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High-rate CH_(4)-to-C_(2)H_(6) photoconversion enabled by Au/ZnO porous nanosheets under oxygen-free system

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Science China chemistry 2024年第3期67卷 869-875页

作者： Kai Zheng Xiaojing Zhang Jun Hu Chengbin Xu Juncheng Zhu Jing Li Mingyu Wu Shan Zhu Li Li Shumin Wang Yumei Lv Xin He Ming Zuo Chengyuan Liu Yang Pan Junfa Zhu Yongfu Sun Yi Xie Hefei National laboratory for Physical Sciences at Microscale National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China key laboratory of photochemical conversion and optoelectronic materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China State Grid Anhui Electric Power Research institute Hefei 230601China

Photocatalytic CH_(4) coupling into high-valued C_(2)H_(6) is highly attractive,whereas the photosynthetic rate,especially under oxygen-free system,is still ***,we designed the negatively charged metal supported on metal oxide nanosheets to activate the inert C-H bond in CH_(4)and hence accelerate CH_(4) coupling *** an example,the synthetic Au/ZnO porous nanosheets exhibit the C_(2)H_(6) photosynthetic rate of 1,121.6μmol g^(-1)_(cat)h^(-1)and the CH_(4) conversion rate of 2,374.6μmol g^(-1)_(cat)h^(-1) under oxygen-free system,2 orders of magnitude higher than those of previously reported *** virtue of several in situ spectroscopic techniques,it is established that the generated Au^(δ-)and O^-species together polarized the C-H bond,while the Au^(δ-)and O^-species jointly stabilized the CH_(3) intermediates,which favored the coupling of CH_(3) intermediate to photosynthesize C_(2)H_(6) instead of overoxidation into CO_(x).Thus,the design of dual active species is beneficial for achieving high-efficient CH_(4)-to-C_(2)H_(6) photoconversion.

关键词： dual surface-active sites selective methane coupling ethane room temperature

Dangling Ligand Enables an Iron Hexa-Coordinated Molecular Catalyst for Water Oxidation by Photocatalysis

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CCS chemistry 2024年第3期6卷 623-630页

作者： Bing Yang Qi Liu Xiang-Zhu Wei Tao Lei Qing-Qing Yang Xu-Zhe Wang Jing-Xin Jian Xin Jiang Chen-Ho Tung Li-Zhu Wu key laboratory of photochemical conversion and optoelectronic materials New Cornerstone Science LaboratoryTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 School of Future Technology University of Chinese Academy of SciencesBeijing 100049

Photocatalytic water oxidation reaction by transition metal complexes remains a challenge because of their poor stability under irradiation,especially for earth-abundant metal *** this regard,ironbased water oxidation catalysts are prone to hydrolysis and/or dissociate the ligands to form nanoparticles under a real catalytic ***,we describe a unique hexa-coordinated catalyst 1[Fe^(II)(Py_(3)tacn)Cl_(2)]and its reference 2[Fe^(II)(PhPy_(2)tacn)Cl_(2)]with a dangling pyridyl ligand and a phenyl group,*** anticipated that the dynamically open and close coordination behaviors of the pyridyl ligand enabled balance of the reactivity and stability of catalyst *** our delight,the“open form”of catalyst 1 provided a free coordination site,and the“close form”guaranteed its molecular integrity,resulting in a water oxidation reaction with high efficiency and *** turnover number and turnover frequency values of 2332 and 60 s^(−1)are the highest known to date among iron-based homogeneous water oxidation systems under visible light irradiation.

