Surface chemistry at the solid–solid interface: mechanically induced reaction pathways of C8 carboxylic acid monolayers on copper

Literature Information

Publication Date 2021-08-16
DOI 10.1039/D1CP03170H
Impact Factor 3.676
Authors

Resham Rana, Robert Bavisotto, Kaiming Hou, Wilfred T. Tysoe


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Abstract

Mechano- or tribochemical processes are often induced by the large pressures, of the order of 1 GPa, exerted at contacting asperities at the solid–solid interface. These tribochemical process are not very well understood because of the difficulties of probing surface-chemical reaction pathways occurring at buried interfaces. Here, strategies for following surface reaction pathways in detail are illustrated for the tribochemical decomposition of 7-octenoic and octanoic acid adsorbed on copper. The chemistry was measured in ultrahigh vacuum by sliding either a tungsten carbide ball or a silicon atomic force microscope (AFM) tip over the surface to test a previous proposal that the nature of the terminal group in the carboxylic acid, vinyl versus alkyl, could influence its binding to the counterface, and therefore the reaction rate. The carboxylic acids bind strongly to the copper substrate as carboxylates to expose the hydrocarbon terminus. The tribochemical reaction rate was found to be independent of the nature of the hydrocarbon terminus, although the pull-off and friction forces measured by the AFM were different. The tribochemical reaction is initiated in the same way as the thermal reaction, by the carboxylate group tilting to eliminate carbon dioxide and deposit alkyl species onto the surface. This reaction occurs thermally at ∼640 K, but tribochemically at room temperature, producing significant differences in the rates and selectivities of the subsequent decomposition pathways of the adsorbed products.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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