Light-Driven Metal Exsolution-Redissolution of High-Entropy Oxide Enabling High-Performance Dry Reforming of Methane.
basic_science · Level V
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- Record sourced from PubMed, PMID 40190194.
- Also identified by DOI 10.1002/adma.202500928.
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Abstract
Solar-driven dry reforming of methane (DRM) is attractive for syngas production as an energy-efficient and environmentally friendly process. However, the remaining challenges of low yield and coke-induced inability in this route severely limit its applicability. Here, a light-induced metal exsolution-dissolution strategy is reported using high-entropy oxide (HEO) as a support for highly active and durable photothermal DRM. As evidenced by structural characterizations and theoretical simulations, the metal exsolution-dissolution process triggers the chemical looping of oxygen vacancies on HEO, in which CH<sub>4</sub> is activated to CO and H<sub>2</sub> by lattice oxygen while oxygen from CO<sub>2</sub> can fill the oxygen vacancy and release CO. Such a pathway greatly improves product formation and coking resistance, overcoming the limitations. As a result, the optimized CoNiFeZnCr-HEO supported Rh nanocomposite achieves a high H<sub>2</sub>/CO production of 0.242/0.246 mol g<sup>-1</sup> h<sup>-1</sup> with a balance selectivity of 0.98 and impressive long-term stability (200 h). The yield is ≈300 and 450 times higher than that of quaternary and ternary oxides-based catalysts, respectively. This work paves the way for new insights into the light-driven DRM process and highlights the integration of dynamic surface evolution with molecular activation to enhance catalytic performance.