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Cucurbit[8]uril-regulated face-to-face dimerization assembly enhanced photosensitization and photocatalysis

Science China Chemistry 2024年第5期67卷 1605-1612页

作者： Haigen Nie Die Hu Zhiyao Zeng Yan Fan Yaxin Zhai Xin-Long Ni Key Laboratory of Chemical Biology and Traditional Chinese Medicine Ministry of Educational of ChinaKey Laboratory of the Assembly and Application of Organic Functional Molecules of Hunan ProvinceCollege of Chemistry and Chemical EngineeringHunan Normal UniversityChangsha 410081China Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education Department of PhysicsHunan Normal UniversityChangsha 410081China

In water, N,N′-diarylpyridinium thiazolo[5,4-d]thiazole guests(G1–G3) were encapsulated by cucurbit[8]uril(Q[8]) to construct Q[8]_(3)/G_(2) complexes, in which the encapsulated G molecules exist as an exact face-to-face dimer. These complexation behaviors have been indicated by proton nuclear magnetic resonance(~1H NMR) spectroscopy and isothermal titration calorimetry(ITC),and have been confirmed by X-ray single crystal structural analysis of Q[8]_(3)/G2_(2). While free guests G1–G3 have no ability to sensitize singlet oxygen, they all become effective singlet oxygen sensitizers when complexed with Q[8]. By irradiation of white light, Q[8]_(3)/G_(2) complexes induced selective oxidation of aryl sulfide to aryl sulfoxide in good yields and selective oxidation of dimethyl sulfide(DMS) to dimethyl sulfoxide(DMSO) in excellent yields without over-oxidation to dimethyl sulfone(DMSO_(2))even for elongated irradiation. High-yield photo-oxidation of DMS to DMSO_(2) was only achieved by irradiation of blue light in the presence of Q[8]_(3)/G1_(2), which was also effective in photobleaching of Rhodamine B in water. The higher photo-oxidation power of Q[8]_(3)/G1_(2) has been ascribed to an additional generation of reactive oxygen species besides singlet oxygen.

关键词： host-guest interaction dimerization macrocycles photosensitization

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Improving photosensitization for photochemical CO2-to-CO conversion

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National Science Review 2020年第9期7卷 1459-1467页

作者： Ping Wang Ru Dong Song Guo Jianzhang Zhao Zhi-Ming Zhang Tong-Bu Lu MOE International Joint Laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and EngineeringTianjin University of Technology State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology

Inspired by nature, improving photosensitization represents a vital direction for the development of artificial photosynthesis. The sensitization ability of photosensitizers(PSs) reflects in their electron-transfer ability, which highly depends on their excited-state lifetime and redox potential. Herein, for the first time,we put forward a facile strategy to improve sensitizing ability via finely tuning the excited state of Ru(Ⅱ)-PSs(Ru-1–Ru-4) for efficient CO2reduction. Remarkably, [Ru(Phen)2(3-pyrenyl Phen)]2+(Ru-3) exhibits the best sensitizing ability among Ru-1–Ru-4, over 17 times higher than that of typical Ru(Phen)32+. It can efficiently sensitize a dinuclear cobalt catalyst for CO2-to-CO conversion with a maximum turnover number of 66 480. Systematic investigations demonstrate that its long-lived excited state and suitable redox driving force greatly contributed to this superior sensitizing ability. This work provides a new insight into dramatically boosting photocatalytic CO2reduction via improving photosensitization.

关键词： photosensitization photocatalysis CO2 reduction excited state Ru(II) complexes

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Construction of FRET-based metallacycles with efficient photosensitization efficiency and photocatalytic activity

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Chinese Chemical Letters 2023年第1期34卷 304-309页

作者： Peipei Jia Yixiong Hu Zhiyong Zeng Yute Wang Bo Song Yanrong Jiang Haitao Sun Ming Wang Wenwei Qiu Lin Xu Shanghai Key Laboratory of Green Chemistry and Chemical Processes Shanghai Frontiers Science Center of Molecule Intelligent SynthesesShanghai Engineering Research Center of Molecular Therapeutics and New Drug DevelopmentSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China State Key Laboratory of Precision Spectroscopy East China Normal UniversityShanghai 200241China Institute of Eco-Chongming Shanghai 202162China

The fabrication of highly effective photosensitizers has received considerable attention because of their attractive functions and applications in the fields of photodynamic therapy, photosynthesis, photocatalysis, etc. Thus, it is highly desirable to develop a new approach to enhance photosensitization ***, through coordination-driven self-assembly, a series of metallacycles with efficient fluorescence resonance energy transfer(FRET) were effectively constructed, which displayed higher photosensitization efficiency and photocatalytic activity than their model metallacycles without FRET due to broadband absorption and singlet energy transfer from the energy acceptor to the energy donor. Moreover, iodization of fluorophores induced a significant enhancement of the photosensitization efficiency and photocatalytic activity of the metallacycles. This research provides an efficient strategy for improving photosensitization efficiency and a promising platform for the preparation of effective photosensitizers and photocatalysts.

