AI Chat Paper
Discover the SciOpen Platform and Achieve Your Research Goals with Ease.
Search articles, authors, keywords, DOl and etc.
{{expandStatus?'Exit ':''}}Advanced Search
Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells (PEMFCs). Despite extensive research on catalysts for the cathodic oxygen reduction reaction (ORR), developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains challenging. Herein, we report a facile synthesis of bimetallic ultrathin PtM (M = Mo, W, and Cr) nanowires (NWs) composed of group VI B transition metal atomic sites anchored on the surface. These NWs possess uniform sizes and well-controlled atomic arrangements. Compared to PtW and PtCr catalysts, the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt−1. Remarkably, they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR, surpassing previously reported Pt-based catalysts. Additionally, the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm−2 (H2-O2 conditions at 80 °C), which is 1.09 times that of commercial Pt/C. The ligand effect in the bimetallic surface not only facilitates strong coupling between Mo (4d) and Pt (5d) atomic orbitals to hinder atom leaching but also modulates the d-states of active site, significantly optimizing the adsorption of key oxygen (*O and *OH) species and accelerating the rate-determining step in ORR pathways.
Han, A. L.; Sun, W. M.; Wan, X.; Cai, D. D.; Wang, X. J.; Li, F.; Shui, J. L.; Wang, D. S. Construction of Co4 atomic clusters to enable Fe-N4 motifs with highly active and durable oxygen reduction performance. Angew. Chem., Int. Ed. 2023, 62, e202303185.
Li, J. J.; Xia, W.; Tang, J.; Gao, Y.; Jiang, C.; Jia, Y. N.; Chen, T.; Hou, Z. F.; Qi, R. J.; Jiang, D. et al. Metal-organic framework-derived graphene mesh: A robust scaffold for highly exposed Fe-N4 active sites toward an excellent oxygen reduction catalyst in acid media. J. Am. Chem. Soc. 2022, 144, 9280–9291.
Xiao, F.; Wang, Q.; Xu, G. L.; Qin, X. P.; Hwang, I.; Sun, C. J.; Liu, M.; Hua, W.; Wu, H. W.; Zhu, S. Q. et al. Atomically dispersed Pt and Fe sites and Pt-Fe nanoparticles for durable proton exchange membrane fuel cells. Nat. Catal. 2022, 5, 503–512.
Sun, Y. Y.; Polani, S.; Luo, F.; Ott, S.; Strasser, P.; Dionigi, F. Advancements in cathode catalyst and cathode layer design for proton exchange membrane fuel cells. Nat. Commun. 2021, 12, 5984.
Jiao, K.; Xuan, J.; Du, Q.; Bao, Z. M.; Xie, B.; Wang, B. W.; Zhao, Y.; Fan, L. H.; Wang, H. Z.; Hou, Z. J. et al. Designing the next generation of proton-exchange membrane fuel cells. Nature 2021, 595, 361–369.
Fan, J. T.; Chen, M.; Zhao, Z. L.; Zhang, Z.; Ye, S. Y.; Xu, S. Y.; Wang, H. J.; Li, H. Bridging the gap between highly active oxygen reduction reaction catalysts and effective catalyst layers for proton exchange membrane fuel cells. Nat. Energy 2021, 6, 475–486.
Chen, Y. P.; Zheng, X. S.; Cai, J. Y.; Zhao, G. Q.; Zhang, B. X.; Luo, Z. X.; Wang, G. M.; Pan, H. G.; Sun, W. P. Sulfur doping triggering enhanced Pt-N coordination in graphitic carbon nitride-supported Pt electrocatalysts toward efficient oxygen reduction reaction. ACS Catal. 2022, 12, 7406–7414.
Lu, B. A.; Shen, L. F.; Liu, J.; Zhang, Q. H.; Wan, L. Y.; Morris, D. J.; Wang, R. X.; Zhou, Z. Y.; Li, G.; Sheng, T. et al. Structurally disordered phosphorus-doped Pt as a highly active electrocatalyst for an oxygen reduction reaction. ACS Catal. 2021, 11, 355–363.
Han, A. L.; Wang, X. J.; Tang, K.; Zhang, Z. D.; Ye, C. L.; Kong, K. J.; Hu, H. B.; Zheng, L. R.; Jiang, P.; Zhao, C. X. et al. An adjacent atomic platinum site enables single-atom iron with high oxygen reduction reaction performance. Angew. Chem., Int. Ed. 2021, 60, 19262–19271.
Li, X.; He, Y. H.; Cheng, S. B.; Li, B. Y.; Zeng, Y. C.; Xie, Z. H.; Meng, Q. P.; Ma, L.; Kisslinger, K.; Tong, X. et al. Atomic structure evolution of Pt-Co binary catalysts: Single metal sites versus intermetallic nanocrystals. Adv. Mater. 2021, 33, 2106371.
Gao, L.; Li, X. X.; Yao, Z. Y.; Bai, H. J.; Lu, Y. F.; Ma, C.; Lu, S. F.; Peng, Z. M.; Yang, J. L.; Pan, A. L. et al. Unconventional p-d hybridization interaction in PtGa ultrathin nanowires boosts oxygen reduction electrocatalysis. J. Am. Chem. Soc. 2019, 141, 18083–18090.
Zaman, S.; Huang, L.; Douka, A. I.; Yang, H.; You, B.; Xia, B. Y. Oxygen reduction electrocatalysts toward practical fuel cells: Progress and perspectives. Angew. Chem. 2021, 133, 17976–17996.
Zhuang, Z. C.; Li, Y.; Li, Y. H.; Huang, J. Z.; Wei, B.; Sun, R.; Ren, Y. J.; Ding, J.; Zhu, J. X.; Lang, Z. Q. et al. Atomically dispersed nonmagnetic electron traps improve oxygen reduction activity of perovskite oxides. Energy Environ. Sci., 2021, 14, 1016–1028.
