Investigation of hydrogen spillover in atomically dispersed metal on WO3 for selective hydrogenation

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2025-02-04 DOI:10.1002/aic.18749

Yu Sun, Jie Gan, Bing Du, You Wang, Jieyi Yin, Sai Zhang

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引用次数: 0

Abstract

Optimizing kinetic barriers of hydrogen spillover for selective hydrogenation on supported catalysts with dual-active sites faces a significant challenge due to inherent contradiction between H₂ activation and *H transformation from metal to support. Herein, the adsorption energy of *H (E_ad(H)) on metal has been demonstrated as a viable descriptor for understanding hydrogenation on the WO₃ surface with dual-active sites of single-atom metals and oxygen vacancies. Theoretical simulations rationalize the optimized value of E_ad(H) of −2.49 eV for these dual-active sites. Furthermore, the absolute value (|ΔE_ad(H)|) between E_ad(H) and −2.49 eV was calculated to directly explore the catalytic activity of M₁/NR-WO₃. Among them, the Pt₁/NR-WO₃ catalysts with the lowest |ΔE_ad(H)| exhibited the weakened *H adsorption and enabled efficient H₂ activation, resulting in a TOF value of 170,480 h⁻¹ and >99.9% selectivity for the hydrogenation of p-chloronitrobenzene to p-chloroaniline. These findings provide new insights into the hydrogen spillover-promoted selective hydrogenation.

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.