关键词： Self-assembly Metallacycle FRET photosensitization Photocatalytic

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INQUIRY OF photosensitization MECHANISM OF YANGZHOU HEMATOPORPHYRIN DERIVATIVE(YHPD)

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Science China Chemistry 1992年第1期35卷 39-49页

作者：张志义陶能兵何润根 Institute of Biophysics Academia Sinica Beijing 100080 PRC

By the use of the advanced ESR technique and through comparing with BHPD, the characteristic of YHPD photosensitization is discussed in this paper in the respect of the primary process of photosensitization. The experiment results showed: （ⅰ） not only 1O2, but also free radicals（O2· OH and YHPD）can be formed by the aid of YHPD; and （ⅱ） as to the ability of producing 1O2, YHPD2 and-OH, YHPD>BHPD. Two points are indicated: first, the photosensitized damage of YHPD is interrelated to not only 1O2, but also free radicals （O2. OH and YHPD）; second, although the photosensitized damage of YHPD is stronger than that of BHPD, yet the photosensitized damage is negatively correlated to the yield of 1O2 but positively correlated to those of O2 and OH. Based on these two points, it is suggested that activated oxygen free radicals（O2 and. OH） instead of 1O2 play the main role as instantaneously activated material in the photosensitized damage of YHPD.

关键词： Yangzhou hematoporphyrin derivative (YHPD) Beijing hematoporphyrin derivative (BHPD) photosensitization primary process ESR.

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CHARACTERISTICS OF THE PRIMARY REACTION OF HYPOCRELLIN A photosensitization

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Science China Chemistry 1989年第9期32卷 1063-1071页

作者：张志义臧伦义徐国瑞陶能兵王大辉 Institute of Biophysics Academia Sinica Beijing

The primary reaction of photosensitization of Hypocrellin A （HA） has been studied byusing techniques of ESR, spin-trapping and spin-counteraction. The experiments show thatHA is able to generate not only 1O2,but also O2-·OH and HA- which are observed for thefirst time. The conversion of generating active oxygen into generating nonoxygen free rad-ical is confirmed as well. Based on the characteristics of the primary reaction which gene-rates these active substances （transient products）, it is proposed that the photosensitized dam-age for the biological system by HA is probably related to not only 1O2 itself, but also amultiple effect from 1O2 as well as O2-,·OH and HA+ free radical.

关键词： hypocrellin A photosensitization primary reaction ESR

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Double-Stranded DNA Matrix for photosensitization Switching

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CCS Chemistry 2021年第9期3卷 2394-2404页

作者： Yanying Wang Hao Hu Tianyu Dong Hayam Mansour Xinfeng Zhang Feng Li Peng Wu Key Laboratory of Green Chemistry and Technology Ministry of EducationCollege of ChemistrySichuan UniversityChengdu 610064 Analytical and Testing Center Sichuan UniversityChengdu 610064 Department of Chemistry Brock UniversitySt.CatharinesON L2S 3A1 Department of Cell Biology National Research CentreCairo 12622 College of Materials and Chemistry&Chemical Engineering Chengdu University of TechnologyChengdu 610059

photosensitization,originated from the activation of triplet states,is the basis of many photodynamic applications,but often competes with a series of nonradiative ***,we communicate a new function of double-stranded DNA(dsDNA)for label-free photosensitization *** to∼70-fold singlet oxygen generation boosting was observed for SYBR Green I(SG)upon binding with *** photophysical and theoretical studies have revealed the role of dsDNA as a matrix,which could efficiently suppress the nonradiative transitions of SG.

关键词： photosensitization DNA singlet oxygen nucleic acid testing SYBR Green I

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Characteristics of photosensitization of Pheophorbide a in liposomal media

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Science China(Life Sciences) 1999年第5期42卷 471-480页

作者：杨红英李美芬张文庚赵红霞张志义 Institute of Biophysics Chinese Academy of Sciences 100101 Beijing China

Pheophorbide a （PPa）, a decomposition product of chlorophyll a, is a photosensitizer. The photosensitization mechanisms （Type Ⅰ and Type Ⅱ） of PPa in simple buffer solutions and in buffer solutions containing double-layered DPPC liposomes have been studied using techniques of ESR, spin-trapping, spin-counteraction and laser flash photolysis. The results showed that adding DPPC liposomes to the buffer solution caused an increase of efficiency of generating 1O2 and PPa- by photoactivating PPa. The increase could be ascribed to the disaggregation of hydrophobic PPa caused by the addition of liposomes and the protective effect of liposomal media on the triplet state of PPa. It is concluded that the photosensitization of PPa in liposomal systems is different from that in simple aqueous solutions, and shows higher efficacy. The results will be useful to elucidating the mechanisms of photodynamic therapy of cancer.

