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Recent progress on photoactive nonprecious transition-metal complexes

Science China Chemistry 2025年第1期 46-95页

作者： Zhong-Liang Gong Hong-Jie Zhang Yan Cheng Jianxun Liu Yuhan Ai Yaqin Li Zhihui Feng Qiong Zhang Shaolong Gong Yong Chen Chang-Jiang Yao Yuan-Yuan Zhu Liang-Jin Xu Yu-Wu Zhong CAS Key laboratory of photochemistry Institute of Chemistry Chinese Academy of Sciences State Key laboratory of Structural Cemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences School of Chemistry and Chemical Engineering Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of Technology State Key laboratory of Explosion Science and Safety Protection School of Mechatronical Engineering Beijing Institute of Technology College of Chemistry and Molecular Sciences Hubei Key Lab on Organic and Polymeric Optoelectronic Materials Wuhan University School of Chemistry and Chemical Engineering Anhui University Key laboratory of Photochemical Conversion and Optoelectronic Materials & CAS-HKU Joint laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Photoactive complexes of nonprecious transition metals, mainly including those in the first-row and partially the second-row of the Periodic table of elements, have received increasing attention in view of their low cost and long-term sustainability. They are recognized as promising alternatives to noble transition metal complex congeners that have been extensively studied in optoelectronic devices, artificial photosynthesis, photocatalysis, biodiagnostics, and therapeutics, etc. This review is devoted to a comprehensive summary on the classical and recent advances on photoactive nonprecious transition metal complexes, including photoactive Zr, V, Cr, Mo, and W complexes, Mn complexes and hybrids, Fe, Co, Ni, and Cu complexes, and Zn and Cd complexes and hybrids. A particular focus is given on the molecular design, modulation of photophysical and photochemical properties, and applications of the representative and lately-developed nonprecious metal complexes. In addition, a perspective on the future development in this field is provided at the end of this review.

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Synthesis, Structure and Catalytic Activity of a Manganese(Ⅲ) Complex Based on 2-(2-Hydroxyphenyl)-5,6-dichlorobenzimidazole Ligands

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Chinese Journal of Structural Chemistry 2014年第10期33卷 1479-1487页

作者：王鸾张纯喜赵井泉 laboratory of photochemistry Institute of ChemistryChinese Academy of Sciences

A new ligand, 2-（2-hydroxyphenyl）-5,6-dichlorobenzimidazole, H2pbmCl2（1）, and a novel MnIII complex, [MnIII（HpbmCl2）（pbmCl2）（DMF）2]（2）,（DMF = N,N-dimethylformamide）, have been synthesized and characterized. The crystal of compound 1（C13H8Cl2N2O, Mr = 279.12） belongs to the monoclinic system, space group P21 with a = 3.770（5）, b = 25.20（3）, c = 5.865（7） A, = 92.727（17）o, V = 556.6（12） A3, Z = 2, Dc = 1.665 g/cm^3, S = 1.137, μ= 0.568 mm^-1, F（000） = 284, the final R = 0.0876 and wR = 0.2334 for 1848 independent reflections. The molecule is planar due to the presence of a strong intramolecular hydrogen bond between O–H group of phenol and N atom of imidazole. H2pbmCl2（1） molecules are arranged into a one-dimensional linear chain through intermolecular hydrogen bonds（N–H…O and C–H…Cl）. The crystal of complex 2（C32H27Cl4MnN6O4, Mr = 756.34） belongs to the monoclinic system, space group P21/c with a = 19.043（10）, b = 10.808（5）, c = 18.704（11）A, β= 115.540（6）°, V = 3473（3） A3, Z = 4, Dc = 1.446 g/cm^3, S = 1.3, μ = 0.733 mm-1, F（000） = 1544, the final R = 0.1219 and wR = 0.2681 for 7811 independent reflections. The Mn ion adopts a distorted octahedral geometry coordinated by two deprotonated H2pbmCl2 ligands and two DMF molecules. The [MnIII（HpbmCl2）（pbmCl2）（DMF）2] molecules are arranged into a three-dimensional structure through hydrogen bonds（N–H…N, C–H…N and C–H…Cl） and weak π···πinteractions. The activity measurements suggest that complex 2 is able to serve as a catalyst for H2O2 disproportionation reaction to form O2 in neutral water solution.

