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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 0,Vol.>> Issue()>> 0-0     doi: 10.3866/PKU.WHXB201711091         中文摘要
Accepted manuscript
[Ag25(SC6H4Pri)18(dppp)6](CF3SO3)7·CH3CN (HSC6H4Pri =4-t-isopropylthiophenol, and dppp=1,3-bis(diphenyphosphino)propane) Cluster Containing a Sandwich-like Skeleton: Structural Characterization and Optical Properties
XIE An1, WANG Zhi2, WU Qiaoyu3, CHENG Liping2,3, LUO Genggeng3, SUN Di2
1 Key Laboratory of Functional Materials and Applications of Fujian Province, School of Materials Science and Engineering, Xiamen University of Technology, Xiamen 361024, Fujian Province, P. R. China;
2 Key Lab of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, P. R. China;
3 College of Materials Science and Engineering, Huaqiao University, Xiamen 361021, Fujian Province, P. R. China
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Crystalline silver cluster compounds are highly interesting owing to their intriguing structure and potential technological application in luminescence, semiconductivity, and as precursors for nonlinear optical materials. Typically, the synthesis of silver clusters involves the use of protecting ligands such as thiolates, phosphines, and alkynes, which have been found to be critical for cluster size and shape tuning. Among these nanoclusters, pentacosanuclear silver clusters (Ag25) have only been reported with either thiolate ligands or phosphine ligands, while those bearing mixed protecting ligands are rather rare. In the course of our exploration of novel silver clusters, a new silver thiolate precursor (iPrC6H4SAg)n was used to construct nanosized silver clusters. In the presence of 1,3-bis(diphenyphosphino)propane (dppp) and CF3SO3Ag, the pentacosanuclear silver cluster[Ag25(SC6H4Pri)18(dppp)6](CF3SO3)7·CH3CN (designated as Ag25, HSC6H4Pri=4-t-isopropylthiophenol) ligated both by thiolate and phosphine ligands was obtained under ultrasonic reaction conditions. Yellow block crystals were isolated from the solution, whose molecular structure was elucidated by single-crystal X-ray analysis. The skeleton of the Ag25 cluster comprises a sandwich-like motif containing two structurally very similar cylinders sharing a metal-cluster plane. The core of each cylinder presents the overall shape of a twisted hexagonal cylinder made of two connected Ag3S3 units, with six sulfur atoms and six silver atoms alternating on a puckered drum-like surface. The metal-cluster plane contains one type of pure-Ag tetragons showing significant Ag…Ag argentophilic interactions. The optical properties of Ag25 were investigated in the solid state. A band gap of~2.5 eV was estimated for Ag25 from the optical absorption spectrum, suggesting this cluster to be a potential wide-gap semiconductor. This Ag25 cluster was also found to emit green luminescence at λ=505 nm and room temperature.



Keywords: Silver cluster   Crystal structure   Optical property   Luminescence   Argentophilicity  
Received: 2017-10-18 Accepted: 2017-11-08 Publication Date (Web): 2017-11-09
Corresponding Authors: SUN Di, LUO Genggeng Email: dsun@sdu.edu.cn;ggluo@hqu.edu.cn

Fund: The project was supported by the National Natural Science Foundation of China (21641011, 21571115, 21701133), the Natural Science Foundation of Fujian Province, China (2015J01053) and the Fujian Key Laboratory of Functional Materials and Applications (fma2017107).

