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Necessity of structural rearrangements for O-O bond formation between O5 and W2 in photosystemⅡ

Journal of Energy Chemistry 2021年第6期30卷 436-442,I0011页

作者： Yu Guo Biaobiao Zhang lars kloo Licheng Sun Department of Chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of Technology.S E-10044 StockholmSweden State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Center on Molecular DevicesDalian University of Technology(DUT)Dalian 116024LiaoningChina Center of Artificial Photosynthesis for Solar Fuels School of ScienceWestlake University.Hangzhou 310024ZhejiangChina

Numerous aspects of the water oxidation mechanism in photosystemⅡhave not been fully elucidated,especially the O-O bond formation ***,a body of experimental evidences have identified the O5 and W2 ligands of the oxygen-evolving complex as the highly probable substrate *** this work,we studied O-O bond formation between O5 and W2 based on the native Mn4 Ca cluster by density functional *** rearrangements before the formation of the S_(4) state were found as a prerequisite for O-O bond formation between O5 and W2,regardless if the suggested pathways involving the typical Mnl(Ⅳ)-O·species or the recently proposed Mn4(Ⅶ)(O)2 *** alternatives for the S2→S_(3) and S_(3)→S_(4) transitions accounting for such required rearrangements are *** findings reflect that the structural flexibility of the Mn4 Ca cluster is essential to allow structural rearrangements during the catalytic cycle.

关键词： Density functional theory Oxygen-evolving complex Substrate water OAO bond formation Structural rearrangement

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A crosslinked polymer as dopant-free hole-transport material for efficient n-i-p type perovskite solar cells

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Journal of Energy Chemistry 2021年第4期30卷 211-218页

作者： Linqin Wang Fuguo Zhang Tianqi Liu Wei Zhang Yuanyuan Li Bin Cai Lanlan He Yu Guo Xichuan Yang Bo Xu James M.Gardner lars kloo Licheng Sun Organic Chemistry Centre of Molecular DevicesDepartment of ChemistryKTH Royal Institute of TechnologySE-10044 StockholmSweden Applied Physical Chemistry Centre of Molecular DevicesDepartment of ChemistryKTH Royal Institute of TechnologySE-10044 StockholmSweden Wallenberg Wood Science Centre Department of Fibre and Polymer TechnologyKTH Royal Institute of TechnologySE-10044 StockholmSweden State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Centre on Molecular DevicesDalian University of TechnologyDalian 116024LiaoningChina

A new crosslinked polymer,called P65,with appropriate photo-electrochemical,opto-electronic,and thermal properties,has been designed and synthesized as an efficient,dopant-free,hole-transport material(HTM)for n-i-p type planar perovskite solar cells(PSCs).P65 is obtained from a low-cost and easily synthesized spiro[fluorene-9,90-xanthene]-30,60-diol(SFX-OH)-based monomer X65 through a freeradical polymerization *** combination of a three-dimensional(3 D)SFX core unit,holetransport methoxydiphenylamine group,and crosslinked polyvinyl network provides P65 with good solubility and excellent film-forming *** employing P65 as a dopant-free hole-transport layer in conventional n-i-p type PSCs,a power conversion efficiency(PCE)of up to 17.7%is *** the best of our knowledge,this is the first time a 3 D,crosslinked,polymeric dopant-free HTM has been reported for use in conventional n-i-p type *** study provides a new strategy for the future development of a 3 D crosslinked polymeric dopant-free HTM with a simple synthetic route and low-cost for commercial,large-scale applications in future PSCs.

关键词： Perovskite solar cell Hole-transport material Dopant-free Crosslinked polymer Spiro[fluorene-9,9’-xanthene](SFX)

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A novel phenoxazine-based hole transport material for efficient perovskite solar cell

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Journal of Energy Chemistry 2015年第6期24卷 698-706页

作者： Ming Cheng Cheng Chen Bo Xu Yong Hua Fuguo Zhang lars kloo Licheng Sun Department of Chemistry Organic ChemistryKTH Royal Institute of Technology Department of Chemistry Applied Physical ChemistryKTH Royal Institute of Technology State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT–KTH Joint Education and Research Centre on Molecular DevicesDalian University of Technology (DUT)

Based on the previous research work in our laboratory, we have designed and synthesized a small-molecule, hole transport material （HTM） POZ6-2 using phenoxazine （POZ） as central unit and dicyanovinyl units as electron-withdrawing terminal groups. Through the introduction ofa 2-ethyl-hexyl bulky chain into the POZ core unit, POZ6-2 exhibits good solubility in organic solvents. In addition, POZ6-2 possesses appropriate energy levels in combination with a high hole mobility and conductivity in its pristine form. Therefore, it can readily be used as a dopant-flee HTM in perovskite solar cells （PSCs） and a conversion efficiency of 10.3% was obtained. The conductivity of the POZ6-2 layer can be markedly enhanced via doping in combination with typical additives, such as 4-tert-butylpyridine （TBP） and lithium bis（trifluoromethanesulfonyl） imide （LiTFS1）. Correspondingly, the efficiency of the PSCs was further improved to 12.3% using doping strategies. Under the same conditions, reference devices based on the well-known HTM Spiro-OMeTAD show an efficiency of 12.8%.

关键词： Dopant-flee Perovskite solar cell Hole transport material Phenoxazine Thin fiim

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