DataVXACS Applied Materials & InterfacesPaper
journal article·2023-07-19

Gold/Substituted Hydroxyapatites for Oxidative Esterification: Control of Thin Apatite Layer on Gold Based on Strong Metal–Support Interaction (SMSI) Results in High Activity

Ayako Taketoshi, Yuvaraj Gangarajula, Ryusei Sodenaga, Akihiro Nakayama, Mitsutaka Okumura, Norihito Sakaguchi, Toru Murayama, Tetsuya Shimada, Shinsuke Takagi, Masatake Haruta, Botao Qiao, Junhu Wang, Tamao Ishida

ACS Applied Materials & Interfaces· Volume 15· Issue 28
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Source abstract

Abstract

Gold nanoparticles (Au NPs) deposited on various cation- and anion-substituted hydroxyapatites (Au/sHAPs) show oxidative strong metal–support interaction (SMSI), wherein a thin layer of the sHAP covered the surface of the Au NPs by heat treatment in an oxidative atmosphere. Calcination of Au/sHAPs at 300 °C caused a partial SMSI and that at 500 °C gave fully encapsulated Au NPs. We investigated the influence of the substituted ions in sHAP and the degree of the oxidative SMSI on the catalytic performance of Au/sHAPs for oxidative esterification of octanal or 1-octanol with ethanol to obtain ethyl octanoate. The catalytic activity depends on the size of the Au NPs but not on the support used, owing to the similarity of the acid and base properties of sHAPs except for Au/CaFAP. The presence of a large number of acidic sites on CaFAP lowered the product selectivity, but all other sHAPs exhibited similar activity when the Au particle size was almost the same, owing to the similarity of the acid and base properties. Au/sHAPs_O 2 with SMSI exhibited higher catalytic activity than Au/sHAPs_H 2 without SMSI despite the fact that the number of exposed surface Au atoms was decreased by the SMSI. In addition, the oxidative esterification reaction proceeded even though the Au NPs were fully covered by the sHAP layer when the thickness of the layer was controlled to be less than 1 nm. The substrate can access the surfaces of the Au NPs covered by the thin sHAP layer (<1 nm), and the presence of the sHAP structure in close contact with the Au NPs resulted in significantly higher catalytic activity compared with that for fully exposed Au NPs deposited on the sHAPs. This result suggests that maximizing the contact area between the Au NPs and the sHAP support based on the SMSI enhances the catalytic activity of Au.
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Research context

NanomaterialsCatalysis & surfacesMaterials processing

OpenAlex topics: Catalytic Processes in Materials Science · Nanocluster Synthesis and Applications · Quantum Dots Synthesis And Properties

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Advanced Materials Chemistry, Graduate School of Engineering, Yokohama National University, 79-5 Tokiwadai, Hodogaya-ku, Yokohama 240-8501, Japan

Center for Advanced Mössbauer Spectroscopy, Mössbauer Effect Data Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China

CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China

Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami-osawa, Hachioji, Tokyo 192-0397, Japan

Department of Chemistry, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka 560-8531, Japan

Innovative Catalysis Science Division, Institute for Open and Transdisciplinary Research Initiatives, Osaka University, Suita, Osaka 565-0871, Japan

Laboratory of Integrated Function Materials, Center for Advanced Research of Energy and Materials, Faculty of Engineering, Hokkaido University, Kita 13 Nishi 8, Kita-ku, Sapporo, Hokkaido 060-8628, Japan

Yantai Key Laboratory of Gold Catalysis and Engineering, Shandong Applied Research Center of Gold Nanotechnology (AU-SDARC), School of Chemistry & Chemical Engineering, Yantai University, 30 Qingquan Road, Yantai 264005, China

Funding

Ministry of Education, Culture, Sports, Science and Technology · Ministry of Science and Technology of the People's Republic of China · Japan Society for the Promotion of Science · JKA Foundation · National Natural Science Foundation of China

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