANJIN UNIVERSITY
·
2021
·Vol. 28
·期 1
·73-79
·
IF 0
Tian Pengfei,Su Jianjun,Song Yun,Ye Ruquan,Zhu Minghui
Great attention has been paid to cofacial porphyrins due to their many unique advantages over their monomeric analogs. However, their synthesis is usually complicated. In this work, a facile impregnation method for preparing heterogenized, cofacially stacked porphyrins is proposed. An anionic porphyrin is introduced as an underlayer for immobilization of cationic cobalt porphyrin via electrostatic force. The metal center of the underlying molecule contributes to the electronic structure of the upper cationic cobalt porphyrin. Screening reveals the anionic iron porphyrin to be the most efficient underlayer molecule, lowering the activation energy barrier of CO 2 electroreduction, with an improved turnover frequency by 74% to 8.0 s −1 at − 0.6 V versus RHE.
研究领域:
化学
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材料科学
·
催化
✓ 已验证
DOI
ENERGY & FUELS
·
2021
·
IF 3.605
Xuechun Ding,Shengchao Wei,He Bian,Lijun Zhu,Daohong Xia
Despite the studies on asphaltene aggregation throughout few decades, the formation of asphaltene aggregates and subsequent deposition are still the biggest challenges in the oil industry. Especially, the role of porphyrins existing in oil naturally on asphaltene aggregation is not completely understood due to asphaltene’s and porphyrin’s special structures. Herein, we investigated the influence of tetraphenylporphyrin (TPP), nickel tetraphenylporphyrin (NiTPP), and vanadium tetraphenylporphyrin (VOTPP) on asphaltene aggregation by a multiscale approach, which provides an in-depth understanding of the role of porphyrins on asphaltene aggregation. UV–vis spectroscopy and fluorescence spectroscopy were performed to examine the self-aggregation of TPP, NiTPP, and VOTPP and the influence of porphyrins on the aggregation of asphaltene. The changes of stacking structures, microscopic structures, and particle size distributions of co-aggregates of asphaltenes with porphyrins were analyzed in detail via X-ray diffraction, inverted fluorescence microscopy, and granulometric distribution, respectively. The characterization results indicated that the aggregation ability of the porphyrins (TPP, NiTPP, and VOTPP) was stronger than that of asphaltene and porphyrins can promote the aggregation of asphaltene, which leads to the increase of the average aromatic sheet number, aggregation morphology, and particle size of asphaltene aggregates. Based on experimental analysis, the possible mechanism by which porphyrins promoted asphaltene aggregation was elucidated. This research provided new insights into the aggregation and disaggregation of asphaltenes.
研究领域:
石油化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2021
·
IF 3.512
Yun Wang,Min Gong,Zhuo Huang,Hai Min,Peng Yu,Fuzhou Tang,Yuannong Ye,Simian Zhu,Zuquan Hu,Zhu Zeng,Jin Chen
Hematoporphyrin (HP) and protoporphyrin IX (PPIX) are useful porphyrin photosensitizers with significant application values in photodynamic therapy. Currently, many strategies have been developed to improve their clinical performance, such as incorporating them with nanoparticle (NP) carriers. In this work, we studied the possibility of using β-lactoglobulin (BLG) as a potential NP carrier due to their hydrophobic affinity, pH sensitivity, and low cost of extraction and preservation. The interaction mechanisms of BLG with HP and PPIX were investigated using spectroscopic techniques and molecular docking methods. The molecular docking results agree well with the experimental results, which demonstrate that the formations of HP-BLG and PPIX-BLG complexes are endothermic processes and the main acting force is hydrophobic force. Furthermore, the opening–closure states of EF loop have a great influence on the HP-BLG complex formation, where the central hydrophobic cavity of β-barrel is available for HP binding at pH 7.4 but not available at pH 6.2. However, the formation of the PPIX-BLG complex is less dependent on the states of the EF loop, and the binding sites of PPIX are both located on the external surface of BLG under both pH 7.4 and 6.2 conditions. All of our results would provide new insight into the mechanisms of noncovalent interactions between BLG and HP/PPIX. It is believed that this work indicated the potential application values of BLG in designing pH-sensitive carriers for the delivery of HP and PPIX, as well as other poorly soluble drugs.
