摘要：Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel *** the utilization of Pt based materials by modulating their morphologies to expose more active sites is a fundamental objective for the practical application of fuel ***,we report a new class of hierarchically skeletal Pt-Ni nanocrystals(HSNs)with a multi-layered structure,prepared by an inorganic acid-induced solvothermal *** addition of H_(2)SO_(4)to the synthetic protocol provides a critical trigger for the successful growth of Pt-Ni nanocrystals with the desired *** Pt-Ni HSNs synthesized by this method exhibit enhanced mass activity of 1.25 A mgpt−1 at 0.9 V(versus the reversible hydrogen electrode)towards ORR in 0.1-M HClO_(4),which is superior to that of Pt-Ni multi-branched nanocrystals obtained by the same method in the absence of inorganic acid;it is additionally 8.9-fold higher than that of the commercial Pt/C ***,it displays enhanced stability,with only 21.6%mass activity loss after 10,000 cycles(0.6–1.0 V)for ***,the Pt-Ni HSNs show enhanced activity and anti-toxic ability in CO for *** superb activity of the Pt-Ni HSNs for ORR and MOR is fully attributed to an extensively exposed electrochemical surface area and high intrinsic activity,induced by strain effects,provided by the unique hierarchically skeletal alloy *** novel open and hierarchical structure of Pt-Ni alloy provides a promising approach for significant improvements of the activity of Pt based alloy electrocatalysts.

摘要：长寿命溶解氧海水电池是深远海观测能源网络的重要组成单元,但海水贫氧复杂环境对设计高性能氧还原催化剂提出了重要挑战.本文以酞菁铁为模型催化剂,通过理论计算与实验验证,提出了活性位点电子轴向拉伸可大幅提升催化剂在极端贫氧环境中的氧还原活性和稳定性.该研究为构建高性能海水电池提供了材料学解决方案,同时为极端环境下催化剂的变革性设计提供了新的思路.