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Featured researches published by Hai-Feng Su.


Journal of the American Chemical Society | 2015

Total Structure and Electronic Structure Analysis of Doped Thiolated Silver [MAg24(SR)18]2– (M = Pd, Pt) Clusters

Juanzhu Yan; Hai-Feng Su; Huayan Yang; Sami Malola; Shui-Chao Lin; Hannu Häkkinen; Nanfeng Zheng

With the incorporation of Pd or Pt atoms, thiolated Ag-rich 25-metal-atom nanoclusters were successfully prepared and structurally characterized for the first time. With a composition of [PdAg24(SR)18](2-) or [PtAg24(SR)18](2-), the obtained 25-metal-atom nanoclusters have a metal framework structure similar to that of widely investigated Au25(SR)18. In both clusters, a M@Ag12 (M = Pd, Pt) core is capped by six distorted dimeric -RS-Ag-SR-Ag-SR- units. However, the silver-thiolate overlayer gives rise to a geometric chirality at variance to Au25(SR)18. The effect of doping on the electronic structure was studied through measured optical absorption spectra and ab initio analysis. This work demonstrates that modulating electronic structures by transition-metal doping is expected to provide effective means to manipulate electronic, optical, chemical, and catalytic properties of thiolated noble metal nanoclusters.


Journal of the American Chemical Society | 2016

Hierarchical Assembly of a {MnII15MnIII4} Brucite Disc: Step-by-Step Formation and Ferrimagnetism

Yong-Kai Deng; Hai-Feng Su; Jia-Heng Xu; Wenguang Wang; Mohamedally Kurmoo; Shui-Chao Lin; Yuan-Zhi Tan; Jiong Jia; Di Sun; Lan-Sun Zheng

In search of functional molecular materials and the study of their formation mechanism, we report the elucidation of a hierarchical step-by-step formation from monomer (Mn) to heptamer (Mn7) to nonadecamer (Mn19) satisfying the relation 1 + Σn6n, where n is the ring number of the Brucite structure using high-resolution electrospray ionization mass spectrometry (HRESI-MS). Three intermediate clusters, Mn10, Mn12, and Mn14, were identified. Furthermore, the Mn19 disc remains intact when dissolved in acetonitrile with a well-resolved general formula of [Mn19(L)x(OH)y(N3)36-x-y](2+) (x = 18, 17, 16; y = 8, 7, 6; HL = 1-(hydroxymethyl)-3,5-dimethylpyrazole) indicating progressive exchange of N3(-) for OH(-). The high symmetry (R-3) Mn19 crystal structure consists of a well-ordered discotic motif where the peripheral organic ligands form a double calix housing the anions and solvent molecules. From the formula and valence bond sums, the charge state is mixed-valent, [Mn(II)15Mn(III)4]. Its magnetic properties and electrochemistry have been studied. It behaves as a ferrimagnet below 40 K and has a coercive field of 2.7 kOe at 1.8 K, which can be possible by either weak exchange between clusters through the anions and solvents or through dipolar interaction through space as confirmed by the lack of ordering in frozen CH3CN. The moment of nearly 50 NμB suggests Mn(II)-Mn(II) and Mn(III)-Mn(III) are ferromagnetically coupled while Mn(II)-Mn(III) is antiferromagnetic which is likely if the Mn(III) are centrally placed in the cluster. This compound displays the rare occurrence of magnetic ordering from nonconnected high-spin molecules.


Journal of the American Chemical Society | 2015

An Intermetallic Au24Ag20 Superatom Nanocluster Stabilized by Labile Ligands

Yu Wang; Hai-Feng Su; Chaofa Xu; Gang Li; Lars Gell; Shui-Chao Lin; Zichao Tang; Hannu Häkkinen; Nanfeng Zheng

