TY - JOUR
T1 - Highly exposed PtPdTe alloy planting with oxyphilic Cu single sites boosting durable multiple alcohol oxidation electrocatalysis
AU - Qin, Rong
AU - Ma, Chao
AU - Wu, Junyao
AU - Chen, Guanzhen
AU - Wang, Jie
AU - Xiong, Yu
AU - Niu, Shuwen
AU - Gan, Tao
AU - Wang, Ziyun
AU - Han, Yunhu
N1 - Publisher Copyright:
© 2025 Science Press
PY - 2025/5
Y1 - 2025/5
N2 - Platinum group alloys have an excellent electronic structure for oxidation of alcohols, but the active sites are more susceptible to deactivation by CO adsorbates (COads). The precise integration of single-atom and alloy structures is highly attractive for energy conversion but still a challenge. Here, we report an ion-exchange coupled in situ reduction strategy to fabricate hollow PtPdTe alloy nanoreactors loaded with atomically dispersed Cu sites (CuSA/h-PtPdTe NRs). The planted oxyphilic Cu single sites and resulted compressive strains are conductive to modulating the electronic structure of the active sites, which changes the rate-determining step of the reaction while inhibiting the formation of COads and modulating the adsorption of intermediates, resulting in the improved activity and stability. Specifically, the obtained CuSA/h-PtPdTe NRs exhibit an excellent oxidation performance of multiple alcohols, especially for methanol and ethanol, with 8.0 and 10.3 times of the mass activity higher than Pt/C, and the activity could be recovered by refreshing the electrolyte and could be sustained for 72,000 and 36,000 s, respectively. Meanwhile, CuSA/h-PtPdTe NRs show superior oxidation performance and durability to ethylene glycol and glycerol. This work pioneers the realization of precise modulation of catalytic sites using single atoms and provides an encouraging pathway for the design of efficient and stable electrocatalysts for the oxidation of multiple alcohols, which could broaden the range of options and sources of fuel cells.
AB - Platinum group alloys have an excellent electronic structure for oxidation of alcohols, but the active sites are more susceptible to deactivation by CO adsorbates (COads). The precise integration of single-atom and alloy structures is highly attractive for energy conversion but still a challenge. Here, we report an ion-exchange coupled in situ reduction strategy to fabricate hollow PtPdTe alloy nanoreactors loaded with atomically dispersed Cu sites (CuSA/h-PtPdTe NRs). The planted oxyphilic Cu single sites and resulted compressive strains are conductive to modulating the electronic structure of the active sites, which changes the rate-determining step of the reaction while inhibiting the formation of COads and modulating the adsorption of intermediates, resulting in the improved activity and stability. Specifically, the obtained CuSA/h-PtPdTe NRs exhibit an excellent oxidation performance of multiple alcohols, especially for methanol and ethanol, with 8.0 and 10.3 times of the mass activity higher than Pt/C, and the activity could be recovered by refreshing the electrolyte and could be sustained for 72,000 and 36,000 s, respectively. Meanwhile, CuSA/h-PtPdTe NRs show superior oxidation performance and durability to ethylene glycol and glycerol. This work pioneers the realization of precise modulation of catalytic sites using single atoms and provides an encouraging pathway for the design of efficient and stable electrocatalysts for the oxidation of multiple alcohols, which could broaden the range of options and sources of fuel cells.
KW - CO adsorbates toxicity
KW - Hollow alloy
KW - Lattice distortion
KW - Oxidation reaction of multiple alcohols
KW - Single-atom Cu modification
UR - http://www.scopus.com/inward/record.url?scp=85217743451&partnerID=8YFLogxK
U2 - 10.1016/j.jechem.2025.01.021
DO - 10.1016/j.jechem.2025.01.021
M3 - 文章
AN - SCOPUS:85217743451
SN - 2095-4956
VL - 104
SP - 609
EP - 617
JO - Journal of Energy Chemistry
JF - Journal of Energy Chemistry
ER -