Cite this article: XIE An, WANG Zhi, WU Qiaoyu, CHENG Liping, LUO Genggeng, SUN Di. [Ag25(SC6H4Pri)18(dppp)6](CF3SO3)7·CH3CN (HSC6H4Pri =4-t-isopropylthiophenol, and dppp=1,3-bis(diphenyphosphino)propane) Cluster Containing a Sandwich-like Skeleton: Structural Characterization and Optical Properties[J]. Acta Phys. -Chim. Sin., 0, (): 0-0.    doi: 10.3866/PKU.WHXB201711091

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71. XIONG Jing; CAI Xiao-Qing; YIN Ping; HU Mao-Lin.Crystal Structure, Spectroscopic and Thermal Properties of 2-(toluene-4-sulfonylamino)-benzoic Acid[J]. Acta Phys. -Chim. Sin., 2007,23(08): 1183-1188
72. YANG Zi-Liang;YANG Si-Hai;LI Guo-Bao;LIN Jian-Hua.Synthesis, Structure and Thermal Properties of [HN(C2H5)3][B5O6(OH)4][J]. Acta Phys. -Chim. Sin., 2007,23(03): 285-288
73. GUO Jin-Yu;ZHANG Jian-Guo;ZHANG Tong-Lai;WU Rui-Feng;YU Wei.Thermal Decomposition Mechanisms of a Three-dimensional Framework Coordination Polymer [Cu(HCOO)2(H2O)2][J]. Acta Phys. -Chim. Sin., 2006,22(10): 1206-1211
74. YUAN Wei;LI He-Xian;WANG Ying;WANG Guo-Chang.Theoretical Prediction of Crystal Structure of N-(1-naphthyl) Succinimide Compound[J]. Acta Phys. -Chim. Sin., 2006,22(09): 1071-1074
75. WANG Shu-Jun;ZHANG Ying-Hui;RUAN Wen-Juan;LUO Dai-Bing;ZHU Zhi-Ang;TIAN Jian-Guo;LIU Zhi-Bo .Studies on the Synthesis and Characters of a Novel Chiral Metalloprophyrin[J]. Acta Phys. -Chim. Sin., 2006,22(08): 981-986
76. CHEN Zhe;YAN You-Wei .Combustion Synthesis and Luminescent Properties of blue-emitting Nanocrystalline Phosphor for PDP Application[J]. Acta Phys. -Chim. Sin., 2006,22(08): 1030-1033
77. CHEN Hu;XU Xing-You;GAO Jian;YANG Xu-Jie;LU Lu-De;WANG Xin.Study on Crystal Structure of [Ni(phen)3](ClO4)2[J]. Acta Phys. -Chim. Sin., 2006,22(07): 856-859
78. YANG Jian;QIU Tai;SHEN Chun-Ying.Synthesis and Characterization of a Novel Precursor for BCN Compound[J]. Acta Phys. -Chim. Sin., 2005,21(12): 1373-1377
79. WU Ai-ling; ZHAO Xian; GUAN Da-ren; YI Xi-zhang.Second Order Optical Nonlinearity in Substituted Benzene Systems: a Dynamical Lie Algebraic Treatment[J]. Acta Phys. -Chim. Sin., 2005,21(11): 1319-1323
80. WANG Shi-ming; LIU Ping; FU Xian-zhi.Preparation and Optical Properties of Nanocrystalline Cadmium Sulfide in Perfluorinated Ionomer Membrane[J]. Acta Phys. -Chim. Sin., 2005,21(10): 1151-1155
81. WANG Shu-jun; LUO Dai-bing; RUAN Wen-juan; ZHU Zhi-ang; MA Yi.Nonlinear Optical Properties and Conformational Study on Molecular Recognition of Imidazole Derivatives by Chiral Zinc Porphyrins[J]. Acta Phys. -Chim. Sin., 2005,21(08): 834-839