An intermetallic nanocluster containing 44 metal atoms, Au24Ag20(2-SPy)4(PhC≡C)20Cl2, was successfully synthesized and structurally characterized by single-crystal analysis and density funtional theory computations. The 44 metal atoms in the cluster are arranged as a concentric three-shell Au12@Ag20@Au12 Keplerate structure having a high symmetry. For the first time, the co-presence of three different types of anionic ligands (i.e., phenylalkynyl, 2-pyridylthiolate, and chloride) was revealed on the surface of metal nanoclusters. Similar to thiolates, alkynyls bind linearly to surface Au atoms using their σ-bonds, leading to the formation of two types of surface staple units (PhC≡C-Au-L, L = PhC≡C(-) or 2-pyridylthiolate) on the cluster. The co-presence of three different surface ligands allows the site-specific surface and functional modification of the cluster. The lability of PhC≡C(-) ligands on the cluster was demonstrated, making it possible to keep the metal core intact while removing partial surface capping. Moreover, it was found that ligand exchange on the cluster occurs easily to offer various derivatives with the same metal core but different surface functionality and thus different solubility.


CrystEngComm | 2012

Syntheses, structures and fluorescence of two coordination complexes of Zn(II) and 1,3-bis(2-methylimidazolyl)propane: solvent effect

Hong-Jun Hao; Fu-Jing Liu; Hai-Feng Su; Zhan-Hui Wang; Dan-Feng Wang; Rong-Bin Huang; Lan-Sun Zheng

Two Zn(II) coordination complexes, formulated as [Zn2(bmip)(tpa)2·2DMF]n (1) and [Zn(bmip)(tpa)·3H2O]n (2) (bmip = 1,3-bis(2-methylimidazolyl)propane, H2tpa = terephthalic acid, DMF = N,N-dimethylformamide) have been prepared by ultrasonic reactions of the flexible ligand bmip and aromatic dicarboxylic acid H2tpa with Zn(II) ions in various solvent systems. Both of these complexes have been characterized by elemental analyses, IR spectra, and single-crystal X-ray diffraction. As controlled by solvent systems, complex 1 is a 2-fold interpenetrating 3D framework with α-Po network topology, while, complex 2 reveals a 3-fold interpenetrating 3D framework with dia topology. Furthermore, the photoluminescence at room temperature and thermogravimetric properties of the complexes 1 and 2 were also investigated in the solid state.


Chemistry: A European Journal | 2016

General Assembly of Twisted Trigonal-Prismatic Nonanuclear Silver(I) Clusters

Xiao-Yu Li; Hai-Feng Su; Rui‐Qi Zhou; Sheng Feng; Yuan-Zhi Tan; Xing-Po Wang; Jiong Jia; Mohamedally Kurmoo; Di Sun; Lan-Sun Zheng

A general class of C3 -symmetric Ag9 clusters, [Ag9 S(tBuC6 H4 S)6 (dpph)3 (CF3 SO3 )] (1), [Ag9 (tBuC6 H4 S)6 (dpph)3 (CF3 SO3 )2 ]⋅CF3 SO3 (2), [Ag9 (tBuC6 H4 S)6 (dpph)3 (NO3 )2 ] ⋅NO3 (3), and [Ag9 (tBuC6 H4 S)7 (dpph)3 (Mo2 O7 )0.5 ]2 ⋅2 CF3 COO (4) (dpph=1,6-bis(diphenylphosphino)hexane), with a twisted trigonal-prism geometry was isolated by the reaction of polymeric {(HNEt3 )2 [Ag10 (tBuC6 H4 S)12 ]}n , 1,6-bis(diphenylphosphino)hexane, and various silver salts under solvothermal conditions. The structures consist of discrete clusters constructed from a girdling Ag9 twisted trigonal prism with the top and bottom trigonal faces capped by diverse anions (i.e., S(2-) and CF3 SO3 (-) for compound 1, 2×CF3 SO3 (-) for compound 2, 2×NO3 (-) for compound 3, and tBuC6 H4 S(-) and Mo2 O7 (2-) for compound 4). This trigonal prism is bisected by another shrunken Ag3 trigon at its waist position. Interestingly, two inversion-related Ag9 trigonal-prismatic clusters are dimerized by the Mo2 O7 (2-) ion in compound 4. The twist is amplified by the bulkier thiolate, which also introduces high steric-hindrance for the capping ligand, that is, the longer dpph ligand. Four more silver-sulfur clusters (namely, compounds 5-8) with their nuclearity ranging from 6-10 were solely characterized by single-crystal X-ray diffraction to verify the above-described synergetic effect of mixed ligands in the construction of Ag9 twisted trigonal prisms. Surprisingly, only cluster 1 emits yellow luminescence at λ=584 nm at room temperature, which may be attributed to a charge transfer from the S 3p orbital to the Ag 5s orbital, or mixed with metal-centered (MC) d(10) →d(9) s(1) transitions. Upon cooling from 300 to 80 K, the emission intensity was enhanced along with a hypsochromic shift. The good linear relationship between the maximum emission intensity and the temperature for compound 1 in the range of 180-300 K indicates that this is a promising molecular luminescent thermometer. Furthermore, cyclic voltammetric studies indicated that the diffusion- and surface-controlled redox processes were determined for compounds 1 and 3 as well as compound 4, respectively.


