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Progress in Chemistry 2020, Vol. 32 Issue (8): 1140-1157 DOI: 10.7536/PC200301 Previous Articles   Next Articles

• Review •

Assembling Effects of Surface Ligands on Metal Nanomaterials

Ruixuan Qin1, Guocheng Deng1, Nanfeng Zheng1,**()   

  1. 1. State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National & Local Joint Engineering Research Center for Preparation Technology of Nanomaterials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
  • Received: Revised: Online: Published:
  • Contact: Nanfeng Zheng
  • About author:
    ** e-mail:
  • Supported by:
    the National Key R&D Program of China(2017YFA0207304); National Natural Science Foundation of China(21890752); National Natural Science Foundation of China(21731005); National Natural Science Foundation of China(21721001); Fundamental Research Funds for Central Universities(20720180026)
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Surface ligands on metal nanomaterials play a crucial role in the controlled synthesis of metal nanoparticles with specific size and morphology. However, the detailed molecular-level structures of surface ligands are difficult to be determined by conventional characterizations, leading to our poor understanding over the effects of surface ligands on the chemical properties of metal nanomaterials. Benefiting from the development of metal nanoclusters and other model nanomaterials, increasing research effort has been devoted to revealing the detailed coordination structure of surface ligands on metal nanomaterials and their catalytic effects. The coordination of organic molecules on the metal surface can not only regulate the electronic structure of the surface metal, but also alter the periodic structure of the surface atoms. Moreover, the assembling of surface organic ligands can create 3D spatial structure on the metal surface for manipulating the interaction strength and configuration of reactants and intermediates with the catalytic surface. The interface created by having organic ligands modify metal surface can also lead to the formation of new catalytic sites for changing the catalytic reaction pathways to improve the catalytic activity and selectivity. The assembling effects of surface ligands on metal nanomaterials make them exhibit advantages of heterogeneous catalysis and homogeneous catalysis.

Contents

1 Introduction

2 Metal nanoclusters as the model system

2.1 Coordination structure of organic ligands

2.2 Ensemble effect of surface ligands

2.3 Nanoclusters as model catalysts

3 Hydrophobicity and hydrophilicity

4 Ensemble effect and steric effect

4.1 Ensemble effect of surface coordination

4.2 Steric effect of surface organic assembly

5 Electronic effect of surface organic ligands

6 Synergistic metal-organic catalytic interfaces

7 Conclusion and outlook

Key words: surface and interface coordination chemistry, metal nanomaterial, metal nanocluster, surface modification with organic ligands, assembling effects on surface, steric effect, electronic effect
Fig.1 The local coordination bonding structure and arrangement structure of ligands on the surface of metal nanomaterials are important factors determining their surface chemical properties
Fig.2 (a) The total structure of thiolated Au102 nanocluster(left) and the coordination structure(right) of the -SR-Au-SR- “staple” motif on the surface of the cluster[24]. Color: gold, inner Au atoms; dark green, surface + 1 valence Au atoms; yellow, S; gray, C; Red, O. Copyright 2007 American Association for the Advancement of Science.(b) The total structure of thiolated Ag44 nanocluster(left) and the coordination structure of its surface Ag2(SR)5 motif(right)[27]. Color: gold, core Ag atoms; dark green, surface and sub-surface Ag atoms; yellow, S; gray, C. Copyright 2013 Springer Nature
Fig.3 The local coordination structures of different surface ligands on typical ligand-stabilized metal nanoclusters.(a) Thoilates[30];(b~d) Alkynyl ligands[31,32,33,34,35];(e) Monodentate phosphines;(f) Carbon monoxide;(g) Halides
Fig.4 The total structures of metal nanoclusters stabilized by bulky ligands.(a) Cyclohexanethiolate-stabilized Ag206[43]. Copyright 2018 Oxford University Press.(b) 1-adamantanethiolate-stabilized Ag141[44]. Copyright 2017 American Chemical Society
Fig.5 (a) PA ligand on Au34Ag28(PA)34 nanoclusters promotes the hydrolytic oxidation of organosilanes[46]. Copyright 2016 American Chemical Society.(b) Pd3Cl cluster catalyzed Suzuki-Miyaura reaction[47]. Copyright 2017 American Chemical Society.(c) Cu25H10 nanocluster catalyzed ketone hydrogenation[42]. Copyright 2019 American Chemical Society
Fig.6 Polymerization of C2H2 on Pd NS enhanced hydrophobicity and styrene hydrogenation activity[48]. Copyright 2014 American Chemical Society
Fig.7 Volcano-shape relationship between the promotional effect of ILs on Pt NPs for ORR and the alkyl chain length of ILs[49]. Copyright 2018 American Chemical Society
Fig.8 Selectivities of Cu catalyzed CO2RR with different modifiers[52]. Copyright 2019 American Chemical Society
Fig.9 Schematic(a) and TEM images(b, c) of PdAu NPs in zeolite with hydrophobic silicane modification[55]. Copyright 2020 American Association for the Advancement of Science
Fig.10 Schematic of SAM on Pd(111)[57]. Copyright 2010 Springer Nature
Fig.11 Thiols with different structure prefer to occupy different surface site[61]. Copyright 2013 Springer Nature
Fig.12 Schematic of rigid oleylamine layer on Pt3Co NPs manipulate adsorption configuration of cinnamaldehyde[68]. Copyright 2012 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
Fig.13 SPhF2 modified Pd4S NS for semihydrogenation of internal alkynes[31]. Copyright 2018 Elsevier Inc
Fig.14 Interaction model of ethyl pyruvate and cinchonidine over Pt surface[73]. Copyright 2004 American Chemical Society
Fig.15 Organic ligands enhance photoluminescence quantum yield of QDs[83]. Copyright 2013 American Chemical Society
Fig.16 Electronic effect of ethylenediamine on Pt NWs for selective hydrogenation of nitrobenzene to N-hydroxylaniline[89].(a) TEM image of Pt NWs,(b) Bader charge analysis of Pt,(c) Schematic of nitrobenzene hydrogenation on Pt NWs. Copyright 2016 Springer Nature
Fig.17 Polymerization of tris(4-vinylphenyl)phosphine in FDU-12. The chelating of phosphine ligands to the encapsulated Pd NPs enhances catalytic activity and selectivity of hydrogenation[90]. Copyright 2018 American Chemical Society
Fig.18 Electronic effect of CO on Au(111) in promoting the adsorption of hydroxyl and electrooxidation of MeOH[97]. Copyright 2011 Springer Nature
Fig.19 Schematic illustration of the interaction between the RDS transition state of CO oxidation and the Pd surface(a) or POF modifiers with different functional group(b, c)[98]. Copyright 2019 Springer Nature
Fig.20 Schematics of adsorption configuration of hydroperoxide intermediates on pure Pd and HHDMA modified Pd surface[101]. Copyright 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
Fig.21 Proposed C=O group hydrogenation mechanism of L-proline modified Pt NPs[102]. Copyright 2015 American Chemical Society
Fig.22 (a) Schematic and energies of heterolytic H2 activation process by ethylene glycol ligands on TiO2.(b) Primary KIE in styrene hydrogenation catalyzed by Pd1/TiO2.(c) Benzaldehyde hydrogenation catalyzed by Pd1/TiO2, Pd/C, and H2PdCl4[110]. Copyright 2016 American Association for the Advancement of Science
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