关键词： 2-(2-hydroxyphenyl)-5 6-dichlorobenzimidazole manganese complex crystal structure H2O2 disproportionation reaction catalyst

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The first artificial Mn_4Ca-cluster mimicking the oxygen-evolving center in photosystem Ⅱ

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Science China(Life Sciences) 2015年第8期58卷 816-817页

作者： ZHANG ChunXi laboratory of photochemistry Institute of Chemistry Chinese Academy of Sciences

The oxygen-evolving center （OEC） in photosystem Ⅱ（PSⅡ） of plants, algae and cyanobacteria, is a unique catalyst in nature to split water into O2, protons and electrons by using sun light. Because of broad fundamental interests and potential applications in artificial photosynthesis, the structure and properties of this unique catalyst have attracted extensive attention during the last two decades. Recent X-ray crystallographic studies of PSⅡ have revealed that the bio- logical OEC is comprised of a unique asymmetric Mn4Cacluster bound to protein groups [1,2] （Figure 1, left）. This biological catalyst serves as a blueprint for the development of efficient and cheap artificial catalysts for water-splitting reaction to overcome the bottleneck of entire field of artificial photosynthesis. However, it is a great challenge for chemists to synthesize the whole structure of the OEC in laboratory mainly due to the following reasons：（i） It is

关键词：人工模拟集群系统氧气生物催化剂人工光合作用 X-射线晶体学 OEC 光系统Ⅱ

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Photo-induced Charge Separation of p-Tricyanovinyl-N,N-Dialkylanilines

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Science China Chemistry 1993年第2期36卷 162-169页

作者：张宝文陈燕曹怡佟振合 laboratory of photochemistry Institute of Photographic Chemistry Academia Sinica Beijing 100101 PRC

In this paper,p-tricyanovinyl-N,N-dialkylanilines were synthesized as model compounds and through their spectroscopic behavior,the photo-induced electron transfer,charge separation were discussed and the aggregation i... 详细信息

关键词： p-tricyanovinyl-N N-dialkylaniline electron transfer charge separation spectroscopic behavior aggregation.

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Urea-bridged diferrocene: structural, electrochemical, and spectroelectrochemical studies

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Science China Chemistry 2015年第9期58卷 1444-1450页

作者： Zhong-Liang Gong Yu-Wu Zhong Beijing National laboratory for Molecular Sciences CAS Key laboratory of photochemistry Institute of Chemistry Chinese Academy of Sciences

Urea-bridged diferrocene derivatives N,N?-diferrocenylurea(1) and N,N?-dimethyl-N,N?-diferrocenylurea(2) were prepared and characterized. Single-crystal X-ray analysis shows that Compound 1 has a trans-trans linear conformation whereas Compound 2 has a trans-cis conformation. Both compounds display two consecutive redox couples with, respectively, E1/2 of +0.29 and +0.42 V vs. Ag/Ag Cl for 1 and +0.31 and +0.50 V for 2. Spectroelectrochemical studies show the presence of distinct intervalence charge transfer(IVCT) transitions for the one-electron-oxidized mixed-valent Compound 1+, with an estimated electronic coupling parameter of 190 cm?1. By contrast, the one-electron-oxidized Compound 2+ shows much weaker IVCT transitions.

关键词： mixed-valent compounds ferrocene electrochemistry urea spectroelectrochemistry

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A new milestone for photosynthesis

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National Science Review 2018年第4期5卷 444-445页

作者： Chunxi Zhang Tingyun Kuang laboratory of photochemistry Institute of Chemistry Chinese Academy of Sciences laboratory of Photobiology Institute of BotanyChinese Academy of Sciences

The photosynthetic water-splitting reaction catalysed by the oxygen-evolving center(OEC)in the photosystem II of plants releases protons,electrons and dioxygen,which is one of the most important processes for energy and material conversions on *** is a Mn4Cacluster and cycles through five different states(Sn,n=0–4),wherein S0is the most reduced state,S1is the dark stable state and S2,S3and S4are intermediate

关键词： OEC A new milestone for photosynthesis

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Synthesis and photovoltaic properties of low bandgap dimeric perylene diimide based non-fullerene acceptors

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Science China Chemistry 2016年第2期59卷 209-217页

作者： Xin Zhang Jiannian Yao Chuanlang Zhan Beijing National laboratory of Molecular Science Key laboratory of photochemistry Chinese Academy of Sciences Institute of Chemistry Chinese Academy of Sciences

Non-fullerene organic acceptors have attracted increasing attention in recent years. One of the challenges in the synthesis of non-fullerene organic acceptors is to tune the absorption spectrum and molecular frontier orbitals, affording low bandgap molecules with improved absorption of the near-infrared solar photons. In this paper, we present the synthesis, optoelectronic and photovoltaic properties of a series of dimeric perylene diimide(PDI) based non-fullerene acceptors. These PDI dimers are bridged by oligothiophene(T) from 1T to 6T. With the increase of the oligothienyl size, the highest occupied molecular orbital(HOMO) energy is raised from ?5.65 to ?5.10 e V, while that of the lowest unoccupied molecular orbit(LUMO) is kept constant at ?3.84 e V, affording narrow bandgap from 1.81 to 1.26 e V. The absorption from the oligothiophene occurs between 350 and 500 nm, which is complementary to that from its bridged PDI units, leading to a wide spectral coverage from 350 to 850 nm. The optimal dihedral angle between the bridged two perylene planes is dependent on the oligothienyl size, varying from 5° to 30°. The solubility of the dimers depends on the oligothienyl size and can be tuned by the alkyl chains on the bridged thienyl units. The possible applications as the solution-processable non-fullerene organic acceptor is primarily studied using commercial P3 HT as the blend donor. The photovoltaic results indicate that 1T, 4T and 6T all yield a higher efficiency of ?1.2%, whereas 2T, 3T and 5T all give a lower efficiency of <0.5%. The difference in the cell performance is related with the tradeoff between the differences of absorption, HOMO level and film-morphology between these dimers.

