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UID:20250810T083725EDT-9387WSn3ed@132.216.98.100
DTSTAMP:20250810T123725Z
DESCRIPTION:The design of new technologies that shift U.S. power consumptio
 n away from fossil fuels toward sustainable alternatives must take into ac
 count the nation's large-scale need for stored chemical fuels. Photoelectr
 ocatalytic CO2 reduction is one such technology\, since it facilitates a p
 rocess whereby solar energy is used to reduce CO2\, a combustion product\,
  into chemical fuels that are compatible with the existing U.S. energy inf
 rastructure.\n\nWe report here on experimental studies of well-defined sur
 faces to investigate the role of the electrode surface in pyridine-catalyz
 ed CO2 reduction\, which is reported to be associated with high yields for
  methanol and formic acid. Ambient pressure photoelectron spectroscopy (AP
 PES) was used to spectroscopically identify in situ surface-bound species 
 formed by the interaction of water on GaP(110)\, the most stable surface o
 f GaP\, at pressures up to 1 Torr. The data show that the interaction with
  water is characterized by the presence of a partially dissociated adlayer
 \, with Ga-OH\, P-H\, and adsorbed molecular H2O species detected on the s
 urface. This is consistent with previously published theoretical work that
  predicts the presence of this layer. In addition\, we used isobaric APPES
  measurements at elevated pressures to probe the thermal stabilities of ad
 sorbed species as well as the oxidation of surface Ga and P. We observe th
 e surface hydride to be remarkably stable in the presence of water\, which
  is notable given the critical role of hydride transfer to catalysts and C
 O2 during chemical fuel synthesis reactions in aqueous environments. It is
  hypothesized that the high observed stability of the hydride on GaP may c
 ontribute to its associated remarkable near-100% faradaic efficiency for m
 ethanol generation by solar-driven CO2 reduction. We have also obtained or
 bital-resolved information on the adsorption state of pyridine (C5H5N) on 
 GaP(110) using scanning tunneling microscopy (STM). By examining the distr
 ibution of unoccupied molecular orbitals with high spatial and energetic r
 esolution\, we showed that scanning probe techniques can be used to positi
 vely identify the sites on pyridine susceptible to nucleophilic attack\, c
 onsistent with frontier orbital theory. This technique can be used to expl
 ore the local reaction centers of adsorbed catalysts relevant to artificia
 l photosynthesis. Our observations of the stable adsorption of both H and 
 pyridine on this surface is notable\, because it characterizes the propose
 d precursor state for the formation of adsorbed dihydropyridine\, which co
 uld be a key hydride-shuttling catalyst for heterogeneous CO2 reduction.\n
 \n \n\n \n
DTSTART:20170621T170000Z
DTEND:20170621T183000Z
LOCATION:room 10\, Maass Chemistry Building\, CA\, QC\, Montreal\, H3A 0B8\
 , 801 rue Sherbrooke Ouest
SUMMARY:The role of the Electrode Surface in Solar-Driven Pyridine-Catalyze
 d CO2 Reduction
URL:/tised/channels/event/role-electrode-surface-solar
 -driven-pyridine-catalyzed-co2-reduction-268651
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