The synergistic effect Pt-1-W dual sites as a highly active and durable catalyst for electrochemical methanol oxidation

Awoke, YAYAAwokeTsai, MCMCTsaiAdam, DBDBAdamAyele, AAAAAyeleYang, SCSCYangHuang, WHWHHuangChen, JLJLChenPao, CWCWPaoCHUNG-YUAN MOUSu, WNWNSuHwang, BJBJHwang2022-12-282022-12-2820220013-4686https://scholars.lib.ntu.edu.tw/handle/123456789/626787Downsizing precious metal catalysts such as Pt to the atomic level is considered effective and efficient in the catalysis industry. However, Pt single-atom alone cannot catalyze the MOR (methanol oxidation reaction) due to the requirement of Pt ensemble sites to activate C-O bonds. Herein, we report for the first Pt single atom dispersed on dual doped TiO2 (Pt1/ Ti0.8W0.2NxOy) as an effective and durable catalyst towards MOR. It is found that synergy between Pt1-WO3-x dual-active-sites enables the adsorption and dehydrogenation of methanol. Density functional theory (DFT) calculations reveal that W-site adsorbs methanol molecule and the synergistic cooperation between Pt1-W dual active sites in Pt1/Ti0.8W0.2NxOy contributes to the high catalytic activity, stability, and selectivity. The Pt1/ Ti0.8W0.2NxOy catalyst displays high MOR performance with a mass activity of 560 mA mg−1Pt at 0.82 V vs. RHE in an alkaline medium. This activity is 9.3 and 1.3 times higher than the corresponding Pt nanoparticle (2 wt% Pt/ Ti0.8W0.2NxOy) and 20% Pt/C catalysts, respectively. The lower Tafel slope (93 mV dec−1) and higher diffusion coefficient (1.5×10−12 cm2/s) indicate MOR is faster on Pt1/Ti0.82W0.18NxOy than the other catalysts. Furthermore, Pt1/ Ti0.8W0.2NxOy oxidizes methanol to formate with 90% selectivity, whereas 2 wt% Pt/Ti0.82W0.18NxOy to formaldehyde with 69% selectivity. Moreover, after 10 h, Pt1/ Ti0.8W0.2NxOy mass activity decayed only by 7.2%. In contrast, 2 wt% Pt/ Ti0.8W0.2NxOy and 20% Pt/C exhibited 23% and 43% of activity losses respectively.enSingle-atom catalyst; Methanol oxidation reaction; Dual active sites; Selectivity; SINGLE-ATOM CATALYSTS; METAL-SUPPORT INTERACTIONS; DOPED TIO2 PHOTOCATALYSTS; IR; PD; ELECTROCATALYSTS; HYDROGENATION; NANOPARTICLES; CONVERSION; STABILITY[SDGs]SDG7The synergistic effect Pt-1-W dual sites as a highly active and durable catalyst for electrochemical methanol oxidationjournal article10.1016/j.electacta.2022.1411612-s2.0-85138109586WOS:000862594200004https://api.elsevier.com/content/abstract/scopus_id/85138109586