Selective dehydrogenation of formic acid (FA, HCOOH) is a promising alternative to fossil fuels, to provide a clean energy carrier for the future energy economy. The preparation of highly efficient catalysts for hydrogen release from FA at room temperature has attracted much attention but still remains a great challenge. Herein, ultrafine bimetallic PdIr nanoparticles (NPs) immobilized by amine-functionalized SBA-15 (PdIr/SBA-15-NH₂) have been successfully synthesized via a facile surface functionalization and co-reduction method. The characterized results showed that ultrafine bimetallic PdIr NPs with a small size of around 1.1 nm were highly dispersed on SBA-15-NH₂. Among all the as-synthesized catalysts, the optimized Pd_0.85Ir_0.15/SBA-15-NH₂ nanocomposites (NCs) exhibited the highest catalytic activity and 100% H₂ selectivity toward the selective dehydrogenation of FA, giving an initial turnover frequency (TOF) value as high as 3087 h⁻¹ at room temperature. To the best of our knowledge, this is the first report showing that the Ir-containing heterogeneous catalyst can achieve a complete dehydrogenation of FA to H₂. The excellent catalytic performance of this catalyst might be attributed to the modified electronic effects of Pd with Ir, the ultrafine size and high dispersion of PdIr NPs, and the synergetic interaction between the PdIr NPs and SBA-15-NH₂. The amine functional groups of SBA-15-NH₂ not only can lead to ultrafine and well-dispersed PdIr NPs and stabilize the PdIr NPs, but also can serve as Brønsted basic sites, which facilitates the O–H bond dissociation of FA and forms a formate intermediate. The present PdIr/SBA-15-NH₂ NCs with efficient catalytic effects on the dehydrogenation of FA may greatly promote the practical application of the FA system on fuel cells.

中文翻译：

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胺官能化介孔二氧化硅负载的PdIr催化剂：促进甲酸在室温下产生氢气

甲酸（FA，HCOOH）的选择性脱氢是一种有前途的替代化石燃料的方法，可为未来的能源经济提供清洁的能源载体。室温下从FA释放氢的高效催化剂的制备备受关注，但仍然是巨大的挑战。在此，已经通过简便的表面官能化和共还原方法成功地合成了由胺官能化的SBA-15（PdIr / SBA-15-NH ₂）固定的超细双金属PdIr纳米颗粒（NPs）。表征结果表明，在SBA-15-NH ₂上高度分散的超细双金属PdIr NPs的大小约为1.1 nm 。在所有合成的催化剂中，优化的Pd _0.85 Ir_0.15 / SBA-15-NH ₂纳米复合材料（NCs）对FA的选择性脱氢表现出最高的催化活性和100％H ₂选择性，在室温下的初始转换频率（TOF）值高达3087 h ^-1。据我们所知，这是第一份报告，表明含Ir的多相催化剂可以实现FA完全脱氢为H ₂。该催化剂的优异催化性能可能归因于钯与Ir的修饰电子效应，PdIr NPs的超细尺寸和高分散性以及PdIr NP与SBA-15-NH ₂的协同作用。SBA-15-NH ₂的胺官能团不仅可以导致超细和良好分散的PdIr NP，并稳定PdIr NP，还可以作为布朗斯台德碱性位点，促进FA的O–H键解离并形成甲酸酯中间体。目前对FA脱氢具有有效催化作用的PdIr / SBA-15-NH ₂ NCs可以大大促进FA系统在燃料电池上的实际应用。