研究领域:
生物化学
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药物递送
·
光动力治疗
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
·
2022
·
IF 4.01
Chenxi Liu,Minghui Chen,Hongrui Li,Quan Shi,Yaqing Feng,Bao Zhang
Unique features, including a high specific surface area, great stability, and crystallinity, make covalent organic frameworks (COFs) intriguing sorbents and catalysts in light-driven water pollutant degradation. Inspired by the light absorption capability of porphyrin derivatives and the carrier separation ability of a donor–acceptor (D–A) configuration, we constructed two-dimensional porphyrin donor-based D–A COFs: COF-HTBD involving only tetrahydroporphyrins and COF-HMTBD (M = Co, Fe, Cu) involving both tetrahydro- and metalloporphyrins via a mixed porphyrin monomer strategy. The monomer 2,1,3-benzothiadiazole-4,7-dicarboxaldehyde (BD) is incorporated as an electron accepting moiety. Interestingly, COF-HTBD, COF-HCuTBD, and COF- HFeTBD exhibit staggered stacking, while the stacking model of COF-HCoTBD transforms from staggered to eclipsed. Notably, COF-HFeTBD demonstrates excellent activities and stabilities toward visible light-driven photocatalytic rhodamine B (RhB) degradation in aqueous solutions with H2O2 present (100% removal in 3 h). Overall, this work provides an interesting strategy for the construction of D–A-type porphyrin COFs for dye pollutant removal.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Meng Kou,Feng Qin,Yongda Wang,Xiyu Zhang,Hua Zhao,Ye Tian,Zhiguo Zhang
The presence of room temperature phosphorescence emission in metalloporphyrin, via the transition from the excited triplet state (T1) to the ground state (S0), relies on the chelated heavy metal ions, which is known as the heavy atom effect (HAE). Despite the HAE being a reliable method to tune the phosphorescence process widely, the realization of the HAE nature is a tough task as the induced phosphorescence process is sensitive to not only the specie of bonded heavy atoms but also chemical environments such as the oxygen quenching and solvent effect. In this study, we have aimed at a quantitative determination of the intrinsic phosphorescent transition rate (kP) in metalloporphyrin gadolinium-labeled hematoporphyrin monomethyl ether (Gd-HMME). After the theoretical analysis based on the rate equation model to remove the nonintrinsic contribution and the experimental results of phosphorescence, the kP is calculated to be ∼2.4 × 10–4 μs–1. This study enables us to approach the intrinsic energy characteristic of metalloporphyrins; moreover, our work provides an effective pathway for the further optimization of the varied functional metalloporphyrin.
研究领域:
化学
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材料科学
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF PORPHYRINS AND PHTHALOCYANINES
·
2017
·Vol. 21
·期 10
·665-670
·
IF 1.043
Jianyu Hua,Lixin Zang,Huimin Zhao,Ting Liu,Ming Fan,Tong Chen,Zhengyu Cao,Ye Tian,Zhiguo Zhang
This paper studies the origin of fluorescence emissions of metalloporphyrins. The absorption spectrum of neodymium-coordinated hematoporphyrin monomethyl ether (Nd-HMME) was found to have four Q bands, which is different from the accepted knowledge (two Q bands). The absorbance of Nd-HMME was comparable to the corresponding absorbance of HMME at wavelengths of 538 nm and 572 nm, but the absorbance of Nd-HMME at wavelengths of 502 nm and 622 nm was approximately 1/30 of that at 572 nm. The doping of Nd 3+ enhanced the symmetry of HMME, and led to changes in energy level properties. Moreover, Nd-HMME still exhibited two fluorescence peaks at 624 nm and 686 nm, similar to HMME, which can be explained by the observation of a weak absorption peak of Nd-HMME at 622 nm.