82. LI Lin-yan; LI Guo-bao; LIAO Fu-hui; LIN Jian-hua.Synthesis and Structure of La[B5O8(OH)(H2O)]NO3•2H2O[J]. Acta Phys. -Chim. Sin., 2005,21(07): 769-773
83. Shi Xue-Song;Du Miao;Bu Xian-He.Development of the Coordination Chemistry of Diazamesocycles[J]. Acta Phys. -Chim. Sin., 2004,20(08S): 917-923
84. Li Zeng-He;Yin Chen;Wang Ru-Ji;Wang Ping;Guo Hong-You.Synthesis and Crystal Structure of an Inorganic-Organic Hybrid CompoundCo(μ2-bpy)V2O6 (bpy=4,4’-bipyridine)[J]. Acta Phys. -Chim. Sin., 2003,19(12): 1133-1137
85. Wang Wen-Zhi;Fan Neng-Ting.Synthesis and Crystal Structure of 4,4’-Oxobis(propham)[J]. Acta Phys. -Chim. Sin., 2003,19(01): 75-78
86. Ning Jia-Cheng;Yang Ao;Guan Ye-Di;Wang Zhe-Ming;Yan Chun-Hua.The Resolution of the Optical Active Derivatives of Ketorolac and the Determination of its Absolute Configuration[J]. Acta Phys. -Chim. Sin., 2002,18(09): 821-824
87. Zhang Hao;Suo Quan-Ling;Wang Yi-Bin;Wang Li;Weng Lin-Hong;Leng Xue-Bing.Synthesis and Crystal Structure of (μ3-S)FeCo2(CO)7(dppfe)[J]. Acta Phys. -Chim. Sin., 2002,18(08): 746-749
88. Liu Guang;Zhang ShiWei.Synthesis and Structure of a Novel 18Mo Polyoxomolybdate[J]. Acta Phys. -Chim. Sin., 2002,18(07): 624-628
89. Li Qi;Wen Xiao-Quan;Cai Xiao-Hai;Wang Xian-Rong;Xie You-Chang.Software BVStr for Analyzing the Structure of Crystal and Surface Based on the Bond Valence Theory[J]. Acta Phys. -Chim. Sin., 2002,18(06): 558-562
90. Song Xiang-Zhi;Liu Guang;Zhang Shi-Wei.Synthesis and Crystal Structures of Cancer Cell Inducers of Differentiation PMDH[J]. Acta Phys. -Chim. Sin., 2002,18(06): 545-549
91. Lu Xue-Fang;Zhang Hai-Rong;Li Yi;Liu Jing;Yang Guo-Qiang.Luminescence Properties and Crystal Structure of Two Metal 8-hydroxyquinoline Complexes at High Pressure[J]. Acta Phys. -Chim. Sin., 2001,17(10): 898-903
92. Liu Xin-Mei;Yan Zi-Feng;Wang Huai-Ping.Optimization of Zeolite for Producing Lighter Olefin and Diesel in FCC Process[J]. Acta Phys. -Chim. Sin., 2001,17(06): 547-551
93. Zeng Xi-Rui;Zhang Yong;You Xiao-Zeng.Substituent Effect of the Peroxyoxalate Chemiluminescence[J]. Acta Phys. -Chim. Sin., 2001,17(04): 361-363
94. Wu Hong-Ying;Wang Xi-Gui;Xie Da-Tao;Weng Shi-Fu;Wu Jin-Guang.Structure and Luminescence Properties of Tb-doped Sibased Light-emitting[J]. Acta Phys. -Chim. Sin., 2001,17(01): 53-58
95. Li Fu-You, Zheng Jie, Liu Ting-Ting, Jin Lin-Pei, Zhao Xin-Sheng, Guo Jian-Quan.Photochemistry and Photoelectrochemistry of Donor-π-acceptor Azo-methine Dyes*[J]. Acta Phys. -Chim. Sin., 2000,16(09): 787-791
96. Zhao Bo, Zhang Dao, Cao Yang, Chen Wen-Jian, Sun Zhen-Rong, Wang Zu-Geng.Analysis of the Second-order Nonlinear Optical Properties of some Chalcones[J]. Acta Phys. -Chim. Sin., 2000,16(05): 422-425
