DataVXACS Applied Materials & InterfacesPaper
journal article·2024-11-27Open access

Catalytic Synergy between Pd Nanoclusters and Ligand-Functionalized Layered Silicates for Improved Formic Acid Dehydrogenation

Esmail Doustkhah, Muhammed Yusufoğlu, Hamza El-Hosainy, Hamaneh Zarenezhad, Yusuke Ide, José Julio Gutiérrez Moreno, M. Hussein N. Assadi

ACS Applied Materials & Interfaces· Volume 16· Issue 47
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Source abstract

Abstract

The synthesis and stabilization of Pd nanoclusters on a support, as well as simultaneously achieving optimal catalytic activity, remain challenging tasks. Functionalizing the support surface with specific ligands offers a promising solution, but it often requires carefully balancing trade-offs between the reaction yield and catalyst stability. Here, we used two different ligands (propylamine and propylthiol) to functionalize the layered silicate’s interlayer surface for Pd nanocluster synthesis and stabilization. For dehydrogenating formic acid, Pd nanoclusters on aminopropyl groups achieved a catalytic activity ∼27-fold higher than that of thiopropyl groups at 70 °C. Our density functional calculations compared the adsorption energetics and bonding characteristics of single Pd atoms and Pd 13 nanoclusters on amino- and thio-functionalized silicate surfaces. Pd–N bonds were predicted to be weaker with minimal covalency, while Pd–S bonds exhibit greater covalency due to higher 4d–3p hybridization, resulting in better stability. However, Pd 13 clusters undergo severe structural deformation on thiol-functionalized surfaces, resulting in a smaller overall surface area and diminished catalytic stability.
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Research context

NanomaterialsCatalysis & surfaces

OpenAlex topics: Catalytic Processes in Materials Science · Carbon dioxide utilization in catalysis · Catalysis and Oxidation Reactions

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

Affiliations

Chemistry Department, Faculty of Engineering and Natural Sciences, Istinye University, Sariyer, Istanbul 34396, Türkiye

Koç University Tüpraş Energy Center (KUTEM), Istanbul 34450, Türkiye

Materials Science and Engineering, Koç University, Istanbul 34450, Türkiye

Research Center for Materials Nanoarchitechtonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan

Institute of Nanoscience and Nanotechnology, Kafrelsheikh University, Kafrelsheikh 33511, Egypt

Graduate School of Engineering Science, Yokohama National University, 79-5 Tokiwadai, Hodogaya-ku, Yokohama 240-8501, Japan

Barcelona Supercomputing Center, Plaça d’Eusebi Güell, 1-3, Barcelona 08034, Spain

RIKEN Center for Emergent Matter Science (CEMS), 2-1 Hirosawa, Wako, Saitama351-0198, Japan

Funding

European Research Council · Agencia Estatal de Investigaci?n · T?rkiye Bilimsel ve Teknolojik Arastirma Kurumu · Japan Science and Technology Corporation

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