A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
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一种制备加氢中具有高化学选择性和区域选择性的单原子催化剂的通用途径
DOI：
10.1038/s41467-019-11619-6
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发表时间：
2019-08-14
影响因子：
16.6
通讯作者：
Ji, Hongbing
中科院分区：
文献类型：
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作者：
He, Xiaohui;He, Qian;Ji, Hongbing
单原子催化剂(SACS)的制备是材料科学家和化学家广泛关注的问题，但仍然是一个巨大的挑战。在这里，我们开发了一种有效的合成SACS的方法，即通过前体稀释策略，将金属卟啉(MTPP)与目标金属与稀释剂(四苯基卟啉，TPP)共聚，然后裂解得到N掺杂的多孔碳负载SACS(M1/N-C)。成功地制备了包括贵金属和非贵金属在内的24种不同的囊泡。此外，还合成了一系列具有不同表面原子密度、双金属中心和金属聚集态的催化剂。这种方法具有显著的可调性和通用性，为原子尺度的催化剂设计和探索SACS独特的催化性能提供了足够的自由度。作为例子，我们发现所制备的Pt1/N-C在加氢反应中表现出良好的化学选择性和区域选择性。它只将末端的炔烃转化为烯烃，而保持其他可还原的官能团，如烯基、硝基，甚至内部炔烃的完整性。
Preparation of single atom catalysts (SACs) is of broad interest to materials scientists and chemists but remains a formidable challenge. Herein, we develop an efficient approach to synthesize SACs via a precursor-dilution strategy, in which metalloporphyrin (MTPP) with target metals are co-polymerized with diluents (tetraphenylporphyrin, TPP), followed by pyrolysis to N-doped porous carbon supported SACs (M1/N-C). Twenty-four different SACs, including noble metals and non-noble metals, are successfully prepared. In addition, the synthesis of a series of catalysts with different surface atom densities, bi-metallic sites, and metal aggregation states are achieved. This approach shows remarkable adjustability and generality, providing sufficient freedom to design catalysts at atomic-scale and explore the unique catalytic properties of SACs. As an example, we show that the prepared Pt1/N-C exhibits superior chemoselectivity and regioselectivity in hydrogenation. It only converts terminal alkynes to alkenes while keeping other reducible functional groups such as alkenyl, nitro group, and even internal alkyne intact.