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Dense Heterointerfaces and Unsaturated Coordination Synergistically Accelerate Electrocatalysis in Pt/Pt_5P_2 Porous Nanocages

机译:Dense Heterointerfaces and Unsaturated Coordination Synergistically Accelerate Electrocatalysis in Pt/Pt_5P_2 Porous Nanocages

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摘要

Designing cost-effective and durable Pt-based catalysts is vital and challengingfor practicable energy storage and conversion technologies. Here,a fast phosphating strategy to establish a Pt/Pt_5P_2 porous nanocage withnumerous heterointerfaces and defects is presented. It exhibits extraordinaryactivity and stability for both hydrogen evolution reaction (HER) with a smalloverpotential of 29 mV at 10 mA cm~(?2) and methanol oxidation reaction(MOR) with a high mass activity of 1.37 A mg~(?1)Pt at peak values, surpassingPt/C. Microstructural analyzes show that many stacking faults are inducedaround heterointerfaces, while rich vacancies and atomic steps are createdby the phosphorus-induced thermal migration of Pt atoms, serving as highlyactive low-coordination sites. X-ray absorption spectroscopy and theoreticalcalculations reveal that introducing P atoms can modify the electronic configurationof Pt, thus optimizing H_2O/H* binding strength and lowering waterdissociation energy to accelerate HER, while decreasing the energy barrier ofthe rate-limiting step (*CHO to *HCOOH) to facilitate MOR.

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