TY - JOUR
T1 - Unrevealing liquid metal Ga isolated Pt atom catalysts efficient hydrogenation capability of acid to alkanes
AU - Long, Feng
AU - Zhang, Bo
AU - Cao, Xincheng
AU - Zhang, Xiaolei
AU - Ying, Hanjie
AU - Xu, Junming
AU - Zhu, Chenjie
N1 - Publisher Copyright:
© 2024 Elsevier B.V.
PY - 2025/5/15
Y1 - 2025/5/15
N2 - Herein, we have achieved successful preparation of atomically dispersed catalytic systems, liquid metal Ptx/Ga catalysts, which eliminate the need for reduction processes. Notably, the 0.5 wt% Ptx/Ga catalyst exhibited exceptional stability in hydrogenation performance, achieving 100 % conversion of stearic acid with an impressive 98.7 % selectivity towards octadecane, especially with unprecedented stability over 19 recycling cycles. X-ray absorption spectra (XPS) and density functional theory (DFT) calculations unequivocally establish that isolated Pt atoms, benefitting from charge transfer from the Ga matrix, synergistically optimize Pt metal atom utilization, thereby efficaciously optimizing the d-band center and augmenting hydrogenation proficiency. Furthermore, isolated Pt configuration's weaker CO adsorption ability effectively mitigates concerns of catalyst poisoning and undesirable agglomeration, thereby engendering superior stability. The stronger adsorption with aldehyde and alcohol intermediates promotes the hydrogenation of stearic acid through hydrodehydration pathway, thereby ensuring a high carbon utilization economy. Overall, our work offers insight into the investigation of hydrogenation conversion of bio-derivatives over atomically dispersed catalytic systems.
AB - Herein, we have achieved successful preparation of atomically dispersed catalytic systems, liquid metal Ptx/Ga catalysts, which eliminate the need for reduction processes. Notably, the 0.5 wt% Ptx/Ga catalyst exhibited exceptional stability in hydrogenation performance, achieving 100 % conversion of stearic acid with an impressive 98.7 % selectivity towards octadecane, especially with unprecedented stability over 19 recycling cycles. X-ray absorption spectra (XPS) and density functional theory (DFT) calculations unequivocally establish that isolated Pt atoms, benefitting from charge transfer from the Ga matrix, synergistically optimize Pt metal atom utilization, thereby efficaciously optimizing the d-band center and augmenting hydrogenation proficiency. Furthermore, isolated Pt configuration's weaker CO adsorption ability effectively mitigates concerns of catalyst poisoning and undesirable agglomeration, thereby engendering superior stability. The stronger adsorption with aldehyde and alcohol intermediates promotes the hydrogenation of stearic acid through hydrodehydration pathway, thereby ensuring a high carbon utilization economy. Overall, our work offers insight into the investigation of hydrogenation conversion of bio-derivatives over atomically dispersed catalytic systems.
KW - Atomically dispersed liquid catalytic systems
KW - Intermediates adsorption and hydrogenation activity
KW - Pt/Ga catalysts
KW - d-band center
UR - http://www.scopus.com/inward/record.url?scp=85211387583&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2024.124915
DO - 10.1016/j.apcatb.2024.124915
M3 - 文章
AN - SCOPUS:85211387583
SN - 0926-3373
VL - 365
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 124915
ER -