关键词： Pheophorbide a (PPa) liposome photosensitization active oxygen free radicals spin trapping spin counteraction laser flash photolysis.

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Studying dynamic process of photosensitization by ESR method

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Science China(Life Sciences) 1997年第4期40卷 356-362页

作者：张红雨赵红霞张志义 Institute of Biophysics Chinese Academy of Sciences Beijing 100101 China

By kinetic methods, functional relation of TAN radical, produced in the process of TEMPONE trapping O2, vs. time during photosensitization was established. Accordingly relative rate constants of generating all kinds of active intermediates through types I and II mechanism of photosensitization can be calculated. Using the formula and experimental results, the relative rate constants of generating O2, O2 and PS2 of three kinds of perylenequinone photosensitizer: HA, HB and CP in DMF-H20 and DMSO-H2O system were calculated, and then the structure-activity relationship of perylenequinone photosensitizer and the relation between photosensitivity and solvent was studied.

关键词： photosensitization type I and type Ⅱ mechanism dynamic process perylenequinone photosensitizer ESR.

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Proton leakage is the mechanism for hematoporphyrin photosensitization-promoted inactivation of rat liver mitochondria

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Progress in Natural Science:Materials International 1995年第4期

作者：周同庆焦选茂魏影允刘树森冯伟华缪明永 Beijing 100080 China Chinese Academy of Sciences Dpartment of Biocbemistry Institute of Zoology State Key Laboratory of Biomembrane and Membrane Biotechnology The Second Military University of Medical Science Shanghai 200433

The effects of hematoporphyrin photosensitization on the energy-transducing functions of isolated rat liver mitochondria have been studied. By using the measurements of the illumination time-and hematoporphyrin concentration-dependent variations of bioenergetical parameters of mitochondria, it is shown clearly that the photosensitization-promoted proton leakage of inner mitochondrial membrane, together with the resultant dissipation of proton electrochemical gradient, is the mechanism leading to the impairment of oxidative phosphorylation of mitochondria.

关键词： hematoporphyrin photosensitization mitochondria singlet oxygen proton leakage.

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Wavelength-sensitive photocatalytic H2 evolution from H2S splitting over g-C3N4 with S,N-codoped carbon dots as the photosensitizer

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Journal of Energy Chemistry 2021年第1期30卷 234-242,I0008页

作者： Zhanghui Xie Shan Yu Xiang-Bing Fan Shiqian Wei Limei Yu Yunqian Zhong Xue-Wang Gao Fan Wu Ying Zhou State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation Southwest Petroleum UniversityChengdu 610500SichuanChina The Center of New Energy Materials and Technology School of New Energy and MaterialsSouthwest Petroleum UniversityChengdu 610500SichuanChina Department of Engineering University of CambridgeCambridge CB30FAUnited Kingdom College of Chemistry Leshan Normal UniversityLeshan 614000SichuanChina Technical Institute of Physics and Chemistry Chinese Academy of SciencesBeijing 100190China

Photocatalytic splitting of hydrogen sulfide(H2S) for hydrogen evolution is a promising method to solve the energy and environmental *** this work,S,N-codoped carbon dots(S,N-CDs)/graphitic carbon nitride(g-C3N4) nanosheet is synthesized by hydrothermal method as an efficient photocatalyst for the decomposition of *** addition to the characterization of the morphology and structure,chemical state,optical and electrochemical performances of S,N-CDs/g-C3N4,hydrogen evolution tests show that the activity of g-C3N4 is improved by introducing S,N-CDs,and the enhancement depends strongly on the wavelength of incident *** photocatalytic hydrogen production rate of S,N-CDs/g-C3N4 composite reaches 832 μmol g-1h-1, which is 38 times to that of g-C3N4 under irradiation at 460 *** functional theory calculations and electron paramagnetic resonance as well as photoluminescence technologies have altogether authenticated that the unique wavelength-dependent photosensitization of S,N-CDs on g-C3N4;meanwhile,a good match between the energy level of S,N-CDs and g-C3N4 is pivotal for the effective photocatalytic *** work has unveiled the detailed mechanism of the photocatalytic activity enhancement in S,N-CDs/g-C3N4 composite and showed its potential in photocatalytic splitting of H2S for hydrogen evolution.

关键词： photosensitization S N-codoped carbon dots Hydrogen sulfide splitting Photocatalytic hydrogen evolution

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