Zhang Xi, Cui Guoqing, Feng Haisong, Chen Lifang, Wang Hui, Wang Bin, Zhang Xin, Zheng Lirong, Hong Song, Wei Min
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, 100029, Beijing, P. R. China.
Beijing Research Institute of Chemical Industry, Sinopec Group, 100013, Beijing, P. R. China.
Nat Commun. 2019 Dec 20;10(1):5812. doi: 10.1038/s41467-019-13685-2.
Selective hydrogenolysis of biomass-derived glycerol to propanediol is an important reaction to produce high value-added chemicals but remains a big challenge. Herein we report a PtCu single atom alloy (SAA) catalyst with single Pt atom dispersed on Cu nanoclusters, which exhibits dramatically boosted catalytic performance (yield: 98.8%) towards glycerol hydrogenolysis to 1,2-propanediol. Remarkably, the turnover frequency reaches up to 2.6 × 10 mol·mol·h, which is to our knowledge the largest value among reported heterogeneous metal catalysts. Both in situ experimental studies and theoretical calculations verify interface sites of PtCu-SAA serve as intrinsic active sites, in which the single Pt atom facilitates the breakage of central C-H bond whilst the terminal C-O bond undergoes dissociation adsorption on adjacent Cu atom. This interfacial synergistic catalysis based on PtCu-SAA changes the reaction pathway with a decreased activation energy, which can be extended to other noble metal alloy systems.
将生物质衍生的甘油选择性氢解为丙二醇是生产高附加值化学品的重要反应，但仍然是一个巨大的挑战。在此，我们报道了一种PtCu单原子合金（SAA）催化剂，其中单个Pt原子分散在Cu纳米团簇上，该催化剂对甘油氢解为1,2-丙二醇表现出显著提高的催化性能（产率：98.8%）。值得注意的是，周转频率高达2.6×10 mol·mol·h，据我们所知，这是报道的多相金属催化剂中的最大值。原位实验研究和理论计算均证实，PtCu-SAA的界面位点是本征活性位点，其中单个Pt原子促进中心C-H键的断裂，而末端C-O键在相邻的Cu原子上发生解离吸附。这种基于PtCu-SAA的界面协同催化改变了反应途径，降低了活化能，并且可以扩展到其他贵金属合金体系。
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