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Photophysical Properties and Photovoltaic Performance of Sensitizers with a Bipyrimidine Acceptor

Transactions of tianjin University 2024年第5期30卷 406-418页

作者： Shiling Liu Kun Gong Wei Li Dongzhi Liu Xueqin Zhou School of Chemical engineering and Technology Collaborative Innovation Center of Chemical Science and Engineering Tianjin Engineering Research Center of Functional Fine Chemicals Tianjin University

Molecular engineering is a crucial strategy for improving the photovoltaic performance of dye-sensitized solar cells（DSSCs）. Despite the common use of the donor–π bridge–acceptor architecture in designing sensitizers, the underlying structure–performance relationship remains not fully understood. In this study, we synthesized and characterized three sensitizers: MOTP-Pyc, MOS2P-Pyc, and MOTS2P-Pyc, all featuring a bipyrimidine acceptor. Absorption spectra, cyclic voltammetry, and transient photoluminescence spectra reveal a photo-induced electron transfer（PET） process in the excited sensitizers. Electron spin resonance spectroscopy confirmed the presence of charge-separated states. The varying donor and π-bridge structures among the three sensitizers led to differences in their conjugation effect, influencing light absorption abilities and PET processes and ultimately impacting the photovoltaic performance. Among the synthesized sensitizers, MOTP-Pyc demonstrated a DSSC efficiency of 3.04%. Introducing an additional thienothiophene block into the π-bridge improved the DSSC efficiency to 4.47% for MOTS2P-Pyc. Conversely, replacing the phenyl group with a thienothiophene block reduced DSSC efficiency to 2.14% for MOS2P-Pyc. Given the proton-accepting ability of the bipyrimidine module, we treated the dye-sensitized TiO2photoanodes with hydroiodic acid（HI）, significantly broadening the light absorption range. This treatment greatly enhanced the short-circuit current density of DSSCs owing to the enhanced electron-withdrawing ability of the acceptor. Consequently, the HI-treated MOTS2P-Pyc-based DSSCs achieved the highest power conversion efficiency of 7.12%, comparable to that of the N719 dye at 7.09%. This work reveals the positive role of bipyrimidine in the design of organic sensitizers for DSSC applications.

关键词： Acidichromic property Bipyrimidine acceptor Charge separation Dye-sensitized solar cells Molecular engineering Photophysical processes

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Enhancement of liquid-liquid micromixing performance in curved capillary microreactor by generation of Dean vortices

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Chinese Journal of Chemical engineering 2024年第4期68卷 76-82页

作者： Shaoyun Wu Zhuang Ma Zichi Yang Suying Zhao Caijin Zhou Huidong Zheng Fujian engineering research center of Advanced Manufacturing Technology for fine chemicals College of Chemical EngineeringFuzhou UniversityFuzhou 350108China Qingyuan Innovation Laboratory Quanzhou362114China

Micromixing efficiency is an important parameter for evaluating the multiphase mass transfer performance and reaction efficiency of *** this work,the novel curved capillary reactor with different shapes was designed to generate Dean flow,which was used to enhance the liquid-liquid micromixing *** Villermaux-Dushman probe reaction was employed to characterize the micromixing performance in different curved capillary *** effects of experiment parameters such as liquid flow rate,inner diameter,tube length,and curve diameter on micromixing performance were systematically *** the optimal conditions,the minimum value of the segmentation factor XS was *** was worth noting that at the low Reynolds number(Re<30),the change of curved shape on the capillary microreactor can significantly improve the micromixing performance with XS reduced by 37.5%.Further,the correlations of segment index XS with dimensionless factor such as Reynolds number or Dean number were developed,which can be used to predict the liquid-liquid micromixing performance in capillary microreactors.

