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Double layer charging driven carbon dioxide adsorption limits the rate of electrochemical carbon dioxide reduction on Gold.
Electrochemical CO[Formula: see text] reduction is a potential route to the sustainable production of valuable fuels and chemicals. Here, we perform CO[Formula: see text] reduction experiments on Gold at neutral to acidic pH values to elucidate the long-standing controversy surrounding the rate-limiting step. We find the CO production rate to be invariant with pH on a Standard Hydrogen Electrode scale and conclude that it is limited by the CO[Formula: see text] adsorption step. We present a new multi-scale modeling scheme that integrates ab initio reaction kinetics with mass transport simulations, explicitly considering the charged electric double layer. The model reproduces the experimental CO polarization curve and reveals the rate-limiting step to be *COOH to *CO at low overpotentials, CO[Formula: see text] adsorption at intermediate ones, and CO[Formula: see text] mass transport at high overpotentials. Finally, we show the Tafel slope to arise from the electrostatic interaction between the dipole of *CO[Formula: see text] and the interfacial field. This work highlights the importance of surface charging for electrochemical kinetics and mass transport
Development of Aerogel Composites for Multilayer Insulation, Thermoelectric Applications and High Temperature Thermal Protection Systems
No abstract availabl
The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO<sub>2</sub> Reduction Conditions: An Experimental and Theoretical Study
A combination
of experiment and theory has been used to understand
the relationship between the hydrogen evolution reaction (HER) and
CO<sub>2</sub> reduction (CO<sub>2</sub>R) on transition metal phosphide
and transition metal sulfide catalysts. Although multifunctional active
sites in these materials could potentially improve their CO<sub>2</sub>R activity relative to pure transition metal electrocatalysts, under
aqueous testing conditions, these materials showed a high selectivity
for the HER relative to CO<sub>2</sub>R. Computational results supported
these findings, indicating that a limitation of the metal phosphide
catalysts is that the HER is favored thermodynamically over CO<sub>2</sub>R. On Ni-MoS<sub>2</sub>, a limitation is the kinetic barrier
for the proton–electron transfer to *CO. These theoretical
and experimental results demonstrate that selective CO<sub>2</sub>R requires electrocatalysts that possess both favorable thermodynamic
pathways and surmountable kinetic barriers
The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO_2 Reduction Conditions: An Experimental and Theoretical Study
A combination of experiment and theory has been used to understand the relationship between the hydrogen evolution reaction (HER) and CO_2 reduction (CO_2R) on transition metal phosphide and transition metal sulfide catalysts. Although multifunctional active sites in these materials could potentially improve their CO_2R activity relative to pure transition metal electrocatalysts, under aqueous testing conditions, these materials showed a high selectivity for the HER relative to CO_2R. Computational results supported these findings, indicating that a limitation of the metal phosphide catalysts is that the HER is favored thermodynamically over CO_2R. On Ni-MoS_2, a limitation is the kinetic barrier for the proton–electron transfer to *CO. These theoretical and experimental results demonstrate that selective CO_2R requires electrocatalysts that possess both favorable thermodynamic pathways and surmountable kinetic barriers
Measurements of double-helicity asymmetries in inclusive production in longitudinally polarized collisions at GeV
We report the double helicity asymmetry, , in inclusive
production at forward rapidity as a function of transverse momentum
and rapidity . The data analyzed were taken during
GeV longitudinally polarized collisions at the Relativistic Heavy Ion
Collider (RHIC) in the 2013 run using the PHENIX detector. At this collision
energy, particles are predominantly produced through gluon-gluon
scatterings, thus is sensitive to the gluon polarization
inside the proton. We measured by detecting the decay
daughter muon pairs within the PHENIX muon spectrometers in the
rapidity range . In this kinematic range, we measured the
to be ~(stat)~~(syst). The
can be expressed to be proportional to the product of the
gluon polarization distributions at two distinct ranges of Bjorken : one at
