Facilitated CO2 hydrogenation by strong metal-support interaction between Ni and BaCO3

IF 11.5 Q1 CHEMISTRY, PHYSICAL Chem Catalysis Pub Date : 2024-09-20 DOI:10.1016/j.checat.2024.101113
Wenhao Zhang, Didi Li, Changwei Liu, Zhaocong Jiang, Chuang Gao, Liang Shen, Qi Liu, Runfa Qiu, Haoyuan Gu, Cheng Lian, Jing Xu, Minghui Zhu
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Abstract

Strong metal-support interactions (SMSIs) have attracted increasing attention due to their geometric and electronic effects in improving catalytic performance. For the first time, an SMSI phenomenon between Ni and BaCO3 was discovered. We observed the migration of BaCO3 support onto metallic nickel nanoparticles following H2 reduction and CO2 hydrogenation. The resulting porous overlayer not only stabilized nickel nanoparticles from sintering but also increased the number of Ni-BaCO3 sites. The abundant Ni-BaCO3 sites significantly promote the adsorption and activation of CO2. We also found that both the hydrogen atmosphere and metallic nickel nanoparticles boost the decomposition of BaCO3, followed by its regeneration in a CO2 atmosphere. Furthermore, the CO2 hydrogenation atmosphere enables the sustainable decomposition-regeneration of BaCO3, remarkedly increasing the CO2 concentration at the Ni-BaCO3 interface. Ultimately, the promoted CO2 activation and localized CO2 enrichment at the Ni-BaCO3 interface collectively facilitate the CO2 hydrogenation reaction.

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镍和 BaCO3 之间强烈的金属-支撑相互作用促进了二氧化碳氢化
强金属-支撑相互作用(SMSIs)因其在改善催化性能方面的几何和电子效应而日益受到关注。我们首次发现了镍和 BaCO3 之间的 SMSI 现象。我们观察到在 H2 还原和 CO2 加氢过程中,BaCO3 支持物迁移到金属镍纳米粒子上。由此产生的多孔覆盖层不仅稳定了纳米镍颗粒,防止其烧结,还增加了 Ni-BaCO3 位点的数量。丰富的 Ni-BaCO3 位点极大地促进了二氧化碳的吸附和活化。我们还发现,氢气环境和金属纳米镍粒子都能促进 BaCO3 的分解,然后在二氧化碳环境中再生。此外,二氧化碳氢化气氛能使 BaCO3 持续分解-再生,显著提高 Ni-BaCO3 界面的二氧化碳浓度。最终,Ni-BaCO3 界面的二氧化碳活化和局部二氧化碳富集共同促进了二氧化碳氢化反应。
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来源期刊
CiteScore
10.50
自引率
6.40%
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0
期刊介绍: Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.
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