Tuning NiCu alloy metallicity and acidity on worm-like SiO2 for stable levulinic acid hydrogenation

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-09-25 DOI:10.1016/j.apcata.2025.120601

Xuan Wang , Hao Zhang , Huan Xiang , Lin Wang , Fangli Jing , Wenhao Fang

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引用次数: 0

Abstract

The ammonia complexation-impregnation method was employed to disperse Ni and Cu species on worm-like SiO₂ (w-SiO₂). The resulting bimetallic Ni_xCu_y/w-SiO₂ demonstrated a significant influence of the Ni/Cu molar ratio (x/y) on structural properties, including crystalline phases, reducibility, chemical state, and acidity. Copper oxide can be reduced to metallic Cu⁰ in all samples, whereas the reduction of nickel species was strongly dependent on the Ni/Cu ratio. The formation of nickel silicates enhanced acidity when x/y < 1, while NiCu alloys formed at other ratios, as evidenced by XRD, XPS and in situ Rapid XAFS, which allowed to finely adjust and well coordinate the bimetallic sites and acidic property to promote the catalytic transfer hydrogenation of levulinic acid. Additionally, the bimetallic NiCu catalysts exhibited good coke resistance, with activity almost fully recoverable during four reaction-regeneration cycles.

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在蠕虫状SiO2上调节NiCu合金的金属丰度和酸度以稳定乙酰丙酸加氢

采用氨络合浸渍法将Ni和Cu分散在蠕虫状SiO2 （w-SiO2）上。所得到的双金属NixCuy/w-SiO2表明，Ni/Cu摩尔比（x/y）对结构性能（包括晶相、还原性、化学状态和酸度）有显著影响。在所有样品中，氧化铜都可以被还原为金属Cu0，而镍的还原则强烈依赖于Ni/Cu比。当x/y <； 1时，镍硅酸盐的形成增强了酸性，而在其他比例下形成NiCu合金，通过XRD， XPS和原位快速XAFS可以很好地调节和协调双金属位点和酸性，促进乙酰丙酸的催化转移加氢。此外，双金属NiCu催化剂表现出良好的抗焦炭性能，在4次反应再生循环中活性几乎完全恢复。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.