moderate range where recent RHIC data of jet and
double helicity spin asymmetries have shown evidence for significant gluon
polarization, and the other one covering the poorly known small- region . Thus our new results could be used to further
constrain the gluon polarization for .Comment: 335 authors, 10 pages, 4 figures, 3 tables, 2013 data. Version
accepted for publication by Phys. Rev. D. Plain text data tables for the
points plotted in figures for this and previous PHENIX publications are (or
will be) publicly available at http://www.phenix.bnl.gov/papers.htm
Cross sections and double-helicity asymmetries of midrapidity inclusive charged hadrons in p+p collisions at sqrt(s)=62.4 GeV
Unpolarized cross sections and double-helicity asymmetries of
single-inclusive positive and negative charged hadrons at midrapidity from p+p
collisions at sqrt(s)=62.4 GeV are presented. The PHENIX measurements for 1.0 <
p_T < 4.5 GeV/c are consistent with perturbative QCD calculations at
next-to-leading order in the strong coupling constant, alpha_s. Resummed pQCD
calculations including terms with next-to-leading-log accuracy, yielding
reduced theoretical uncertainties, also agree with the data. The
double-helicity asymmetry, sensitive at leading order to the gluon polarization
in a momentum-fraction range of 0.05 ~< x_gluon ~< 0.2, is consistent with
recent global parameterizations disfavoring large gluon polarization.Comment: PHENIX Collaboration. 447 authors, 12 pages, 5 figures, 5 tables.
Submitted to Physical Review
Inclusive cross section and single-transverse-spin asymmetry for very forward neutron production in polarized p+p collisions at sqrt(s)=200 GeV
The energy dependence of the single-transverse-spin asymmetry, A_N, and the
cross section for neutron production at very forward angles were measured in
the PHENIX experiment at RHIC for polarized p+p collisions at sqrt(s)=200 GeV.
The neutrons were observed in forward detectors covering an angular range of up
to 2.2 mrad. We report results for neutrons with momentum fraction of x_F=0.45
to 1.0. The energy dependence of the measured cross sections were consistent
with x_F scaling, compared to measurements by an ISR experiment which measured
neutron production in unpolarized p+p collisions at sqrt(s)=30.6--62.7 GeV. The
cross sections for large x_F neutron production for p+p collisions, as well as
those in e+p collisions measured at HERA, are described by a pion exchange
mechanism. The observed forward neutron asymmetries were large, reaching
A_N=-0.08+/-0.02 for x_F=0.8; the measured backward asymmetries, for negative
x_F, were consistent with zero. The observed asymmetry for forward neutron
production is discussed within the pion exchange framework, with interference
between the spin-flip amplitude due to the pion exchange and nonflip amplitudes
from all Reggeon exchanges. Within the pion exchange description, the measured
neutron asymmetry is sensitive to the contribution of other Reggeon exchanges
even for small amplitudes.Comment: 383 authors, 16 pages, 18 figures, 6 tables. Submitted to Phys. Rev.
D. Plain text data tables for the points plotted in figures for this and
previous PHENIX publications are (or will be) publicly available at
http://www.phenix.bnl.gov/papers.htm
Inclusive cross section and double helicity asymmetry for pi^0 production in p+p collisions at sqrt(s) = 62.4 GeV
The PHENIX experiment presents results from the RHIC 2006 run with polarized
proton collisions at sqrt(s) = 62.4 GeV for inclusive pi^0 production at
mid-rapidity. Unpolarized cross section results are measured for transverse
momenta p_T = 0.5 to 7 GeV/c. Next-to-leading order perturbative quantum
chromodynamics calculations are compared with the data, and while the
calculations are consistent with the measurements, next-to-leading logarithmic
corrections improve the agreement. Double helicity asymmetries A_LL are
presented for p_T = 1 to 4 GeV/c and probe the higher range of Bjorken_x of the
gluon (x_g) with better statistical precision than our previous measurements at
sqrt(s)=200 GeV. These measurements are sensitive to the gluon polarization in
the proton for 0.06 < x_g < 0.4.Comment: 387 authors from 63 institutions, 10 pages, 6 figures, 1 table.
Submitted to Physical Review D. Plain text data tables for the points plotted
in figures for this and previous PHENIX publications are (or will be)
publicly available at http://www.phenix.bnl.gov/papers.htm
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