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Gold Nanocatalysts Supported on Carbon for Electrocatalytic Oxidation

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Gold Nanocatalysts Supported on Carbon for Electrocatalytic Oxidation Dalton Transactions View Article Online PERSPECTIVE View Journal Gold nanocatalysts supported on carbon for electrocatalytic oxidation of organic molecules Cite this: DOI: 10.1039/c8dt01966e including guanines in DNA a,c b,c c,d c,d,e,f Zheng Chang, † Yue Yang,† Jie He * and James F. Rusling * Gold (Au) is chemically stable and resistant to oxidation. Although bulk Au is catalytically inert, nano- structured Au exhibits unique size-dependent catalytic activity. When Au nanocatalysts are supported on conductive carbon (denoted as Au@C), Au@C becomes promising for a wide range of electrochemical reactions such as electrooxidation of alcohols and electroreduction of carbon dioxide. In this mini-review, we summarize Au@C nanocatalysts with specific attention on the most recent achievements including the findings in our own laboratories, and show that Au nanoclusters (AuNCs, <2 nm) on nitrided carbon are excellent electrocatalysts for the oxidation of organic molecules including guanines in DNA. The Received 16th May 2018, state-of-the-art synthesis and characterization of these nanomaterials are also documented. Synergistic Accepted 20th July 2018 interactions among Au-containing multicomponents on carbon supports and their applications in elec- DOI: 10.1039/c8dt01966e trocatalysis are discussed as well. Finally, challenges and future outlook for these emerging and promising rsc.li/dalton nanomaterials are envisaged. aDepartment of Applied Chemistry of College of Science, Xi’an University of 1. Introduction Technology, Xi’an 710054, China b Department of Chemical Engineering, Nanjing University of Science and Technology, Gold (Au) is chemically stable and resistant to oxidation. Jiangsu 210094, China cDepartment of Chemistry, University of Connecticut, Storrs, CT 06269, USA. When it has a particle size in the low nanometer range, nano- E-mail: [email protected], [email protected] structured Au with unique size-dependent catalytic properties d Institute of Materials Science, University of Connecticut, Storrs, CT 06269, USA that diff er from those of its bulk counterpart has attracted con- e Department of Surgery and Neag Cancer Center, UConn Health, Farmington, siderable attention in catalysis.1–4 Relevant to this review, early Published on 20 July 2018. Downloaded by University of Connecticut on 9/6/2018 5:46:00 PM. 5:46:00 on 9/6/2018 of Connecticut by University Downloaded 2018. 20 July on Published CT 06032, USA examples reported by Haruta and others showed that small Au fSchool of Chemistry, National University of Ireland at Galway, Galway H91 TK33, Ireland nanoparticles (AuNPs, <5 nm) supported on a number of † These authors contributed equally. metal oxides are extremely active for low-temperature CO Zheng Chang is a lecturer at the Yue Yang is a PhD student of Department of Applied Materials Science and Chemistry of College of Science, Engineering at Nanjing Xi’an University of Technology, University of Science and China. She is currently working Technology (NUST), China. She with Professors Jie He and James currently works in the Hybrid F. Rusling at the Department of Materials Laboratory with Dr Jie Chemistry, University of He at the University of Connecticut (USA) as a visiting Connecticut as a visiting student. Professor. She received a PhD in She obtained her BSc degree in Chemistry at Northwest chemistry from NUST in 2015. University (China) in 2011. Her Her current research interests Zheng Chang research focuses on the design Yue Yang focus on the synthesis of bi- and synthesis of functional nano- metallic and transition metal particles and their applications in bioelectroanalytical chemistry oxide nanomaterials to understand their electrochemistry for and luminescence analysis. applications in fuel cells and clean energy. This journal is © The Royal Society of Chemistry 2018 Dalton Trans. View Article Online Perspective Dalton Transactions 5–7 8 oxidation, CO2 hydrogenation, catalytic combustion of etc. The merits of simple synthesis and superior conductivity 9 10 11 methanol, NO reduction, selective epoxidation of propene, have enormously enriched the practical applications of carbon 12 44–46 low-temperature water gas shift reactions, etc. All these supported noble metal nanocatalysts in electrocatalysis. results point out that AuNPs with a small size (<5 nm) are On the other hand, due to the relatively inert nature of carbon usually more catalytically active compared to larger ones and the weak interaction between Au and the support, AuNPs (>10 nm).13 Atomically precise alkylthiol-protected Au nano- tend to overgrow and aggregate. Thus, the modification and clusters (AuNCs, e.g., Au25, Au38 and Au144) with