研究领域:
化学
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光谱学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
OPTICS EXPRESS
·
2025
·Vol. 33
·期 11
·22185-22195
·
IF 3.3
Lu Li,Feng Qin,Zhiguo Zhang,Zhiguo Zhang,Tao Jia
The determination of the energy of the lowest triplet excited state (ET1) for metalloporphyrin photosensitizers, a key parameter for rationalizing energy transfer processes in metalloporphyrins, facilitates a better understanding and optimization of their functionality. In this study, a strategy was proposed for determining the ET1 values in metalloporphyrin systems by analyzing the temperature dependence of the oxygen quenching rate constant using time-resolved spectroscopy, with Platinum(II) octaethylporphyrin (PtOEP) and Palladium(II) octaethylporphyrin (PdOEP) as representative examples. Through a thermal equilibrium approximation of the excited triplet state (T1) and the excited state of oxygen, a theoretical model was introduced in which the oxygen quenching rate exhibits a nonlinear dependence on temperature, enabling the determination of ET1 values. Additionally, the validity of this approach was demonstrated through excitation spectra of metalloporphyrins. Our work provides an effective pathway and offers new insights into the energy-loss mechanisms involved in related photoconversion processes.
研究领域:
物理化学
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光化学
·
光谱学
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材料科学
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分子物理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Huimin Zhao,Lixin Zang,Jianyu Hua,Bo Yuan,Qinyu Liu,Bingjie Ma,Chengshan Guo
A temperature-sensing method immune to oxygen interference is established based on phosphorescent metalloporphyrins on regenerated cellulose (RC). A series of metalloporphyrins (hematoporphyrin monomethyl ether coordinated to Pd, Gd, and Lu ions: Pd-, Gd-, and Lu-HMME) are designed to be embedded in RC. The phosphorescence emissions of these metalloporphyrins are effectively enhanced on RC, affording phosphorescence quantum yields of 1.8%, 3.3%, and 2.2%, respectively. The phosphorescence emissions of these metalloporphyrins on RC (metalloporphyrins/RC) are independent of oxygen concentration because RC provides an oxygen-impermeable microenvironment. Meanwhile, the phosphorescence emissions are effectively quenched with increasing temperature. The phosphorescence lifetimes also decrease with temperature, indicating an increase in non-radiative relaxation, which weakens phosphorescence emission. The oxygen-independence and temperature-dependence of these metalloporphyrins/RC reveal that they could serve as promising anti-oxygen-interference temperature indicators. Temperature-response plots are obtained in the range from −75 to 50 °C. The temperature sensitivities of Pd-, Gd-, and Lu-HMME on RC are evaluated to be 0.50, 0.28, and 0.36%/°C based on the temperature-response plots. The temperature resolution values of Pd-, Gd-, and Lu-HMME on RC are 0.5, 1.3, and 1.2 °C. These temperature indicators have high photostability under extended irradiation, making them suitable for practical use. The method offers attractive new insights into phosphorescent temperature-sensing materials and the development of oxygen sensors with temperature compensation.