关键词： non-fullerene acceptor organic photovoltaic cell perylene diimide solution-processed bulk-heterojuncti ~n

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Photoinduced energy transfer and charge transfer on squarylium cyanine dyes

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Chinese Journal of Chemistry 1998年第6期16卷 499-508页

作者：赵为张宝文侯原军曹怡 photochemistry laboratory Institute of Photographic ChemistryChinese Academy of SciencesBeijing 100101China

A series of squarylium cyanine dyes (Sqs) were synthesised to explore their applications in functional devices. Preliminary investigation on the mechanism involved in these devices was carried out. Spectroscopic behavior of Sqs with porphyrin (P), 8-hydroxyquinolium aluminum (Alq) and ruthenium bipyridyl complex (Ru(bipy)) in solution, in film and on nanocrystalline TiO2 was investigated, respectively. A mechanism including photoinduced energy transfer and charge transfer processes was suggested in the corresponding practical devices. By means of doping, a red organic electroluminescent device (ELD) using Sq-doped Alq as the emission layer (EML) has been developed, and the total light to electricity efficiency of nanocrystalline TiO2 electrode based on using Sq-doped Ru(bipy) M photosensitizer has been improved greatly in the whole visible region, particularly in the red area above 600 nm.

关键词： Electroluminescence photoinduced energy transfer photoinduced charge transfer photoelectric conversion

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Syntheses, Crystal Structures and Catalytic Activities of Two Novel Mn_2Dy_2O_2 Complexes

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Chinese Journal of Structural Chemistry 2019年第1期38卷 109-116,4页

作者： ZHAO Guo-Qing LI Yan-Xi CHEN Chang-Hui ZHANG Chun-Xi laboratory of photochemistry Institute of ChemistryChinese Academy of Sciences University of Chinese Academy of Sciences

Two novel heteronuclear manganese-dysprosium complexes have been synthesized and characterized, both of which contain a [Mn_2Dy_2O_2] core ligated by eight But CO_2-anions and four neutral ligands. In complex 1, [Mn_2Dy_2O_2(Bu^tCO_2)_8(Bu^tCO_2H)_4], all the four neutral ligands coordinated to Dy^(3+) are pivalic acids; Instead, two of these four pivalic acids have been replaced by ethanol in complex 2 [Mn2 Dy2 O2(Bu^tCO_2)_8(Bu^tCO_2H)_2(CH_3CH_2OH)_2]. The crystal of complex 1(C_(60)H_(112)Dy_2Mn_2O_(26), Mr = 1684.36) belongs to the orthorhombic system, space group Pbca with a =19.853(3), b = 18.565(3), c = 20.952(3) ?, V = 7723(2) ?3, Z = 4, Dc = 1.449 g/cm^3, S = 1.210, μ =2.302 mm^(-1), F(000) = 3448, the final R = 0.0802 and w R = 0.1570 for 8736 independent *** crystal of complex 2(C_(54)H_(104)Dy_2Mn_2O_(24), Mr = 1572.25) belongs to the monoclinic system,space group C2/c with a = 27.814(6), b = 13.194(3), c = 22.912(5) ?, β = 124.89(3)o, V = 6897(3) ?3,Z = 4, Dc = 1.514 g/cm^3, S = 1.086, μ = 2.570 mm^(-1), F(000) = 3208, the final R = 0.0256 and wR =0.0592 for 7763 independent reflections. The cyclic voltammogram and catalytic activity measurements of complex 1 suggest that this type of complex can serve as a catalyst for oxygen-evolving reaction.

关键词： manganese-dysprosium cluster crystal structure catalytic activity

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Syntheses of bifunctional molecules containing [12]aneN_3 and carbazol moieties as effective DNA condensation agents

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Science China Chemistry 2014年第2期57卷 296-306页

作者： YAN Hao YUE Pan LI ZhiFen GUO ZhiFo LU ZhongLin Key laboratory of Theoretical and Computational photochemistry Ministry of Education College of Chemistry Beijing Normal University

Bifunctional molecules containing macrocyclic polyamine [12]aneN3 and carbazol units, 1-4, have been efficiently synthe sized and fully characterized. Through gel electrophoresis, atomic force microscopy, and dynamic light scattering experiments, compounds 3 and 4b bearing both [12]aneN3 and carbazol moieties showed effective DNA condensation ability at the concen- tration of 80 jaM. Investigations from EB displacement fluorescence spectra, viscosity titration, and ionic strength effects re vealed that the effective DNA condensation comes from the appropriate combination of carbazol and [12]aneN3 units in the bifunctional molecules, and the DNA condensation process is reversible. The incorporation of triazole units in the molecules clearly reduced the cytotoxicity.

关键词： DNA condensation macrocyclic polyamines carbazoles triazole gel electrophoresis AFM

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