97. Zhang Wen-Qin, Zhang Zhi-Ming, Zheng Yan, Wang Shu-Li, Zhao Shu-Na.Crystal Structure and Photochemical Properties of r-1,c-2,t-3,t-4-1,3-bis(4-biphenyl)-2,4-di(4-pyridyl)cyclobutane[J]. Acta Phys. -Chim. Sin., 2000,16(03): 207-213
98. Chen Zhen, Wang Ru-Ji.Synthesis of Transition Metal Chalcogenide [M(en)3]2Sn2Se6(M=Mn,Zn) and Studies of Thermogravimeric Properties[J]. Acta Phys. -Chim. Sin., 1999,15(12): 1070-1075
99. Miao Fang-Ming, Fan Zhi, Zhou Wei-Hong, Qi Li-Ning, Li Ai-Xiu, Liu Xiao-Lan.Synthesis and Crystal Structure and Quantum Chemistry of Tris(2-benzimidazylmethyl)amine with Manganese(II)[J]. Acta Phys. -Chim. Sin., 1999,15(09): 775-782
100. Wang Xiao-Ling, Suo Quan-Ling, Wang Yi-Bing, Sun Jie.Synthesisi and Crystal Structure of FeCo2(CO)73-S)(O[P(SCH2)2]2)[J]. Acta Phys. -Chim. Sin., 1999,15(08): 757-760
101. Ding Er-Run, Wu Shu-Lin, Li Qing-Shan, Yin Yuan-Qi.Synthesis,Structural Characterization and Reaction of the Chiral Clusters[J]. Acta Phys. -Chim. Sin., 1999,15(03): 241-246
102. Wei Kun, Shi Yan, He Lun-Yan.Crystal Structure and Infrared Spectra of Nanocrystalling Rare Earth Mixed Oxides Dy1-xSrxCoO3-y[J]. Acta Phys. -Chim. Sin., 1998,14(10): 957-960
103. Li Yue-Qing, Deng Li-Zhi, Zhou Xiao-Hai, Zhang Shao-Hui, Yang Qing-Chuan.The Crystal Structure and the Second Harmonic Generation Efficiency of the Sulfosalicylate[J]. Acta Phys. -Chim. Sin., 1998,14(09): 778-783
104. Chen Xue-An,Zhao Ling,Li Yan,Chen Ben-Ming.Preparation and Crystal Structure of PbCuP2O7[J]. Acta Phys. -Chim. Sin., 1997,13(02): 113-118
105. Zhuang Hong-Hui,Wu Ding-Ming,Huang Jian-Quan,Huang Jin-Ling.Synthesis and Crystal Structure of [Cu4Cl4(TTTA)2][J]. Acta Phys. -Chim. Sin., 1996,12(08): 761-765
106. Lu Qing-Wei,Wang Yi-Bing,Suo Quan-Ling,Wu Bao-Shan,Sun Jie.Synthesis and Crystal Strucutre of Fe3(CO)8(C6H5NC)(μ3-S)2[J]. Acta Phys. -Chim. Sin., 1996,12(06): 532-536
107. Jin Xiang-Lin,Jiang Yi-Jia,Zhang Shi-Wei,Tang You-Qi.Synthesis and Crystal Structure of the Imidazale-bridged Dicopper(II) Complex with Tetraaza Macrocycles[J]. Acta Phys. -Chim. Sin., 1995,11(10): 932-936
108. Miao Fang-Ming, Liu Xiao-Lan, Chen Hong-Li, Cui Xue-Qi, Wang Hong-Gen, Wang Ru-Ji, Yao Xin-Kan.Synthesis and Structural Study of Bis(N-Phenylsalicylaldiminato)(1,10-Phenanthroline) Co(II)[J]. Acta Phys. -Chim. Sin., 1995,11(09): 824-827
109. Guo Jin-Liang,Sun Feng,Li Yong,Dong Chang-Xiong.Crystal Structure of Dichloro-(5,10,15,20-tetraphenylporphinato) phosphorus(V) Chloride Dichloromethane Solvate[J]. Acta Phys. -Chim. Sin., 1995,11(04): 360-364