Proceedings of the National Academy of Sciences of the United States of America | 2017

Assembly of silver Trigons into a buckyball-like Ag180 nanocage

Zhi Wang; Hai-Feng Su; Yuan-Zhi Tan; Stan Schein; Shui-Chao Lin; Wei Liu; Shu-Ao Wang; Wenguang Wang; Chen-Ho Tung; Di Sun; Lan-Sun Zheng

Significance Here we present a striking outcome from the alliance between chemistry and mathematics in the design, synthesis, and characterization of a silver cage, Ag180. In principle, the design replaces each carbon atom of C60 with a triplet of argentophilicity-bonded silver atoms to produce a 3.4.6.4 (1,1) polyhedron with sixty 3-gons, ninety 4-gons, twelve 5-gons, and twenty 6-gons. Results from mass spectroscopy suggest an assembly mechanism in solution based on such triplets––the Silver-Trigon Assembly Road (STAR). Indeed, the STAR mechanism may be a general synthetic pathway toward even larger silver polyhedral cages. Besides its fundamental appeal, this synthetic cage may be considered for use as a molecular luminescent thermometer. Buckminsterfullerene (C60) represents a perfect combination of geometry and molecular structural chemistry. It has inspired many creative ideas for building fullerene-like nanopolyhedra. These include other fullerenes, virus capsids, polyhedra based on DNA, and synthetic polynuclear metal clusters and cages. Indeed, the regular organization of large numbers of metal atoms into one highly complex structure remains one of the foremost challenges in supramolecular chemistry. Here we describe the design, synthesis, and characterization of a Ag180 nanocage with 180 Ag atoms as 4-valent vertices (V), 360 edges (E), and 182 faces (F)––sixty 3-gons, ninety 4-gons, twelve 5-gons, and twenty 6-gons––in agreement with Euler’s rule V − E + F = 2. If each 3-gon (or silver Trigon) were replaced with a carbon atom linked by edges along the 4-gons, the result would be like C60, topologically a truncated icosahedron, an Archimedean solid with icosahedral (Ih) point-group symmetry. If C60 can be described mathematically as a curling up of a 6.6.6 Platonic tiling, the Ag180 cage can be described as a curling up of a 3.4.6.4 Archimedean tiling. High-resolution electrospray ionization mass spectrometry reveals that {Ag3}n subunits coexist with the Ag180 species in the assembly system before the final crystallization of Ag180, suggesting that the silver Trigon is the smallest building block in assembly of the final cage. Thus, we assign the underlying growth mechanism of Ag180 to the Silver-Trigon Assembly Road (STAR), an assembly path that might be further employed to fabricate larger, elegant silver cages.


Advanced Science | 2015

Single‐Crystalline Rhodium Nanosheets with Atomic Thickness

Li Zhao; Chaofa Xu; Hai-Feng Su; Jinghong Liang; Shui-Chao Lin; Lin Gu; Xingli Wang; Mei Chen; Nanfeng Zheng

CO confinement strategy for ultrathin Rh nanosheets: CO is introduced as a confining agent to regulate the anisotropic growth of unique 2D structure. The single‐crystalline Rh nanosheets have a thickness of three to five atomic layers and tunable edge length ranging from 500 to 1300 nm. By understanding the formation mechanism, surface‐clean Rh nanosheets are also prepared and display better catalytic performance that their surfactant‐capped nanosheets.


