Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering and College of Engineering, and BIC-ESAT, Peking University, Beijing, China.
State Key Laboratory of Fine Chemicals, College of Chemical Engineering, Dalian University of Technology, Dalian, China.
Nature. 2021 Jan;589(7842):396-401. doi: 10.1038/s41586-020-03130-6. Epub 2021 Jan 20.
The water-gas shift (WGS) reaction is an industrially important source of pure hydrogen (H) at the expense of carbon monoxide and water. This reaction is of interest for fuel-cell applications, but requires WGS catalysts that are durable and highly active at low temperatures. Here we demonstrate that the structure (Pt-Pt)/α-MoC, where isolated platinum atoms (Pt) and subnanometre platinum clusters (Pt) are stabilized on α-molybdenum carbide (α-MoC), catalyses the WGS reaction even at 313 kelvin, with a hydrogen-production pathway involving direct carbon monoxide dissociation identified. We find that it is critical to crowd the α-MoC surface with Pt and Pt species, which prevents oxidation of the support that would cause catalyst deactivation, as seen with gold/α-MoC (ref. ), and gives our system high stability and a high metal-normalized turnover number of 4,300,000 moles of hydrogen per mole of platinum. We anticipate that the strategy demonstrated here will be pivotal for the design of highly active and stable catalysts for effective activation of important molecules such as water and carbon monoxide for energy production.
水气变换(WGS)反应是一种工业上重要的制氢方法,以一氧化碳和水为代价产生纯氢气(H)。该反应对于燃料电池应用具有重要意义,但需要具有耐用性和在低温下高活性的 WGS 催化剂。在这里,我们证明了结构(Pt-Pt)/α-MoC 可以催化 WGS 反应,即使在 313 开尔文下也具有催化活性,其中涉及到直接一氧化碳解离的产氢途径。我们发现,将 Pt 和 Pt 物种密集地堆积在α-MoC 表面非常重要,这可以防止载体氧化导致催化剂失活,就像金/α-MoC(参考文献)一样,并且使我们的系统具有高稳定性和高金属归一化周转率,每摩尔铂可产生 4,300,000 摩尔氢气。我们预计,这里展示的策略对于设计高效和稳定的催化剂将至关重要,这些催化剂可以有效地激活重要分子,如水和一氧化碳,以用于能源生产。