110. Hou Yong-Kang, Gao Min, Li Li-Pu, Ma Zhi-Mei.Studies of Trail and Error Method for Cyrstal Structural Determinations(III) Application and Program System of SYSTEM 90[J]. Acta Phys. -Chim. Sin., 1994,10(12): 1087-1092
111. Wu Bing-Fang, Su Hai-Quan, Yan Xiu-Ying, Hu Xiang, Liu Shu-Tang, Liu Qi-Wang, Shi Jian-Qiu.Synthesis and Crystal Structure of Rh2(μ-SC6H5)2(CO)4[J]. Acta Phys. -Chim. Sin., 1994,10(09): 847-851
112. Zhang Bin, Wang Zhe-Min, Liu Shi-Xiong, Huang Jin-Ling.Synthesis and Crystal Structure of a New Metal-rich Layered Ternary Tantalum Telluride TaNi2Te2[J]. Acta Phys. -Chim. Sin., 1994,10(06): 508-513
113. Wang Zhe-Min, Guan Tie-Tang, Zhuang Hong-Hui.Crystal Structure of Soft X-Ray Analyzer Crystal——Octadecyl Hydrogen Maleate(OHM, C22H40O4)[J]. Acta Phys. -Chim. Sin., 1994,10(05): 413-417
114. Zheng Ji-Min, Che Yun-Xia, Wang Ru-Ji, Wang Hong-Gen.Crystal Structure of 1:1 Adduct of Glycine and m-nitrobenzoic Acid[J]. Acta Phys. -Chim. Sin., 1994,10(01): 64-68
115. Ma Jian-Fang; Wei Ge-Cheng; Ni Jia-Zuan.Syntheses and Crystal Structures of the Complexes of rare Earth with Fumaric Acid[J]. Acta Phys. -Chim. Sin., 1993,9(06): 752-759
116. Yang Qing-Chuan; Dai Sheng; Zhou Hong-Bing; Zhou Qi-Feng; Tang You-Qi.The Molecular and Crystal Structures and Thermal Properties of the Mesogenic 2,5-BIS(4-Ethylbenzoyl) Oxystyrene and 2,5-BIS(4-Methoxybenzoyl) Oxybenzaldehyde[J]. Acta Phys. -Chim. Sin., 1993,9(06): 795-801
117. Ye Dai-Qi; Liang Hong; Huang Zhong-Tao.Study on the Interaction Between the Active Phase and Support on V2O5/TiO2 Catalyst[J]. Acta Phys. -Chim. Sin., 1993,9(04): 501-508
118. Zhuang Hong-Hui; Wu Ding-Ming; Lu Can-Zhong; Tong Wen.Synthesis and Crystal Structure of (C5H7S2)2[Cu3I5][J]. Acta Phys. -Chim. Sin., 1993,9(04): 548-552
119. Wu Bing-Fang; Yan Xiu-Ying; Liu Qi-Wang; Liu Shu-Tang; Hu Xiang.Synthesis and Crystal Structure of Cluster (μ-SC6H5)(μ-P(SC6H5)2)Fe2(CO)6[J]. Acta Phys. -Chim. Sin., 1992,8(06): 749-752
120. Zeng Guang-Fu; Guo Xin; Wang Cui-Ying; Lin Yong-Hua; Li Han.Infrared Spectra and Crystal Structure of BIS-(Dimethoxylphosphato) Copper[J]. Acta Phys. -Chim. Sin., 1992,8(06): 778-782
121. Wang Zeng-Lin; Hu Ning-Hai; Niu Chun-Ji; Ni Jia-Zuan; Cui Ai-Li.Crystal Structure and Thermal Analysis of Erbium Complex with Benzene Acetic Acid[J]. Acta Phys. -Chim. Sin., 1992,8(05): 642-646
122. Du Shao-Bin; Wang Jin; Ma Fu-Tai; Zheng Hong-Yuan; Lou Hui; Jing Cheng-Heng.Correlation of Composition、Crystal Structure、Reducibility and Catalytic Oxidation Activity on La-Mn-Ni-O System[J]. Acta Phys. -Chim. Sin., 1992,8(05): 630-635
