Key Lab of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
Department of Chemistry and Biochemistry, San Diego State University, 5500 Campanile Drive, San Diego, CA, 92182-1030, USA.
Nat Commun. 2019 Feb 28;10(1):982. doi: 10.1038/s41467-019-08877-9.
Engineering catalytic sites at the atomic level provides an opportunity to understand the catalyst's active sites, which is vital to the development of improved catalysts. Here we show a reliable and tunable polyoxometalate template-based synthetic strategy to atomically engineer metal doping sites onto metallic 1T-MoS, using Anderson-type polyoxometalates as precursors. Benefiting from engineering nickel and oxygen atoms, the optimized electrocatalyst shows great enhancement in the hydrogen evolution reaction with a positive onset potential of ~ 0 V and a low overpotential of -46 mV in alkaline electrolyte, comparable to platinum-based catalysts. First-principles calculations reveal co-doping nickel and oxygen into 1T-MoS assists the process of water dissociation and hydrogen generation from their intermediate states. This research will expand on the ability to improve the activities of various catalysts by precisely engineering atomic activation sites to achieve significant electronic modulations and improve atomic utilization efficiencies.
在原子水平上设计催化位点为理解催化剂的活性位点提供了机会，这对于开发改进的催化剂至关重要。在这里，我们展示了一种可靠且可调的多金属氧酸盐模板合成策略，通过将安德森型多金属氧酸盐作为前体，在金属 1T-MoS 上原子级设计金属掺杂位点。受益于镍和氧原子的工程化，优化后的电催化剂在碱性电解质中表现出优异的析氢反应性能，具有正的起始电位约为 0 V 和低的过电势-46 mV，可与基于铂的催化剂相媲美。第一性原理计算表明，将镍和氧共掺杂到 1T-MoS 中有助于水离解和从中间态生成氢气的过程。这项研究将通过精确设计原子活性位点来提高各种催化剂的活性的能力扩展到实现显著的电子调制和提高原子利用率。
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