关键词： water oxidation photocatalysis homogeneous catalysis iron complexes dangling ligand intermediates characterization

Trifluoromethyl enable high-performance single-emitter white organic light-emitting devices based on quinazoline acceptor

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Chinese Chemical Letters 2024年第4期35卷 442-446页

作者： Xiangan Song Shaogang Shen Mengyao Lu Ying Wang Yong Zhang School of materials Science and Engineering Harbin Institute of TechnologyHarbin 150001China key laboratory of photochemical conversion and optoelectronic materials and TIPC-CityU Joint Laboratory of Functional Materials and DeviceChinese Academy of SciencesTechnical Institute of Physics and ChemistryBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Single-emitter white organic light-emitting diode(WOLED) based on small organic molecule exhibits great potential in simplifying fabrication process of WOLEDs. However, the design and synthesis of molecule for highly efficient single-emitter WOLED still remains a challenge. Herein, two asymmetric donor-acceptor-acceptor'(D-A-A') type molecule(PTZ-PQ-F and PTZ-PQ-CF3) are developed by employing trifluoromethyl(CF_(3)) or fluorine atom as secondary acceptor, which can exhibit white lighting with dual emission bands consisting of blue traditional fluorescence from quasi-axial(ax) conformer and orange thermally activated delayed fluorescence(TADF) from quasi-equatorial(eq) conformer. The introduction of CF_(3) into PTZ-PQ-CF3 greatly enhanced the photoluminescence quantum yield(PLQY) by suppressing the nonradiative deactivation. Owing to electron-inductive-effect of CF3, the “eq” conformer of PTZ-PQCF3 exhibits a much smaller ΔESTof 0.01 e V to realize more efficient reverse intersystem crossing(RISC)process, and then enhance the exciton utilization(nearly 100%) of the whole dual emission system. Consequently, single-emitter WOLEDs based on PTZ-PQ-CF3 show nearly standard white emission with EQE of 13.0% and CIE of(0.35, 0.36) in m CP host and show warm white emission with high EQE of 25.5%and CIE of(0.40, 0.47) in 35 Dcz PPy host, which are the best performance among reported single-emitter WOLEDs.

关键词： Single-emitter white organic light-emitting diode Conformational isomerism Thermally activated delayed fluorescence Trifluoromethyl Exciton utilization

H2O2-Responsive Injectable Polymer Dots Hydrogel for Long-term Photodynamic Therapy of Tumors

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Chinese Journal of Polymer Science 2024年第11期 1690-1698页

作者： Jian Wang Ke Liang Jian Li Yun-Xiu Zhang Xiao-Kuang Xue Tie-Jin Chen Yong-Liang Hao Jia-Sheng Wu Jie-Chao Ge key laboratory of photochemical conversion and optoelectronic materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences School of Future Technology University of Chinese Academy of Sciences

Photodynamic therapy （PDT） has been emerged as a promising modality for cancer ***,the development of drug delivery system enabling continuous release of photosensitizers （PSs） for long-term PDT treatment still remains ***,a H2O2-responsive injectable hydrogel,covalently crosslinked by N1-（4-boronobenzyl）-N3-（4-boronophenyl）-N1,N1,N3,N3-tetramethylpropane-1,3-diaminium（TSPBA） with PVA containing polythiophene quaternary ammonium salt （PT2） polymer dots （PDots） as a photosensitizer was *** the stimulation of H2O2,the obtained injectable hydrogel gradually degrades and releases *** vitro experiments suggested that the released PDots could realize efficient tumor cells inhibition through its robust singlet oxygen generation capability upon 577 nm laser *** vivo studies demonstrated a sustained retention of PDots for at least 7 days following single-dose administration,facilitating efficient tumor inhibition with light treatments for 3 times without apparent *** work presents an innovative polymer dots-based composite local drug delivery system for long-term PDT in cancer treatment.

