Insights into Compositional and Structural Effects of Bimetallic Hollow Mesoporous Nanospheres toward Ethanol Oxidation Electrocatalysis
Lv, H (Lv, Hao)[ 1 ] ; Sun, LZ (Sun, Lizhi)[ 1 ] ; Lopes, A (Lopes, Aaron)[ 2 ] ; Xu, DD (Xu, Dongdong)[ 1 ] ; Liu, B (Liu, Ben)[ 1 ]*（刘犇）

[ 1 ] Nanjing Normal Univ, Sch Chem & Mat Sci, Jiangsu Key Lab New Power Batteries, Jiangsu Collaborat Innovat Ctr Biomed Funct Mat, Nanjing 210023, Jiangsu, Peoples R China
[ 2 ] MIT, Dept Chem Engn, Cambridge, MA 02139 USA

JOURNAL OF PHYSICAL CHEMISTRY LETTERS，201909,10(18),5490-5498

A one-pot soft-templating method is reported to fabricate nanosized bimetallic PdAg hollow mesoporous nanospheres (HMSs) for electrocatalytic ethanol oxidation reaction (EOR). The synthesis relies on the "dual-template" surfactant of dioctadecyldimethylammonium chloride that drives in situ growth of mesoporous frameworks on the surface of vesicles into the HMSs with radially opened mesochannels. The synthetic protocol is extendable to engineer elemental compositions and hierarchical nanostructures of PdAg nanoalloys. This system thus provides a direct yet solid platform to understand catalytic add-in synergies of PdAg HMSs toward electrochemical EOR. By evaluating compositional and structural features separately, bimetallic Pd(65)Ag(35 )HMSs display the highest EOR activity with a mass activity of 4.61 A mg(Pd)(-1). Mechanism studies indicate that synergistically electronic and bifunctional effects as well as structural advantages of Pd65Ag35 HMSs kinetically optimize the removal of poisoning carbonaceous intermediates and accelerate the diffusion processes (the rate-determining step), and thus promote the EOR performance accordingly.

文章链接：
https://pubs.acs.org/doi/10.1021/acs.jpclett.9b02218

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