TY - JOUR
T1 - Lanthanide electronic perturbation in Pt-Ln (La, Ce, Pr and Nd) alloys for enhanced methanol oxidation reaction activity
AU - Zhang, Shuai
AU - Zeng, Zhichao
AU - Li, Qingqing
AU - Huang, Bolong
AU - Zhang, Xinyu
AU - Du, Yaping
AU - Yan, Chun Hua
N1 - Funding Information:
We gratefully acknowledge the support from the China National Funds for Excellent Young Scientists (grant no. 21522106), the National Natural Science Foundation of China (grant No. 21971117; 21771156), the 111 Project (B18030) from China, and the Open Funds of the State Key Laboratory of Rare Earth Resource Utilization (RERU2019001), the Functional Research Funds for the Central Universities, Nankai University (ZB19500202) Beijing-Tianjin-Hebei Collaborative Innovation Project (19YFSLQY00030), the Outstanding Youth Project of Tianjin Natural Science Foundation (20JCJQJC00130), and the Key Project of Tianjin Natural Science Foundation (20JCZDJC00650). The authors have submitted a Chinese patent application on the disclosed approach for the large-scale synthesis of halide materials.
Publisher Copyright:
© 2021 The Royal Society of Chemistry.
PY - 2021/11
Y1 - 2021/11
N2 - Simultaneously achieving high activity and robust stability is still challenging for direct methanol fuel cells in practical applications. Although noble metal Pt has been applied as an electrocatalyst, it still suffers from low stability and high cost, which significantly limits its wide applications on a large scale. Here, a series of Pt-Ln/C (Ln = La, Ce, Pr, Nd) nanoalloy catalysts were synthesized to improve the electroactivity towards methanol oxidation and suppress the CO poisoning effect of Pt. DFT calculations have unravelled the different electronic structures of different Pt5Ln samples, in which the optimal d-f coupling in Pt5Ce leads to significant improvements in both electroactivity and selectivity. Such an electronic structure also effectively suppresses the CO poisoning effect during the MOR. Pt5Ce/C shows the best performance, with a specific activity of 32.74 mA cmPt-2, which is 11.1 times higher than that of commercial Pt/C (2.94 mA cmPt-2). This work demonstrates the critical promotion effect of lanthanide elements in the electroactivity of Pt due to the electronic structure perturbation, which provides new ideas for the design of efficient lanthanide alloy catalysts.
AB - Simultaneously achieving high activity and robust stability is still challenging for direct methanol fuel cells in practical applications. Although noble metal Pt has been applied as an electrocatalyst, it still suffers from low stability and high cost, which significantly limits its wide applications on a large scale. Here, a series of Pt-Ln/C (Ln = La, Ce, Pr, Nd) nanoalloy catalysts were synthesized to improve the electroactivity towards methanol oxidation and suppress the CO poisoning effect of Pt. DFT calculations have unravelled the different electronic structures of different Pt5Ln samples, in which the optimal d-f coupling in Pt5Ce leads to significant improvements in both electroactivity and selectivity. Such an electronic structure also effectively suppresses the CO poisoning effect during the MOR. Pt5Ce/C shows the best performance, with a specific activity of 32.74 mA cmPt-2, which is 11.1 times higher than that of commercial Pt/C (2.94 mA cmPt-2). This work demonstrates the critical promotion effect of lanthanide elements in the electroactivity of Pt due to the electronic structure perturbation, which provides new ideas for the design of efficient lanthanide alloy catalysts.
UR - http://www.scopus.com/inward/record.url?scp=85119509424&partnerID=8YFLogxK
U2 - 10.1039/d1ee02433g
DO - 10.1039/d1ee02433g
M3 - Journal article
AN - SCOPUS:85119509424
SN - 1754-5692
VL - 14
SP - 5911
EP - 5918
JO - Energy and Environmental Science
JF - Energy and Environmental Science
IS - 11
ER -
