TY - JOUR
T1 - Highly active platinum single-atom catalyst grafted onto 3D carbon cloth support for the electrocatalytic hydrogen evolution reaction
AU - Yu, Po Wei
AU - Elmas, Sait
AU - Roman, Tanglaw
AU - Pan, Xun
AU - Yin, Yanting
AU - Gibson, Christopher T.
AU - Andersson, Gunther G.
AU - Andersson, Mats R.
PY - 2022/9/1
Y1 - 2022/9/1
N2 - Platinum single-atom catalysts (PtSACs) on 3D support are emerging as the new frontier in catalysis due to their atom-economy, outstanding performance, and the advantage to bridge the gap between homogeneous and heterogeneous catalysis. Here we report on a simple, single-step electrochemical grafting attachment of a metal-selective ligand, 2,6:2′,2″-terpyridine, and the synthesis of platinum single-atom electrocatalyst via metal uptake from aqueous salt solution. At an ultra-low loading of 0.26 ± 0.02 μg•cm−2 of platinum, the single-atom catalysts supported on porous 3D carbon cloth electrode via chemical bonding revealed higher mass activity ratios, up to 83.0 at η = 50 mV/RHE, compared to the commercial catalyst 20 % Pt/C. Using hydrogen binding energy as the descriptor for efficiency, density functional theory calculations show that promoting hydrogen evolution using terpyridine-Pt proceeds when the catalyst is in a 2+ charge state and with a single hydroxy co-ligand attached to Pt catalytic center. Calculations predict an HER overpotential of about 0.28 V. The electro-grafted terpyridine ligand proved to act as effective scavenger for leached platinum from the counter electrode during extended operational hours. The method to make the PtSAC is facile, non-hazardous and versatile without involving any elaborate pre- and/or post-treatment steps and, the cost of the added platinum to the ligand is only 0.1 US$ m−2.
AB - Platinum single-atom catalysts (PtSACs) on 3D support are emerging as the new frontier in catalysis due to their atom-economy, outstanding performance, and the advantage to bridge the gap between homogeneous and heterogeneous catalysis. Here we report on a simple, single-step electrochemical grafting attachment of a metal-selective ligand, 2,6:2′,2″-terpyridine, and the synthesis of platinum single-atom electrocatalyst via metal uptake from aqueous salt solution. At an ultra-low loading of 0.26 ± 0.02 μg•cm−2 of platinum, the single-atom catalysts supported on porous 3D carbon cloth electrode via chemical bonding revealed higher mass activity ratios, up to 83.0 at η = 50 mV/RHE, compared to the commercial catalyst 20 % Pt/C. Using hydrogen binding energy as the descriptor for efficiency, density functional theory calculations show that promoting hydrogen evolution using terpyridine-Pt proceeds when the catalyst is in a 2+ charge state and with a single hydroxy co-ligand attached to Pt catalytic center. Calculations predict an HER overpotential of about 0.28 V. The electro-grafted terpyridine ligand proved to act as effective scavenger for leached platinum from the counter electrode during extended operational hours. The method to make the PtSAC is facile, non-hazardous and versatile without involving any elaborate pre- and/or post-treatment steps and, the cost of the added platinum to the ligand is only 0.1 US$ m−2.
KW - Electro-grafting
KW - Electrocatalysis
KW - Hydrogen evolution
KW - Platinum
KW - Self-supported electrodes
KW - Single-atom catalyst
KW - Terpyridine
UR - http://www.scopus.com/inward/record.url?scp=85129625042&partnerID=8YFLogxK
UR - http://purl.org/au-research/grants/ARC/DP210101243
U2 - 10.1016/j.apsusc.2022.153480
DO - 10.1016/j.apsusc.2022.153480
M3 - Article
AN - SCOPUS:85129625042
SN - 0169-4332
VL - 595
JO - Applied Surface Science
JF - Applied Surface Science
M1 - 153480
ER -