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From the perspective of experimental practice: High-throughput computational screening in photocatalysis

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Green Energy & Environment 2024年第1期9卷 1-6页

作者： Yunxuan Zhao Junyu Gao Xuanang Bian Han Tang Tierui Zhang key laboratory of photochemical conversion and optoelectronic materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing100190China Center of materials Science and optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China institute for AI Industry Research(AIR) Tsinghua UniversityBeijing100084China

Photocatalysis,a critical strategy for harvesting sunlight to address energy demand and environmental concerns,is underpinned by the discovery of high-performance photocatalysts,thereby how to design photocatalysts is now generating widespread interest in boosting the conversion efﬁ-ciency of solar *** the past decade,computational technologies and theoretical simulations have led to a major leap in the development of high-throughput computational screening strategies for novel high-efﬁciency *** this viewpoint,we started with introducing the challenges of photocatalysis from the view of experimental practice,especially the inefﬁciency of the traditional“trial and error”***-sequently,a cross-sectional comparison between experimental and high-throughput computational screening for photocatalysis is presented and discussed in *** the basis of the current experimental progress in photocatalysis,we also exempliﬁed the various challenges associated with high-throughput computational screening ***,we offered a preferred high-throughput computational screening procedure for pho-tocatalysts from an experimental practice perspective(model construction and screening,standardized experiments,assessment and revision),with the aim of a better correlation of high-throughput simulations and experimental practices,motivating to search for better descriptors.

关键词： Photocatalysis High-throughput computational screening Photocatalyst Theoretical simulations Experiments

Acceptor-planarized typeⅠphotosensitizer for lipid droplet-targeted two-photon photodynamic therapy by ferroptosis

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Science China chemistry 2024年第7期67卷 2392-2402页

作者： Jie Sha Weimin Liu Jiasheng Wu Yanping Wang Xuewei Li Haohui Ren Zhi Pang Wenjun Zhang Chun-Sing Lee Pengfei Wang key laboratory of photochemical conversion and optoelectronic materials CityU-CAS Joint Laboratory of Functional Materials and DevicesTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China School of Future Technology University of Chinese Academy of SciencesBeijing 100049China Center of Super-Diamond and Advanced Films&Department of materials Science and Engineering City University of Hong KongHong KongChina

Two-photon photodynamic therapy(TP-PDT)has garnered significant attention because of its excellent depth of tissue penetration and high spatiotemporal ***,the limited targeting ability and oxygen dependency of photosensitizers(PSs)significantly hinder the effectiveness of photodynamic therapy in hypoxic tumor ***,we designed and synthesized two lipid droplet(LD)-targeted two-photon PSs(TBPCP and TBCP)by reducing benzene rings to achieve“acceptor planarization”.Notably,acceptor planarization not only enhanced the intramolecular charge transfer but also transferred the photochemical reaction from typeⅡ(TBPCP)to typeⅠ(TBCP).Under the irradiation of 940 nm femtosecond pulsed laser,TBPCP and TBCP showed bright two-photon-excited fluorescence and excellent LD targeting in living *** TBPCP(typeⅡPS),the outstanding TP-PDT efficacy of TBCP(typeⅠPS)under hypoxic conditions could be obtained in both cellular experiments and multicellular tumor spheroids(MCTS)***,both TBPCP and TBCP could induce the lipid peroxidation in the typeⅠor typeⅡPDT due to the location of LD,depleting GSH and inactivating GPX4 to induce nonprogrammed ferroptosis in cells.

关键词： two-photon photodynamic therapy lipid droplet targeting acceptor planarization hypoxia tumor ferroptosis

Hydrophobic long-chain two-dimensional perovskite scintillators for underwater X-ray imaging

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Rare Metals 2024年第1期43卷 175-185页

作者： Jin-Xiao Zheng Zi-An Zhou Tiao Feng Hui Li Cheng-Hua Sun NüWang Yang Tian Yong Zhao Shu-Yun Zhou key laboratory of photochemical conversion and optoelectronic materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China laboratory of Bioinspired Smart Interfacial Science and Technology of the Ministry of Education Beijing Key Laboratory of Bioinspired Energy Materials and DevicesSchool of ChemistryBeijing Advanced Innovation Center for Biomedical EngineeringBeihang UniversityBeijing 100191China Department of Engineering physics Tsinghua University and Key Laboratory of Particle and Radiation Imaging Ministry of EducationTsinghua UniversityBeijing 100084China e-mail:yangt@***