Zhuang, Z. C.; Xia, L. X.; Huang, J. Z.; Zhu, P.; Li, Y.; Ye, C. L.; Xia, M. G.; Yu, R. H.; Lang, Z. Q.; Zhu, J. X. et al. Continuous modulation of electrocatalytic oxygen reduction activities of single-atom catalysts through p -n junction rectification. Angew. Chem., Int. Ed. 2023, 62, e202212335.
Cheng, Q. Q.; Yang, S.; Fu, C. H.; Zou, L. L.; Zou, Z. Q.; Jiang, Z.; Zhang, J. L.; Yang, H. High-loaded sub-6 nm Pt1Co1 intermetallic compounds with highly efficient performance expression in PEMFCs. Energy Environ. Sci. 2022, 15, 278–286.
Chang, F. F.; Bai, Z. Y.; Li, M.; Ren, M. Y.; Liu, T. C.; Yang, L.; Zhong, C. J.; Lu, J. Strain-modulated platinum-palladium nanowires for oxygen reduction reaction. Nano Lett. 2020, 20, 2416–2422.
Hu, Y. Z.; Guo, X. Y.; Shen, T.; Zhu, Y.; Wang, D. L. Hollow porous carbon-confined atomically ordered PtCo3 intermetallics for an efficient oxygen reduction reaction. ACS Catal. 2022, 12, 5380–5387.
Zaman, S.; Su, Y. Q.; Dong, C. L.; Qi, R. J.; Huang, L.; Qin, Y. Y.; Huang, Y. C.; Li, F. M.; You, B.; Guo, W. et al. Scalable molten salt synthesis of platinum alloys planted in metal-nitrogen-graphene for efficient oxygen reduction. Angew. Chem., Int. Ed. 2022, 61, e202115835.
He, T. O.; Wang, W. C.; Yang, X. L.; Shi, F. L.; Ye, Z. Y.; Zheng, Y. Z.; Li, F.; Wu, J. B.; Yin, Y. D.; Jin, M. S. Deposition of atomically thin Pt shells on amorphous palladium phosphide cores for enhancing the electrocatalytic durability. ACS Nano 2021, 15, 7348–7356.
Jin, H.; Xu, Z. W.; Hu, Z. Y.; Yin, Z. W.; Wang, Z.; Deng, Z.; Wei, P.; Feng, S. H.; Dong, S. H.; Liu, J. F. et al. Mesoporous Pt@Pt-skin Pt3Ni core–shell framework nanowire electrocatalyst for efficient oxygen reduction. Nat. Commun. 2023, 14, 1518.
Liu, Z. Y.; Zhao, Z. P.; Peng, B. S.; Duan, X. F.; Huang, Y. Beyond extended surfaces: Understanding the oxygen reduction reaction on nanocatalysts. J. Am. Chem. Soc. 2020, 142, 17812–17827.
Wang, L. G.; Wu, J. B.; Wang, S. W.; Liu, H.; Wang, Y.; Wang D. S. The reformation of catalyst: From a trial-and-error synthesis to rational design. Nano Res. 2024, 17, 3261–3301
Feng, Q. C.; Wang, X. L.; Klingenhof, M.; Heggen, M.; Strasser, P. Low-Pt NiNC-supported PtNi nanoalloy oxygen reduction reaction electrocatalysts— In situ tracking of the atomic alloying process. Angew. Chem., Int. Ed. 2022, 61, e202203728.
Wei, M.; Huang, L.; Li, L. B.; Ai, F.; Su, J. Z.; Wang, J. K. Coordinatively unsaturated PtCo flowers assembled with ultrathin nanosheets for enhanced oxygen reduction. ACS Catal. 2022, 12, 6478–6485.
Tu, W. Z.; Luo, W. J.; Chen, C. L.; Chen, K.; Zhu, E. B.; Zhao, Z. P.; Wang, Z. L.; Hu, T.; Zai, H. C.; Ke, X. X. et al. Tungsten as “adhesive” in Pt2CuW0.25 ternary alloy for highly durable oxygen reduction electrocatalysis. Adv. Funct. Mater. 2020, 30, 1908230.
Zhang, Z.; Yang, S.; Jiang, R.; Sheng, T.; Shi, C.; Chen, Y.; Wang, L. Intensifying uneven charge distribution via geometric distortion engineering in atomically dispersed M-N x /S sites for efficient oxygen electroreduction. Nano Res. 2022, 15, 8928–8935.
Zhu, S. Q.; Qin, X. P.; Yao, Y.; Shao, M. H. pH-dependent hydrogen and water binding energies on platinum surfaces as directly probed through surface-enhanced infrared absorption spectroscopy. J. Am. Chem. Soc. 2020, 142, 8748–8754.
Wandlowski, T.; Ataka, K.; Pronkin, S.; Diesing, D. Surface enhanced infrared spectroscopy-Au (111-20 nm)/sulphuric acid-new aspects and challenges. Electrochim. Acta 2004, 49, 1233–1247.
Li, P.; Jiao, Y. Z.; Ruan, Y. E.; Fei, H. G.; Men, Y. N.; Guo, C. L.; Wu, Y. E.; Chen, S. L. Revealing the role of double-layer microenvironments in pH-dependent oxygen reduction activity over metal-nitrogen-carbon catalysts. Nat. Commun. 2023, 14, 6936.
Kulkarni, A.; Siahrostami, S.; Patel, A.; Nørskov, J. K. Understanding catalytic activity trends in the oxygen reduction reaction. Chem. Rev. 2018, 118, 2302–2312.
京公网安备11010802044758号