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Cover Story of Nature Nanotechnology: A New Concept of Synergetic Catalysis over Neighboring Monomers
2018-05-09

Prof. ZENG Jie's group made a great breakthrough in single-atom catalysis. The researchers demonstrated the synergetic interaction between neighboring monomers by constructing atomically dispersed Pt atoms on MoS2 (Pt1/MoS2). On March 19th, the work was published on Nature Nanotechnology with the title of "Synergetic Interaction between Neighbouring Pt Monomers in CO2 Hydrogenation" and selected as the cover paper [Nature Nanotechnology, 2018, 13, 411-417].

Over the past decade, atomically dispersed catalysts drawn increasing research attention owing to the high atom utilization, low-coordination number of metal atoms, and strong metal-support interaction. Nowadays investigation on single-atom catalysis only focused on the isolated metal atoms or the interaction between metal atoms and supports. Whether the interaction between isolated active sites in single-atom catalysts exists still remains as a major question.

The researchers revealed the synergetic interaction between Pt monomers by facilely increasing the Pt mass loading up to 7.5% while still maintaining the atomic dispersion of Pt. In Pt1/MoS2, Pt atoms replaced Mo atoms in MoS2 nanosheets, wherein every Pt atom and its directly-bonded S atoms composed an "active center". When two active centers were partly overlapped or adjacent, the two relevant Pt atoms were regarded as neighboring monomers. During CO2 hydrogenation, neighboring Pt monomers exhibited higher activity than isolated ones. The researchers further investigated the catalytic mechanism of different types of Pt monomers by combining temperature-programmed desorption, in-situ diffuse reflectance infrared Fourier transform, and in-situ X-ray photoelectron spectroscopy, and density functional theory calculations. Mechanistic studies reveal that CO2 was converted into methanol without experiencing the formation of formic acid intermediates over isolated Pt monomers. In contrast, neighboring Pt monomers worked in synergy to alter reaction pathways, where CO2 undergoes sequential transformation into formic acid and methanol.

The work for the first time proposes the concept of synergetic catalysis over neighboring monomers and breaks the stereotype that the active centers in single-atom catalysts are isolated without any interaction. This work also shows that the synergy works via the coordinated atoms, offering a new research direction in single-atom catalysis.

This work was supported by the CAS, MOST, NSFC, and National Synchrotron Radiation Laboratory.

Cover image by WANG Guoyan and MA Yanbing

Source: http://www.nature.com/articles/s41565-018-0089-z

(Hefei National Laboratory for Physical Sciences at the Microscale & School of Chemistry and Materials Science )

http://en.ustc.edu.cn/highlight/201805/t20180510_316637.html


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