123. Fan Guang-Yu; Wang Huan-Zhong; Cui Xiu-Shan; Li Yun-Zheng; Zhu He-Sun.Crystal Structures of 1,2-Dimethyl-3-Indolmethyl-Idene Succinic Fulgide Anhydride and 1,2-Dimethyl-3-Indolylethylidene Succinic Fulgide Anhydride[J]. Acta Phys. -Chim. Sin., 1992,8(04): 545-549
124. Liu Yong-Sheng; Shu Ning-Cheng; Hu Ning-Hai.An Algebraic Method to Estimate General Type of Phases of Structure Factors[J]. Acta Phys. -Chim. Sin., 1992,8(02): 255-260
125. Liu Xiao-Lan; Sun Ming; Miao Fang-Ming; Li Yu-Gui; Wang Jian-Ji; Han Yu-Zhen; Xu Xiao-Jie.Crystal and Molecular Structure of 1-Oxo-4-(Substituent)-1-Phospha-2,6,7-Trioxacyclo(2,2,2) Octane[J]. Acta Phys. -Chim. Sin., 1992,8(01): 100-108
126. Huang Ming-Sheng; Zhang Peng; Zhang Ying; Yang Hua-Hui; Zheng Lan-Sun.Synthesisi and Structure of a new Polynuclear Silver Complex [Ag4(dppe)3(NO3)4][J]. Acta Phys. -Chim. Sin., 1991,7(06): 694-698
127. Jin Xiang-Lin; Tong You-Zhi; Xu Xiao-Jie; Tang You-Qi.The Synthesis and Crystal Structure of Thiocyanate-Bridged Bi-Copper(II) Macrocyclic Complex of 1,4,7,12,15,18-Hexaazacyclodocosane [Cu2(SCN)3(C16H38N6)]2(ClO4)2[J]. Acta Phys. -Chim. Sin., 1991,7(03): 323-328
128. Xin Min; Sun Xiao-Lin; Liu Qi-Wang; Hu Yu-Cai.The Crystal and Molecular Structure of β-Cyanoethyl-α-Ferrocenylhalogenbenzyl Ethers[J]. Acta Phys. -Chim. Sin., 1991,7(02): 136-139
129. Hu Sheng-Zhi; Chen Ming-Dan; Liu Xiao-Yun; Zhou Yuan-Lang.Crystal Structure and Molecular Mechanics Calculations of the Addition Product of Acetylacetone and Methyl 1-Naphthoate, C17H18O4[J]. Acta Phys. -Chim. Sin., 1991,7(02): 191-195
130. Hu Sheng-Zhi; Huang Ming-Sheng; Cheng Xian-En; Zhou Yuan-Lang.Crystal Structure and Molecular Mechanics Calculations of the Photodimerization Product of Acetylacetone, C10H16O4[J]. Acta Phys. -Chim. Sin., 1991,7(02): 196-201
131. Shangguan Guo-Qiang; Zhang Shu-Gong; Jin Zhong-Sheng; Liu Shu-Ying; Ni Jia-Zuan.Crystal and Molecular Structures and MS Analyse of β-Carboxylethyl (or α-methylethyl) Germanium Trichlorides[J]. Acta Phys. -Chim. Sin., 1991,7(02): 223-226
132. Yang Qing-Chuan; Li Yi-Li; Tang You-Qi; Fu Heng.Study on the Thermal Motion N-Phenylphthalimide and 2-Phenylquinoxaline in Solid State[J]. Acta Phys. -Chim. Sin., 1991,7(01): 77-81
133. FANG Lei, SUN Mingjun, CAO Xinrui, CAO Zexing.Mechanical and Optical Properties of a Novel Diamond-like Si(C≡C-C6H4-C≡C)4 Single-Crystalline Semiconductor:a First-Principles Study[J]. Acta Phys. -Chim. Sin., 0,(): 0-0
134. HAN Xue, YANG Jin, LIU Yingying, MA Jianfang.Syntheses and Luminescent Properties of Coordination Polymers Based on 1,2,4-Triazole-Substituted Resorcin[4]arene[J]. Acta Phys. -Chim. Sin., 0,(): 0-0
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