TY - JOUR
T1 - Some Attributes of Mn3+ Sites in Nickel-Based Layered Double Hydroxides during Methanol Electro-oxidation in Alkaline Media
AU - Oliver-Tolentino, Miguel A.
AU - Ramos-Sánchez, Guadalupe
AU - Manzo-Robledo, Arturo
AU - Ramírez-Rosales, Daniel
AU - Flores-Moreno, Jorge L.
AU - Lima, Enrique
AU - Guzmán-Vargas, Ariel
N1 - Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2018/2
Y1 - 2018/2
N2 - Ni-based layered double hydroxides (LDHs), or hydrotalcite-like materials (HTs), were synthetized through co-precipitation at constant pH (NiAl and NiMg) and urea hydrolysis (NiMn) methods, and they were tested in the electrochemical methanol oxidation (MOR). The physicochemical properties were explored by using techniques such as X-ray diffraction, FT-IR spectroscopy, as well as electron paramagnetic resonance. In addition, correlation between active site arrangements and electrocatalytic activity was evidenced by density functional calculations. Specific site μ(Ni2Mn-OH) showed the lowest proton energy removal at approximately 3.6 eV and the NiMn LDH sample containing a higher proportion of this site exhibited the best performance for the MOR process, with an enhancement factor of 5.16, which is attributed to limited deactivation of Ni during the reaction. CO2 production was detected by differential electrochemical mass spectrometry to be on the order of ten times greater than O2.
AB - Ni-based layered double hydroxides (LDHs), or hydrotalcite-like materials (HTs), were synthetized through co-precipitation at constant pH (NiAl and NiMg) and urea hydrolysis (NiMn) methods, and they were tested in the electrochemical methanol oxidation (MOR). The physicochemical properties were explored by using techniques such as X-ray diffraction, FT-IR spectroscopy, as well as electron paramagnetic resonance. In addition, correlation between active site arrangements and electrocatalytic activity was evidenced by density functional calculations. Specific site μ(Ni2Mn-OH) showed the lowest proton energy removal at approximately 3.6 eV and the NiMn LDH sample containing a higher proportion of this site exhibited the best performance for the MOR process, with an enhancement factor of 5.16, which is attributed to limited deactivation of Ni during the reaction. CO2 production was detected by differential electrochemical mass spectrometry to be on the order of ten times greater than O2.
KW - Jahn-Teller distortions
KW - Methanol Oxidation
KW - catalytic deactivation
KW - deprotonation energy
KW - electron mobility
UR - http://www.scopus.com/inward/record.url?scp=85038348815&partnerID=8YFLogxK
U2 - 10.1002/celc.201701093
DO - 10.1002/celc.201701093
M3 - Artículo
SN - 2196-0216
VL - 5
SP - 708
EP - 716
JO - ChemElectroChem
JF - ChemElectroChem
IS - 4
ER -