Reversible Control of Hydrogenation of a Single Molecule
Satoshi Katano,1
Yousoo Kim,1*
Masafumi Hori,1,2
Michael Trenary,3
Maki Kawai1,2*
Low-temperature scanning tunneling microscopy was used to selectively
break the N-H bond of a methylaminocarbyne (CNHCH
3) molecule
on a Pt(111) surface at 4.7 kelvin, leaving the C-H bonds intact,
to form an adsorbed methylisocyanide molecule (CNCH
3). The methylisocyanide
product was identified through comparison of its vibrational
spectrum with that of directly adsorbed methylisocyanide as
measured with inelastic electron tunneling spectroscopy. The
CNHCH
3 could be regenerated in situ by exposure to hydrogen
at room temperature. The combination of tip-induced dehydrogenation
with thermodynamically driven hydrogenation allows a completely
reversible chemical cycle to be established at the single-molecule
level in this system. By tailoring the pulse conditions, irreversible
dissociation entailing cleavage of both the C-H and N-H bonds
can also be demonstrated.
2 Department of Advanced Materials, University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8651, Japan.
3 Department of Chemistry, University of Illinois at Chicago, 845 West Taylor Street, Chicago, IL 60607–7061, USA.
* To whom correspondence should be addressed. E-mail: maki{at}riken.jp (M.K.); ykim{at}riken.jp (Y.K.)
