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Lattice-strained Pt nanoparticles anchored on petroleum vacuum residue derived N-doped porous carbon as highly active and durable cathode catalysts for PEMFCs
Affiliation:1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, PR China;2. Research Institute of Petroleum Prcessing, SINOPEC, Beijing 100083, PR China;1. School of Materials and Energy, Southwest University, Chongqing 400715, China;2. College of Architecture and Environment, Sichuan University, Chengdu 610065, China;3. Institute of Materials, China Academy of Engineering Physics, P.O. Box 9071, Mianyang 621907, China;1. State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum, Huadong, Qingdao, 266580, China;2. Institute for Advanced Study, Shenzhen University, Shenzhen, 518060, China;1. Department of Pharmacy, Jinzhou Medical University, Jinzhou, 121001, PR China;2. College of Veterinary Medicine, Institute of Comparative Medicine, Jiangsu Co-innovation Center for Prevention and Control of Important Animal Infectious Diseases and Zoonoses, Yangzhou University, Yangzhou, 225009, PR China;1. State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116024, PR China;2. Liaoning Key Laboratory of Petrochemical Technology and Equipments, Dalian University of Technology, Dalian 116024, PR China
Abstract:High cost and poor durability of Pt-based cathode catalysts for oxygen reduction reaction (ORR) severely hamper the popularization of proton exchange membrane fuel cells (PEMFCs). Tailoring carbon support is one of effective strategies for improving the performance of Pt-based catalysts. Herein, petroleum vacuum residue was used as carbon source, and nitrogen-doped porous carbon (N-PPC) was synthesized using a simple template-assisted and secondary calcination method. Small Pt nanoparticles (Pt NPs) with an average particles size of 1.8 nm were in-situ prepared and spread evenly on the N-PPC. Interestingly, the lattice compression (1.08%) of Pt NPs on the N-PPC (Pt/N-PPC) was clearly observed by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), which was also verified by the shift of (111) crystal plane of Pt on N-PPC to higher angles. The X-ray photoelectron spectroscopy (XPS) results suggest that the N-PPC support had a strong effect on anchoring Pt NPs and endowing surface Pt NPs with lowered d band center. Thus, the Pt/N-PPC as a catalyst simultaneously boosted the ORR activity and durability. The specific activity (SA) and mass activity (MA) of the Pt/N-PPC at 0.9 V reached 0.83 mA cm?2 and 0.37 A mgPt?1, respectively, much higher than those of the commercial Pt/C (0.21 mA cm?2 and 0.11 A mgPt?1) in 0.1 M HClO4. The half-wave potential (E1/2) of Pt/N-PPC exhibited only a minimal negative shift of 7 mV after 30,000 accelerated durability tests (ADT) cycles. More importantly, an H2–O2 fuel cell with a Pt/N-PPC cathode achieved a power density of 866 mW cm?2, demonstrating that the prepared catalyst has a promising application potential in working environment of PEMFCs.
Keywords:Petroleum vacuum residue  N-doped porous carbon  Lattice-strained Pt  Oxygen reduction reaction
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