Atomically intimate assembly of dual metal–oxide interfaces for tandem conversion of syngas to ethanol

IF 38.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Nature nanotechnology Pub Date : 2024-11-25 DOI:10.1038/s41565-024-01824-w

Shang Li, Li Feng, Hengwei Wang, Yue Lin, Zhihu Sun, Lulu Xu, Yuxing Xu, Xinyu Liu, Wei-Xue Li, Shiqiang Wei, Jin-Xun Liu, Junling Lu

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Abstract

Selective conversion of syngas to value-added higher alcohols (containing two or more carbon atoms), particularly to a specific alcohol, is of great interest but remains challenging. Here we show that atomically intimate assembly of FeO_x-Rh-ZrO₂ dual interfaces by selectively architecting highly dispersed FeO_x on ultrafine raft-like Rh clusters supported on tetragonal zirconia enables highly efficient tandem conversion of syngas to ethanol. The ethanol selectivity in oxygenates reached ~90% at CO conversion up to 51%, along with a markedly high space-time yield of ethanol of 668.2 mg g_cat⁻¹ h⁻¹. In situ spectroscopic characterization and theoretical calculations reveal that Rh-ZrO₂ interface promotes dissociative CO activation into CH_x through a formate pathway, while the adjacent Rh-FeO_x interface accelerates subsequent C–C coupling via nondissociative CO insertion. Consequently, these dual interfaces in atomic-scale proximity with complementary functionalities synergistically boost the exclusive formation of ethanol with exceptional productivity in a tandem manner.

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用于串联转化合成气为乙醇的双金属氧化物界面的原子紧密装配

选择性地将合成气转化为高附加值的高级醇类（含两个或两个以上碳原子），尤其是转化为特定醇类，是人们非常感兴趣的问题，但仍然具有挑战性。在这里，我们展示了通过选择性地在四方氧化锆上支撑的超细筏状 Rh 簇上构建高度分散的 FeOx，从而在原子上紧密装配 FeOx-Rh-ZrO2 双界面，实现了合成气到乙醇的高效串联转化。在一氧化碳转化率高达 51% 时，乙醇在含氧化合物中的选择性达到约 90%，同时乙醇的时空产率高达 668.2 mg gcat-1 h-1。原位光谱表征和理论计算显示，Rh-ZrO2 界面通过甲酸途径促进解离一氧化碳活化为 CHx，而相邻的 Rh-FeOx 界面则通过非解离一氧化碳插入加速随后的 C-C 耦合。因此，这些具有互补功能的双界面在原子尺度上相互靠近，以串联方式协同促进了乙醇的独家形成，并具有极高的生产率。

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来源期刊

Nature nanotechnology 工程技术-材料科学：综合

CiteScore

59.70

自引率

0.80%

发文量

196

审稿时长

4-8 weeks

期刊介绍： Nature Nanotechnology is a prestigious journal that publishes high-quality papers in various areas of nanoscience and nanotechnology. The journal focuses on the design, characterization, and production of structures, devices, and systems that manipulate and control materials at atomic, molecular, and macromolecular scales. It encompasses both bottom-up and top-down approaches, as well as their combinations. Furthermore, Nature Nanotechnology fosters the exchange of ideas among researchers from diverse disciplines such as chemistry, physics, material science, biomedical research, engineering, and more. It promotes collaboration at the forefront of this multidisciplinary field. The journal covers a wide range of topics, from fundamental research in physics, chemistry, and biology, including computational work and simulations, to the development of innovative devices and technologies for various industrial sectors such as information technology, medicine, manufacturing, high-performance materials, energy, and environmental technologies. It includes coverage of organic, inorganic, and hybrid materials.