关键词： Microreactor Process intensification Micromixing performance Dean flow

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Propane dehydro-aromatization reaction over PtFe@S-1 coupling with Zn/ZSM-5 tandem catalysts: the role of Zn species

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Frontiers of Chemical Science and engineering 2024年第8期18卷 25-35页

作者： Kai Bian Sirui Liu Huahua Fan Guanghui Zhang Xinwei Zhang Gideon Abaidoo Ocran Mingrui Wang Quanjie Liu Xiaowa Nie Shuandi Hou Xinwen Guo Sinopec Dalian research Institute of Petroleum and Petrochemicals Dalian 116045China State Key Laboratory of fine chemicals Frontier Science Center for Smart MaterialsPSU-DUT Joint Center for Energy ResearchSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China

Unraveling the structure-activity relationship and improving the catalytic performance is paramount in propane dehydro-aromatization reactions. Herein, a tandem catalyst with high propane dehydro-aromatization reaction performance was prepared via coupling the PtFe@S-1 with Zn/ZSM-5 zeolites (PtFe@S-1&1.0Zn/ZSM-5), which exhibits high dehydrogenation activity, aromatics selectivity (~60% at ~78% propane conversion), and stability. The addition of zinc inhibits the cleavage of C_(6)^(=) intermediates on ZSM-5 and promotes the aromatization pathway by weakening zeolite acid strength, significantly improving the selectivity to aromatics. This understanding of the structure-activity relationship in propane dehydro-aromatization reaction helps develop future high-performance catalysts.

关键词： propane dehydro-aromatization reaction tandem catalysts the structure-activity relationship of zinc species

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Effect of Free Radicals on Irradiation Chemistry of a Double-Coordination Organotin(Sn_(4))Photoresist by Adjusting Alkyl Ligands

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CCS Chemistry 2024年第8期6卷 2044-2053页

作者： Hao Chen Yifeng Peng Haichao Fu Fuping Han Guangyue Shi Feng Luo Jun Zhao Danhong Zhou Pengzhong Chen Xiaojun Peng State Key Laboratory of fine chemicals Frontiers Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024 research and Development center of Valiant Co. Ltd.YEDAYantai 264006 School of Materials Science and engineering Nankai UniversityTianjin 300350 Shanghai Advanced research Institute Chinese Academy of SciencesShanghai 201203 State Key Laboratory of fine chemicals College of Materials Science and EngineeringShenzhen UniversityShenzhen 518060

Metal oxide cluster(MOC)photoresists are highly promising materials for the next generation of extreme ultraviolet lithography(EUVL).The consecutive exploration of novel MOC materials and their structural irradiation chemistry are the major concerns associated with ***,we report two bicoordinated tin-oxo clusters(TOCs),the organic ligands of which contain both adamantane carboxylic acids and alkyl groups(methyl:Sn_(4)–Me–C10;butyl:Sn_(4)–Bu–C10).We explore the correlation between the structures of the TOCs and their patterning properties by adjusting the alkyl groups coordinated to the Sn *** structural variation causes different irradiation chemistry,with Sn_(4)–Me–C10 exhibiting improved resolution and Sn_(4)–Bu–C10 demonstrating higher *** differences are attributed to the bonding energies of the Sn-methyl and Sn-butyl groups,the size of the resulting alkyl radicals,and their reaction *** clusters occur in the reactions of Sn–C bond cleavage and the decarboxylation of adamantane carboxylic acids upon ***,the entire process exhibits distinct *** on the electron-beam lithography and other experiments,we proposed irradiationinduced reaction mechanisms for both *** Sn_(4)–Bu–C10 cluster predominantly undergoes alkane chain linkage,whereas the Sn_(4)–Me–C10 cluster mainly follows the adamantanes linkage pathway.

关键词： extreme ultraviolet photoresist tin-oxo clusters free radical alkyl ligand lithographic process semiconductor manufacturing

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Lifetime-tunable circularly polarized luminescent system based on triplet-to-singlet Förster resonance energy transfer

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Science China Chemistry 2024年第9期67卷 2918-2922页

作者： Zhenyi He Zizhao Huang Xiang Ma Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint research center Institute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

Circularly polarized luminescence(CPL)materials have received widespread attention due to their remarkable performance and broad ***,current CPL material research primarily focuses on tunable color,intensity,and *** CPL with adjustable lifetime remains a significant ***,a series of CPL polymeric materials with tunable lifetime were obtained by employing phosphorescent terephthalic acid and chiral organic small molecule R/S-BNAF(a luminescent binaphthol derivative)to copolymerize with acrylamide in different *** was verified that this performance results from the different energy transfer efficiency between luminophores with varying ratios of the monomers for *** strategy to realize CPL with tunable lifetime by modulating the energy transfer efficiency will provide a new perspective to broaden the applications of CPL materials.

