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Anti-Corrosive SnS_2/SnO_2 Heterostructured Support for Pt Nanoparticles Enables Remarkable Oxygen Reduction Catalysis via Interfacial Enhancement

机译:Pt纳米颗粒的防腐蚀SnS_2/SnO_2异质结构支持通过界面增强实现显著的氧还原催化

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摘要

The stability of Pt-based catalysts for oxygen reduction reaction (ORR) inhydrogen fuel cells is seriously handicapped by the corrosion of their carbonsupports at high potentials and acidic environments. Herein, a novel SnS_2/SnO_2 hetero-structured support is reported for Pt nanoparticles (NPs) as theORR catalyst, where Pt NPs are mainly deposited at the interfaces of SnS_2and SnO_2 moieties. The Pt-support interactions, which can be tuned by theconcentration of the heterointerfaces, can accelerate the electronic transferand enrich the electron density of Pt with a favorable shift of the d-bandcenter. In electrochemical measurements, the ORR mass activity (MA) of theoptimal Pt-SnS_2/SnO_2 catalyst at 0.9 V versus RHE (0.40 A mg_(Pt)~(?1)) is fourtimes higher than that of Pt/C. As for the stability, the electrochemical activesurface area and MA of Pt-SnS_2/SnO_2 are only decreased by 18.2 and 23.7after 50 000 potential cycles at a high potential region (1.0-1.6 V), representingthe best ORR stability among the reported Pt-based catalysts. Densityfunctional theory calculations indicate that the binding energy and migrationbarrier of Pt atom/cluster on the SnS_2/SnO_2 heterojunction are much higherrelative to other supports, accounting for the outstanding stability of thecatalyst.
机译:铂基催化剂在氢燃料电池中氧还原反应(ORR)的稳定性受到其碳载体在高电位和酸性环境下的腐蚀的严重影响。本文报道了一种新型的SnS_2/SnO_2异质结构载体,以Pt纳米颗粒(NPs)作为ORR催化剂,其中Pt纳米颗粒主要沉积在SnS_2和SnO_2部分的界面上。Pt-载体相互作用可以通过异质界面的浓度来调节,可以加速电子转移,并通过d波段中心的有利位移来丰富Pt的电子密度。在电化学测量中,最佳Pt-SnS_2/SnO_2催化剂在0.9 V与RHE的ORR质量活度(MA)为0.40 A mg_(Pt)~(?1))是Pt/C的4倍。在稳定性方面,Pt-SnS_2/SnO_2在高电位区(1.0-1.6 V)循环50 000次后,电化学活性表面积和MA分别降低了18.2%和23.7%,是已报道的Pt基催化剂中ORR稳定性最好的。密度泛函理论计算表明,Pt原子/团簇在SnS_2/SnO_2异质结上的结合能和迁移势垒相对于其他载体要高得多,这是催化剂具有突出稳定性的原因。

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