Scalable Atomic-Layer Tailoring of Abundant Oxide Supports Unlocks Superior Interfaces for Low-Metal-Loading Dehydrogenation

Yeonsu Kwak; Yu-Jin Lee; Seongeun Moon; Kimoon Lee; Safira Ramadhani; Eui-Rim On; Chang-Il Ahn; Son-Jong Hwang; Hyuntae Sohn; Hyangsoo Jeong; Suk Woo Nam; Chang Won Yoon; Yongmin Kim

doi:10.1002/anie.202417598

Scalable Atomic-Layer Tailoring of Abundant Oxide Supports Unlocks Superior Interfaces for Low-Metal-Loading Dehydrogenation

Angew Chem Int Ed Engl. 2024 Nov 6:e202417598. doi: 10.1002/anie.202417598. Online ahead of print.

Authors

Yeonsu Kwak^{1

2}, Yu-Jin Lee¹, Seongeun Moon¹, Kimoon Lee¹, Safira Ramadhani^{1

3}, Eui-Rim On^{1

4}, Chang-Il Ahn^{1

5}, Son-Jong Hwang⁶, Hyuntae Sohn^{1

7}, Hyangsoo Jeong^{1

4

7}, Suk Woo Nam¹, Chang Won Yoon^{1

5}, Yongmin Kim¹

Affiliations

¹ Center for Hydrogen and Fuel Cell Research, Korea Institute of Science and Technology (KIST), 5 Hwarang-ro 14-gil, Seoul, 02792, Republic of Korea.
² Current Address: Department of Chemical and Biomolecular Engineering, University of Delaware, 150 Academy Street, Newark, 19716, United States.
³ Department of Chemical and Biological Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul, 02841, Republic of Korea.
⁴ KHU-KIST Department of Converging Science and Technology, Kyung Hee University, 26 Kyungheedae-ro, Dongdaemun-gu, Seoul, 02447, Republic of Korea.
⁵ Current Address: Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), 77 Cheongam-Ro, Nam-Gu, Pohang, 37673, Republic of Korea.
⁶ Division of Chemistry and Chemical Engineering, California Institute of Technology, 1200 East California Boulevard, Pasadena, CA 91125, United States.
⁷ Division of Energy and Environment Technology, Korea Institute of Science and Technology (KIST) School, 5 Hwarang-ro 14-gil, Seoul, 02792, Republic of Korea.

PMID: 39505697
DOI: 10.1002/anie.202417598

Abstract

Liquid organic hydrogen carriers (LOHCs) offer a promising solution for global hydrogen infrastructure, but their practical application faces two key challenges: sluggish dehydrogenation processes and the reliance on catalysts with high noble metal loadings. This study presents a scalable approach to reduce noble metal usage while maintaining high catalytic activity. We synthesized an ultralow Pt content (0.1 wt %) catalyst using γ-Al₂O₃-based pellet support with atomic layer deposition (ALD) of TiO₂. Advanced characterization techniques reveal that the thin ALD-TiO₂ shell provides a heterogeneous interface, confining electronically rich Pt-nanoparticle ensembles. The catalyst outperforms both equivalent Pt-content catalysts and a commercial 0.5 wt % Pt/γ-Al₂O₃ catalyst in homocyclic LOHC dehydrogenation. This study provides insights into the beneficial role of ALD-engineered interfaces for catalytic supports and offers an efficient approach for scalable production of low-noble-metal-content catalysts, with implications for various catalytic processes.

Keywords: Atomic Layer Deposition; Dehydrogenation; Low-loading Catalysts; Methylcyclohexane; Titania (TiO2).

Abstract

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