Journal of the American Chemical Society | 2018

Anisotropic Assembly of Ag52 and Ag76 Nanoclusters

Jia-Wei Liu; Lei Feng; Hai-Feng Su; Zhi Wang; Quan-Qin Zhao; Xing-Po Wang; Chen-Ho Tung; Di Sun; Lan-Sun Zheng

Although there has been an upsurge of interest in anisotropic assembly of inorganic nanoparticles, atomically precise self-assembly of anisotropic metal clusters is extremely rare. Herein, we presented two novel silver nanoclusters, Ag52 (SD/Ag23) and Ag76 (SD/Ag24), which are interiorly templated by five MoO42- and a pair of Mo6O228- anions, respectively, and coprotected by bridging RSH and terminal diphosphine ligands exteriorly. Regiospecific distribution diphosphine ligands on the surface and the arrangement of multiple molybdate templates within the nanoclusters synergetically tailor their shapes to anisotropic oblate spheroid and elongated rod, respectively. This work not only open up new avenues for the synthesis of silver nanoclusters with novel metal skeleton shapes and anisotropic surface structures but also give important insights for the anisotropic growth of silver nanoclusters through surface modifications or/and template organizations.


Journal of the American Chemical Society | 2017

Core–Shell {Mn7⊂(Mn,Cd)12} Assembled from Core {Mn7} Disc

Ling-Yu Guo; Hai-Feng Su; Mohamedally Kurmoo; Chen-Ho Tung; Di Sun; Lan-Sun Zheng

Postsynthetic decoration of the Mn7, {MnIII⊂MnII6}, core with CdII in the outer shell to form the next generation Mn13Cd6, {MnIII⊂MnIII3MnII3⊂ MnII6CdII6}, core-shell disc was achieved and confirmed by single-crystal X-ray diffraction. The formation of Mn13Cd6 has only been successful with CdII and if the Cd salt is added within the first half hour window when the inner Mn7 has formed. EDX and ICP-AES gave the accurate content and confirm the average found by X-ray diffraction. HR-ESI-MS was even more precise by revealing three prominent molecular species, Mn13Cd6, Mn14Cd5 and Mn15Cd4, having a distribution of metals. The presence of nonmagnetic metal on the periphery reduces the exchange between these clusters as well as the low magnetic moment decreases the dipolar interaction resulting in a paramagnet compared to the ferrimagnetism found for the parent Mn19, {MnIII⊂MnIII3MnII3⊂MnII12}, disc. This study opens the way for the syntheses of heterometallic core-shell clusters in a controllable fashion.


Journal of the American Society for Mass Spectrometry | 2009

Desorption electrospray ionization mass spectrometry for monitoring the kinetics of Baeyer-Villiger solid-state organic reactions

Ying Xie; Li-Fang He; Shui-Chao Lin; Hai-Feng Su; Su-Yuan Xie; Rong-Bin Huang; Lan-Sun Zheng

Desorption electrospray ionization mass spectrometry (DESI-MS) has been used for monitoring solid-state organic reaction in ambient air, specifically the Baeyer-Villiger (BV) type reaction involving the oxidation of ketones (benzophenone or deoxybenzoin) by m-chloroperbenzoic acid (m-CPBA) in solid-state. The DESI mass spectra obtained at regular intervals during the BV reaction processes are featured, with the amount of ester products increasing as those of ketone reactants decrease. Quantitative analyses of relative intensities of the product, made to quantify the reaction degree of typical solid-state organic reaction (SSOR), show a precision with RSDs of around 5% to 12%, though the RSDs for direct analysis of intensities of the reactant or the product in the solid-state are obviously larger. The kinetics of the Baeyer-Villiger type reactions in solid-state are shown to be dramatically different, in reaction rate, kinetic curve, as well as concentration dependence, from those of the same reactions taking place in solution.

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Di Sun

Shandong University

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Guilin Zhuang

Zhejiang University of Technology

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