Ligand-Free Noble Metal Nanocluster Catalysts on Carbon Supports via "Soft" Nitriding.
Ligand-Free Noble Metal Nanocluster Catalysts on Carbon Supports via "Soft" Nitriding.
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DOI：
10.1021/jacs.6b01702
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发表时间：
2016-04-13
影响因子：
15
通讯作者：
He J
中科院分区：
文献类型：
--
作者：
Liu B;Yao H;Song W;Jin L;Mosa IM;Rusling JF;Suib SL;He J
我们报道了一种健壮的、通用的“软”氮化方法，可以在碳上原位生长无配体的超小型贵金属纳米催化剂(例如，金、钯和铂)。采用300°C的低温尿素预处理，软氮化使碳载体表面的含氮物种丰富，并增强了贵金属前驱体在这些载体上的亲和力。我们展示了通过化学还原或热分解在七种不同类型的氮化碳上原位生长亚2 nm、无配体的UNN。与具有表面封端剂或相同碳载体上的较大纳米晶的载体相比，碳载体上的无配体MUNN对甲醇氧化表现出更好的电催化活性。我们的方法有望为在各种载体上制备无配体的UNN提供指导，并拓宽其在能量转换和电化学催化中的应用。
We report a robust, universal “soft” nitriding method to grow in situ ligand-free ultrasmall noble metal nanocatalysts (UNMN; e.g., Au, Pd, and Pt) onto carbon. Using low-temperature urea pretreatment at 300 °C, soft nitriding enriches nitrogen-containing species on the surface of carbon supports and enhances the affinity of noble metal precursors onto these supports. We demonstrated sub-2-nm, ligand-free UNMNs grown in situ on seven different types of nitrided carbons with no organic ligands via chemical reduction or thermolysis. Ligand-free UNMNs supported on carbon showed superior electrocatalytic activity for methanol oxidation compared to counterparts with surface capping agents or larger nanocrystals on the same carbon supports. Our method is expected to provide guidelines for the preparation of ligand-free UNMNs on a variety of supports and, additionally, to broaden their applications in energy conversion and electrochemical catalysis.