研究领域:
材料科学
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光学传感
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温度传感
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磷光材料
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jiajing Zhang,Suwei Wang,Pin Song,Ang Li,Wei Jiang,Jun Di
The insufficient solar light response ability of the photocatalyst, rapid recombination of interface charges, and lack of active sites significantly inhibit the efficiency of photocatalytic CO 2 reduction. Addressing these challenges simultaneously is a very challenging task. Herein, an interface engineering coupled surface polarization strategy is proposed to optimize the CO 2 photoreduction performance. The copper tetracarboxyphenylporphyrin (CuTCPP) modified BiOBr/Bi 19 S 27 Br 3 (BBS) heterostructure was developed. The built-in electric field formed between BiOBr and Bi 19 S 27 Br 3 interfaces induces the effective interfacial charge separation, while the surface polarization of CuTCPP induces the transfer of electrons from the conduction band (CB) of BBS to the CB of CuTCPP. Benefiting from this unique configuration and abundant active sites in CuTCPP, greatly improved photocatalytic CO 2 reduction performance can be realized. Without adding cocatalysts and sacrificial agents, the optimized CO generation performance of CuTCPP-BiOBr/Bi 19 S 27 Br 3 (BBS-CT) is 3.5 times higher than that of BBS. This work provides valuable insights of interface engineering coupled surface polarization strategy for collaborative improve the photocatalytic CO 2 reduction performance.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2024
·
IF 15.8
Ying Tang,Yongdan Qi,Yang Chen,Yu-Qiang Wang,Cheng Zhang,Yunxia Sun,Cui Huang,Xian-Zheng Zhang
Porphyromonas gingivalis has been demonstrated to have the strongest association with periodontitis. Within the host, P. gingivalis relies on acquiring iron and heme through the aggregation and lysis of erythrocytes, which are important factors in the growth and virulence of P. gingivalis. Additionally, the excess obtained heme is deposited on the surface of P. gingivalis, protecting the cells from oxidative damage. Based on these biological properties of the interaction between P. gingivalis and erythrocytes, this study developed an erythrocyte membrane nanovesicle loaded with gallium porphyrins to mimic erythrocytes. The nanovesicle can target and adhere with P. gingivalis precisely, being lysed and utilized by P. gingivalis as erythrocytes. Ingested gallium porphyrin replaces iron porphyrin in P. gingivalis, causing intracellular metabolic disruption. Deposited porphyrin generates a large amount of reactive oxygen species (ROS) under blue light, causing oxidative damage, and its lethality is enhanced by bacterial metabolic disruption, synergistically killing P. gingivalis. Our results demonstrate that this strategy can target and inhibit P. gingivalis, reduce its invasion of epithelial cells, and alleviate the progression of periodontitis.
研究领域:
牙科学
·
纳米技术
·
微生物学
·
药学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2015
·
IF 2.037
Chunlin Li,Qinbo Wang,Binwei Shen,Zhenhua Xiong,Chuxiong Chen
The mole fraction solubilities of 5,10,15,20-tetraphenylporphyrin (TPP) and 5,10,15,20-tetra(p-chlorophenyl)porphyrin (p-ClTPP) in binary system N,N-dimethylformamide (DMF) + water solvent mixtures were measured at atmospheric pressure by using the static method. The temperature and effects of mole fraction of DMF in the solvent mixtures on solubility were studied. The results show that the solubilities of TPP and p-ClTPP increase with the increasing temperature for a certain solvent composition, and the solubilities show a maximum in pure DMF, then the solubilities decrease when the water was added to the system. The experimental data were correlated with modified Apelblat equation. The solubilities calculated by the model were in good agreement with experimental observations. Thermodynamic parameters such as dissolution enthalpy, isobaric heat capacity and Gibbs energy were obtained from the solubility data by using the Clark–Glew equation together with the modified Apelblat equation. The result demonstrated that the dissolving process of TPP and p-ClTPP in DMF + water solvent mixtures is endothermic and not spontaneous.
研究领域:
化学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 3
·1459
·
IF 4.6
Xinying Zhang,Xialing Hou,Decheng Lu,Yingying Chen,Lingyan Feng
Porphyrin (TMPyP) functionalized carbon quantum dots (CQDs-TMPyP), a novel and efficient carbon nanocomposite material, were developed as a novel luminescent material, which could be very useful for the sensitive detection of copper ions in the Cu2+quenching luminescence of functionalized carbon quantum dots. Therefore, we constructed a sensitive “signal off” ECL biosensor for the detection of Cu2+. This sensor can sensitively respond to copper ions in the range of 10 nM to 10 μM, and the detection limit is 2.78 nM. At the same time, it has good selectivity and stability and a benign response in complex systems. With excellent properties, this proposed ECL biosensor provides an efficient and ultrasensitive method for Cu2+detection.Keywords:carbon quantum dots;porphyrin;electrochemiluminescence;Cu2+detection
研究领域:
分析化学
·
纳米材料
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）