The underwater X-ray imaging technology development is significant to subaqueous target reconnaissance/detection/identification, subfluvial archaeology,submerged resource exploration, etc. As the core of X-ray imaging detection, the scintillator has been plagued by inherent moisture absorption and decomposition, and strict requirements for seamless packaging and ***, we designed a manganese-doped two-dimensional(2D) perovskite scintillator modified by hydrophobic longchain organic amine through the combination of component and doping engineering. The modified perovskites show high water repellency that can be used as an underwater X-ray scintillator. X-ray images of aquatic organisms or other objects with a high spatial resolution of10 lp·mm^(-1) at a big view field(32 mm × 32 mm) were obtained by scintillation screen. This hydrophobic perovskite scintillator based on molecular design is of great promise in underwater X-ray nondestructive testing technology development.

关键词： Two-dimensional perovskite Hydrophobic Scintillators Underwater X-ray imaging Underwater nondestructive testing technology

Metal-Free,Site-Selective C-H Fluorination of Heteroarenes Under Visible Light

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CCS chemistry 2024年第7期6卷 1681-1688页

作者： Cheng Huang Chang-Ming You Yu-Shu Qin Rui-Nan Ci Peng Xiao Sheng Tang Bin Liu Zhenhong Wei Li-Zhu Wu Hu Cai School of chemistry and Chemical Engineering Nanchang UniversityNanchangJiangxi 330031 key laboratory of photochemical conversion and optoelectronic materials Technical Institute of Physics and ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesBeijing 100190 School of Future Technology University of Chinese Academy of SciencesBeijing 100049

The site-selective C-H fluorination of heteroarenes is a straightforward approach to accessing valuable heteroaryl fluorides but remains a formidable ***,we report a general strategy for visible-light-induced C-H fluorination of heteroarenes via the merger of N-F fluorinating reagents and *** paramagnetic resonance experiments provide evidence for the homolytic cleavage of the N-F bond under blue light-emitting diode irradiation,which is the key step in the *** transformation is metal-free,photocatalysts-free,and site-selective under mild reaction conditions(ambient temperature,visible-light irradiation,tolerant to H2O).The robustness of this protocol has also been highlighted by late-stage modification of complex and medicinally relevant molecules.

关键词： selective C-H fluorination heteroaryl fluorides C(sp^(2))-F bond formation photochemistry radical chemistry

Photo-induced Intramolecular Charge Transfer in Strained Organic Cage Containing Orthogonally Arranged Donors and Acceptors

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CCS chemistry 2024年第8期6卷 1920-1928页

作者： Jingxuan Yang Run Shi Liang-Liang Mao Hongyan Xiao Yi Zeng Guohong Liao Yuxiang Weng Xu-Bing Li Jiaqi Zhao Yunxuan Zhao Tierui Zhang Chen-Ho Tung Li-Zhu Wu Huan Cong key laboratory of photochemical conversion and optoelectronic materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 key laboratory of Bio-Inspired materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 Beijing National laboratory for Condensed Matter physics Laboratory of Soft Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049 Binzhou institute of Technology Weiqiao-UCAS Science and Technology ParkBinzhou CityShandong 256606 Songshan Lake materials laboratory DongguanGuangdong 523808

Designing and creating molecular structures with precisely organized organic chromophores as donors and acceptors are critical for exploring photo-induced charge transfer *** and acceptor moieties can be incorporated to the confined skeletons of organic cages,thereby offering opportunities tomanipulate excited state characters for the development of novel photofunctional ***,we present the convergent synthesis and photophysical characterizations of an organic cage with anisotropic *** strained and rigid cage can be concisely prepared by connecting two distinct macrocycles through axial stacking strategy,featuring triarylamine and amide moieties as separate donors and acceptors,***-state and time-resolved spectra reveal photo-induced through-space intramolecular charge transfer and long-lived charge separation,thereby verifying the cage’s photocatalytic utility for efficient hydrogen production.

关键词： organic cage macrocycles photoinduced charge transfer through-space photocatalytic hydrogen evolution