关键词： circularly polarized luminescence tunable lifetime Förster resonance energy transfer room temperature phosphorescence

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Recent advances in multifunctional shape memory photonic crystals and practical applications

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Nano research 2024年第1期17卷 79-96页

作者： Yong Qi Shufen Zhang State Key Laboratory of fine chemicals Frontier Science Center for Smart MaterialsDalian University of TechnologyDalian 116024China

Shape memory photonic crystals(SMPCs)are smart composite materials with changeable structural color integrated by shape memory polymer and photonic *** can produce one or more temporary shapes through nanoscale deformation,memorizing current *** can be recovered to their original shapes or some intermediate states under external stimuli,accompanied by the variation of structural *** porous carriers with built-in sensing properties,SMPCs promoted the interdisciplinary development of nanophotonic technology in materials science,environmental engineering,biomedicine,chemical engineering,and ***,the recent progress on multifunctional SMPCs and practical applications,including traditional and cold programmable SMPCs,is summarized and *** primary concern is shape programming at the nanoscale that has demonstrated numerous attractive functions,including smart sensing,ink-free printing,solvent detection,reprogrammable gradient wetting,and controllable bubble transportation,under variations of the surface *** aims to figure out the nanoscale shape memory effects on structural color conversion and additional performance,inspiring the fabrication of the next generation of ***,perspectives on future research directions and applications are also *** is believed that multifunctional SMPCs are powerful nanophotonic tools for the interdisciplinary development of numerous disciplines in the future.

关键词： photonic crystal shape memory structural color cold programmable shape recovery

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A method for establishing a bearing residual life prediction model for process enhancement equipment based on rotor imbalance response analysis

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Chinese Journal of Chemical engineering 2024年第2期66卷 203-215页

作者： Feng Wang Haoran Li Zhenghui Zhang Yan Bai Hong Yin Jing Bian National Foundation research Laboratory of Fault Prevention and Control in Hazardous chemicals Production System Engineering Research Center of Chemical Technology SafetyBeijing University of Chemical TechnologyBeijing 100029China China Nuclear Power engineering Co. LtdBeijing 100840China CNOOC tianjin Chemical research and Design Institute Co. LtdTianjin Key Laboratory of Energy and Chemical Explosion SafetyAcademician Expert Collaborative Innovation CenterTianjin 300131China

A rotating packed bed is a typical chemical process enhancement equipment that can strengthen micromixing and mass *** the operation of the rotating packed bed,the nonreactants and products irregularly adhere to the wire mesh packing in the rotor,thus resulting in an imbalance in the vibration of the rotor,which may cause serious damage to the bearing and material *** study proposes a model prediction for estimating the bearing residual life of a rotating packed bed based on rotor imbalance response *** method is used to determine the influence of the mass on the imbalance in the vibration of the rotor on bearing *** major influence on rotor vibration was found to be exerted by the imbalanced mass and its distribution radius,as revealed by the results of orthogonal *** implementing finite element analysis,the imbalance response curve for the rotating packed bed rotor was obtained,and a correlation among rotor imbalance mass,distribution radius of imbalance mass,and bearing residue life was established via data *** predicted value of the bearing life can be used as the reference basis for an early safety warning of a rotating packed bed to effectively avoid accidents.

关键词： Rotating packed bed Mass imbalance Harmonic response analysis Residual life Prediction model

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Efficient wide-bandgap perovskite solar cells with open-circuit voltage deficit below 0.4 V via hole-selective interface engineering

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Science China Chemistry 2024年第6期67卷 2102-2110页

作者： Xiaoyu Ji Shuo Zhang Furong Yu Huidong Zhang Liqing Zhan Yue Hu Wei-Hong Zhu Yongzhen Wu Key Laboratory for Advanced Materials and Joint International research Laboratory of Precision Chemistry and Molecular engineering Shanghai Key Laboratory of Functional Materials ChemistryFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China School of Chemistry University of EdinburghKing’s BuildingsEdinburghEH93FJUK

