TY - JOUR
T1 - Single-Atom Pt+Derived from the Laser Dissociation of a Platinum Cluster
T2 - Insights into Nonoxidative Alkane Conversion
AU - Liu, Zheyi
AU - Li, Zhimin
AU - Li, Guanna
AU - Wang, Zhipeng
AU - Lai, Can
AU - Wang, Xiaolei
AU - Pidko, Evgeny A.
AU - Xiao, Chunlei
AU - Wang, Fanjun
AU - Li, Gao
AU - Yang, Xueming
PY - 2020/7/7
Y1 - 2020/7/7
N2 - In this study, we construct a 193 nm ultraviolet laser dissociation high-resolution mass spectrometry (HRMS) platform to produce Pt+ cations with high efficiency, which is in situ applied for monitoring the "Pt+ + alkanes"reactions (where alkanes include methane, ethane, and propane). The conversion intermediates and products could be accurately determined by an orbitrap detector with high resolution (up to 150â»000). Importantly, methane conversion by Pt+ cations yields [Pt + ethane]+ and [Pt + ethylene]+ as the sole products formed via the cross-coupling reaction of the Pt-CH2 intermediate with gaseous methane. However, the Pt+ cations promote only the nonoxidative dehydrogenation of ethane and propane to give the corresponding [Pt + alkenes]+ and [Pt + alkynes]+. The details of the reaction mechanism are corroborated by density functional theory (DFT) calculations. These results highlight the power of HRMS with the laser dissociation of metal clusters in the generation and reaction characterization of metal ions.
AB - In this study, we construct a 193 nm ultraviolet laser dissociation high-resolution mass spectrometry (HRMS) platform to produce Pt+ cations with high efficiency, which is in situ applied for monitoring the "Pt+ + alkanes"reactions (where alkanes include methane, ethane, and propane). The conversion intermediates and products could be accurately determined by an orbitrap detector with high resolution (up to 150â»000). Importantly, methane conversion by Pt+ cations yields [Pt + ethane]+ and [Pt + ethylene]+ as the sole products formed via the cross-coupling reaction of the Pt-CH2 intermediate with gaseous methane. However, the Pt+ cations promote only the nonoxidative dehydrogenation of ethane and propane to give the corresponding [Pt + alkenes]+ and [Pt + alkynes]+. The details of the reaction mechanism are corroborated by density functional theory (DFT) calculations. These results highlight the power of HRMS with the laser dissociation of metal clusters in the generation and reaction characterization of metal ions.
U2 - 10.1021/acs.jpclett.0c01416
DO - 10.1021/acs.jpclett.0c01416
M3 - Article
C2 - 32633522
AN - SCOPUS:85089617756
SN - 1948-7185
VL - 11
SP - 5987
EP - 5991
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 15
ER -