Single platinum atoms embedded in nanoporous cobalt selenide as electrocatalyst for accelerating hydrogen evolution reaction
Single platinum atoms embedded in nanoporous cobalt selenide as electrocatalyst for accelerating hydrogen evolution reaction
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嵌入纳米多孔硒化钴中的单铂原子作为加速析氢反应的电催化剂
DOI：
10.1038/s41467-019-09765-y
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发表时间：
2019-04-15
影响因子：
16.6
通讯作者：
Tan, Yongwen
中科院分区：
文献类型：
--
作者：
Jiang, Kang;Liu, Boyang;Tan, Yongwen
设计高效的析氢电催化剂对可再生能源的可持续利用具有重要意义。在这里，我们报告单原子铂修饰的纳米多孔Co 0. 85 Se（Pt/np-Co 0. 85 Se）作为有效的析氢电催化剂。Pt/np-Co 0. 85 Se催化剂具有很高的催化性能，起始过电位接近零，在中性介质中的Tafel斜率为35 mV dec−1，在-100 mV时的转换频率为3.93 s− 1，优于商业Pt/C催化剂和其他已报道的过渡金属基化合物。结合密度泛函理论计算的X射线吸收谱研究表明，Pt/np-Co 0. 85 Se中的单原子Pt不仅可以优化Co 0. 85 Se活性中心在实际工作条件下的表面状态，而且可以显著降低水解离的能垒，改善氢的吸附/脱附行为，从而协同促进热力学和动力学。这项工作开辟了进一步的机会，局部电子结构调整的电催化剂，有效地操纵其催化性能的原子级工程策略。
Designing efficient electrocatalysts for hydrogen evolution reaction is significant for renewable and sustainable energy conversion. Here, we report single-atom platinum decorated nanoporous Co0.85Se (Pt/np-Co0.85Se) as efficient electrocatalysts for hydrogen evolution. The achieved Pt/np-Co0.85Se shows high catalytic performance with a near-zero onset overpotential, a low Tafel slope of 35 mV dec−1, and a high turnover frequency of 3.93 s−1at −100 mV in neutral media, outperforming commercial Pt/C catalyst and other reported transition-metal-based compounds. Operando X-ray absorption spectroscopy studies combined with density functional theory calculations indicate that single-atom platinum in Pt/np-Co0.85Se not only can optimize surface states of Co0.85Se active centers under realistic working conditions, but also can significantly reduce energy barriers of water dissociation and improve adsorption/desorption behavior of hydrogen, which synergistically promote thermodynamics and kinetics. This work opens up further opportunities for local electronic structures tuning of electrocatalysts to effectively manipulate its catalytic properties by an atomic-level engineering strategy.