Wide-bandgap mixed-halide perovskite solar cells(WBG-PSCs)are promising top cells for efficient tandem photovoltaics to achieve high power conversion efficiency(PCE)at low ***,the open-circuit voltage(V_(OC))of WBG-PSCs is still unsatisfactory as the V_(OC)-deficit is generally larger than 0.45 ***,we report a buried interface engineering strategy that substantially improves the V_(OC)of WBG-PSCs by inserting amphiphilic molecular hole-selective materials featuring with a cyanovinyl phosphonic acid(CPA)anchoring group between the perovskite and *** assembly and redistribution of CPA-based amphiphilic molecules at the perovskite-substrate buried interface not only promotes the growth of a low-defect crystalline perovskite thin film,but also suppresses the photo-induced halide phase *** energy level alignment between wide-bandgap perovskite and the hole-selective layer is further improved by modulating the substituents on the triphenylamine donor moiety(methoxyls for MPA-CPA,methyls for Me PA-CPA,and bare TPA-CPA).Using a 1.68 e V bandgap perovskite,the Me PA-CPA-based devices achieved an unprecedentedly high V_(OC)of 1.29 V and PCE of 22.3%under standard AM 1.5 *** V_(OC)-deficit(<0.40 V)is the lowest value reported for *** work not only provides an effective approach to decreasing the V_(OC)-deficit of WBG-PSCs,but also confirms the importance of energy level alignment at the charge-selective layers in PSCs.

关键词： cyanovinyl phosphonic acid energy level alignment hole-selective material open-circuit voltage wide-bandgap perovskite

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Exploration of Strong Metal-Support Interaction in Heterogeneous Catalysts by in situ Transmission Electron Microscopy

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Chinese Journal of Chemistry 2024年第9期42卷 1004-1008页

作者： Yongjun Jiang Sheng Dai Key Laboratoryfor Advanced Materials and Feringa Nobel Prize Scientist Joint research center Institute of Fine ChemicalsSchool of Chemistry&Molecular EngineeringEast China Universityof Science and TechnologyShanghai 200237China

The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research attention due to its significance in heterogeneous ***,great progress has been made in recent years in investigating SMSI by in situ transmission electron microscopy(TEM),along with an enhanced comprehension of the underlying mechanisms governing SMSI *** emerging topic summarizes recent progress utilizing in situ TEM to study the interaction between metal and support and the relationship between the structure and performance of the supported catalyst under reaction conditions.A brief perspective about the use of in situ TEM for further study of SMSI is also presented,showing prospects in this field that will stimulate further upsurging research in promoting the catalytic efficiency of supported catalysts.

关键词： Heterogeneous catalysis In situ TEM Strong metal-support interaction Structure changes Interfaces Structural evolution

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Asymmetrically ligated single atomic nickel sites for efficient hydrogen peroxide electrosynthesis

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Nano research 2024年第3期17卷 1094-1100页

作者： Xusheng Cheng Jinwen Hu Wenzhe Shang Jingya Guo Cuncun Xin Songlin Zhang Suchan Song Wei Liu Yantao Shi State Key laboratory of fine chemicals Frontier Science Center for Smart MaterialsSchool of ChemistryDalian University of TechnologyDalian 116024China

Atomic transition-metal-nitrogen-carbon electrocatalysts hold great promise as alternatives to benchmark Pt in the oxygen reduction *** pristine metal centers with quasi square-planar D_(4h) configuration,however,still suffer from unfavorable energetics and thereby strong activity/selectivity trade-off during the catalytic *** we present a ligand-field engineering of single-atom Ni-N-C catalysts to boost the sluggish kinetics via rationally constructing prototypical asymmetrically ligated Ni-N_(3)O_(1) *** as-obtained Ni-supported multi-walled carbon nanotubes with molten salt-treated(defined as Ni/CNS)catalyst delivered an excellent H_(2)O_(2) selectivity(>90%)within a wide potential window(0.2–0.7 V *** hydrogen electrode(RHE))and robust stability(for 10 h)in alkaline *** electron paramagnetic resonance and theoretical analysis rationalize this finding and demonstrate that the broken symmetry facilitates the electron transfer of a σ* to O–O orbital as compared to the Ni-N_(4) counterpart,playing an indispensable role in efficient O_(2) activation.

关键词： broken D4h single nickel sites oxygen reduction H_(2)O_(2)production

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