excellent size functionalization of the carbon surface, such as the introduc- control have been synthesized later via wet-chemical reduction. tion of hydroxyl groups and heteroatom doping, have become This further allows quantifying size-dependent catalytic useful tools to enhance the interaction of Au and carbon and 14,15 performance. thus to stabilize AuNPs supported on carbon. In addition, the In addition to the intrinsic size eff ect, the activity of Au synergistic eff ect of Au/support may vary the charge state of nanocatalysts can be influenced by the nature and morphology AuNPs, resulting in an electron-rich NP surface. In a recent of supports.16,17 The primary role of the support is to anchor study, we showed that electron-rich AuNCs supported on nanoparticles (NPs) onto its surface, preventing the NPs from nitrided carbon supports favor the adsorption of electrophile sintering and agglomerating during catalytic reactions. reactants like CO2; therefore, this can promote the activity and Supported Au nanocatalysts can be very stable and resistant selectivity for CO2 electroreduction in comparison with AuNCs from corrosion in harsh environments like strong acid/base on pristine carbon, due to the strong electronic interaction of and high temperature. There are many diff erent types of sup- Au/support.47 This will be discussed in detail in Section 2.3. ports used for adsorption and stabilization of AuNPs, such as Au-Based multicomponent nanocatalysts have attracted – metal oxide powder,18 21 magnetic microspheres,22,23 polymer much attention and benefited from the controllable synthesis 24–26 27,28 nanospheres or nanofibers, mesoporous silica, car- of bimetallic or multimetallic NPs. So, a second metal, such as 29–33 bonaceous supports, etc. Low-cost carbon supports have Ag, Co, Cu, Ni, Pd, Pt, Sn, etc., has been introduced in the shown to be superior compared to other supports in terms of syntheses to form Au-based binary or multicomponent nanoca- their conductivity, the cost of raw materials, resistance to talysts. It has been an effi cient strategy to reduce the noble strong acid or base and the possibility to control porosity and metal loading and show a remarkable enhancement of electro- 34,35 surface chemistry. A good example of the influence of the catalytic activity due to the multifunctionality synergistic support was shown by Benkó et al., where carbon-supported eff ects.48,49 As briefly summarized in Table 1, a variety of Au nanocatalysts (denoted Au@C) outperformed other Au heterogeneous reactions can be catalyzed by using multicom- 30,32,50–65 nanocatalysts supported on TiO2, SiO2 and CeO2 in CO oxi- ponent nanocatalysts. For example, incorporation of 35 dation and glucose oxidation reactions. Pt and Pd with Au can usually promote electrochemical reac- Various kinds of carbon materials have been extensively tions like methanol oxidation and oxygen reduction. 36,37 studied in electrocatalysis, including carbon nanotubes Meanwhile, the presence of Au could retain eff ective CO toler- 38 39 57,64 (CNTs), carbon nanofibers, two-dimensional graphene ance during the catalytic reaction. 40 oxide/reduced graphene oxide (GO/RGO), mesoporous The remainder of this review will discuss typical synthetic 41,42 carbon and hollow carbon nanospheres (HCNS), metal– routes for Au@C nanocatalysts. Next, we will focus on their Published on 20 July 2018. Downloaded by University of Connecticut on 9/6/2018 5:46:00 PM. 5:46:00 on 9/6/2018 of Connecticut by University Downloaded 2018. 20 July on Published 43 organic framework (MOF)-derived carbonaceous materials, fascinating applications for various electrocatalytic oxidative Jie He received his BS and MS James f. Rusling obtained his degrees in Polymer Materials B.Sc. degree in Chemistry from from Sichuan University and his Drexel University in 1969, and PhD in Chemistry from Ph. D. from Clarkson University Universite de Sherbrooke with in 1979. He is a Professor of Professor Yue Zhao. He then Chemistry at the University of worked as a postdoctoral fellow Connecticut and a Professor of at the University of Maryland Surgery at UConn Health. His with Professor Zhihong Nie. current research includes the In 2014, he joined the faculty development of nano-science of the University of Connecticut based arrays for cancer diagnos- where he is currently an tics, electro-optical and LC-MS/ Jie He Assistant Professor in Chemistry James F. Rusling MS arrays for toxicity screening, Department. His research and fundamental bioelectro- focuses on the design and synthesis of polymer/inorganic hybrid chemistry. He has authored over 400 research papers and several materials for bioinspired catalysis and renewable energy books, and he is an accomplished musician interested in Irish and conversion. American folk styles. Dalton Trans. This journal is © The Royal Society of Chemistry
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