The role of halogens in Au–S bond cleavage for energy-differentiated catalysis at the single-bond limit

Physics

Text available via DOI:

https://doi.org/10.1038/s41467-023-43639-8
Final published version
Available under license: CC BY: Creative Commons Attribution 4.0 International License

Research output: Contribution to Journal/Magazine › Journal article › peer-review

Published

Standard

The role of halogens in Au–S bond cleavage for energy-differentiated catalysis at the single-bond limit. / Li, Peihui; Hou, Songjun ; Wu, Qingqing et al.
In: Nature Communications, Vol. 14, No. 1, 7695, 24.11.2023.

Research output: Contribution to Journal/Magazine › Journal article › peer-review

Bibtex

@article{46104a04d4a94a2581aef2e8f5e6fdd9,

title = "The role of halogens in Au–S bond cleavage for energy-differentiated catalysis at the single-bond limit",

abstract = "The transformation from one compound to another involves the breaking and formation of chemical bonds at the single-bond level, especially during catalytic reactions that are of great significance in broad fields such as energy conversion, environmental science, life science and chemical synthesis. The study of the reaction process at the single-bond limit is the key to understanding the catalytic reaction mechanism and further rationally designing catalysts. Here, we develop a method to monitor the catalytic process from the perspective of the single-bond energy using high-resolution scanning tunneling microscopy single-molecule junctions. Experimental and theoretical studies consistently reveal that the attack of a halogen atom on an Au atom can reduce the breaking energy of Au−S bonds, thereby accelerating the bond cleavage reaction and shortening the plateau length during the single-molecule junction breaking. Furthermore, the distinction in catalytic activity between different halogen atoms can be compared as well. This study establishes the intrinsic relationship among the reaction activation energy, the chemical bond breaking energy and the single-molecule junction breaking process, strengthening our mastery of catalytic reactions towards precise chemistry.",

author = "Peihui Li and Songjun Hou and Qingqing Wu and Yijian Chen and Boyu Wang and Haiyang Ren and Jinying Wang and Zhaoyi Zhai and Zhongbo Yu and Lambert, {Colin J.} and Chuancheng Jia and Xuefeng Guo",

year = "2023",

month = nov,

day = "24",

doi = "10.1038/s41467-023-43639-8",

language = "English",

volume = "14",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Publishing Group",

number = "1",

}

RIS

TY - JOUR

T1 - The role of halogens in Au–S bond cleavage for energy-differentiated catalysis at the single-bond limit

AU - Li, Peihui

AU - Hou, Songjun

AU - Wu, Qingqing

AU - Chen, Yijian

AU - Wang, Boyu

AU - Ren, Haiyang

AU - Wang, Jinying

AU - Zhai, Zhaoyi

AU - Yu, Zhongbo

AU - Lambert, Colin J.

AU - Jia, Chuancheng

AU - Guo, Xuefeng

PY - 2023/11/24

Y1 - 2023/11/24

N2 - The transformation from one compound to another involves the breaking and formation of chemical bonds at the single-bond level, especially during catalytic reactions that are of great significance in broad fields such as energy conversion, environmental science, life science and chemical synthesis. The study of the reaction process at the single-bond limit is the key to understanding the catalytic reaction mechanism and further rationally designing catalysts. Here, we develop a method to monitor the catalytic process from the perspective of the single-bond energy using high-resolution scanning tunneling microscopy single-molecule junctions. Experimental and theoretical studies consistently reveal that the attack of a halogen atom on an Au atom can reduce the breaking energy of Au−S bonds, thereby accelerating the bond cleavage reaction and shortening the plateau length during the single-molecule junction breaking. Furthermore, the distinction in catalytic activity between different halogen atoms can be compared as well. This study establishes the intrinsic relationship among the reaction activation energy, the chemical bond breaking energy and the single-molecule junction breaking process, strengthening our mastery of catalytic reactions towards precise chemistry.

AB - The transformation from one compound to another involves the breaking and formation of chemical bonds at the single-bond level, especially during catalytic reactions that are of great significance in broad fields such as energy conversion, environmental science, life science and chemical synthesis. The study of the reaction process at the single-bond limit is the key to understanding the catalytic reaction mechanism and further rationally designing catalysts. Here, we develop a method to monitor the catalytic process from the perspective of the single-bond energy using high-resolution scanning tunneling microscopy single-molecule junctions. Experimental and theoretical studies consistently reveal that the attack of a halogen atom on an Au atom can reduce the breaking energy of Au−S bonds, thereby accelerating the bond cleavage reaction and shortening the plateau length during the single-molecule junction breaking. Furthermore, the distinction in catalytic activity between different halogen atoms can be compared as well. This study establishes the intrinsic relationship among the reaction activation energy, the chemical bond breaking energy and the single-molecule junction breaking process, strengthening our mastery of catalytic reactions towards precise chemistry.

U2 - 10.1038/s41467-023-43639-8

DO - 10.1038/s41467-023-43639-8

M3 - Journal article

VL - 14

JO - Nature Communications

JF - Nature Communications

SN - 2041-1723

IS - 1

M1 - 7695

ER -

Research

Links

Text available via DOI: