Fully exposed Ptn cluster catalysts enable cascade oxidation of polyol to dicarboxylic acid

Hao Yan, Jie Li, Zhiqiang Rao, Ying Liao, Yaqian Li, Xin Zhou, Fanchun Meng, Lina Li, Bin Zhang, Yong Qin, Hui Zhao, Yibin Liu, Xiaobo Chen, Xiang Feng (), Chen De, Chaohe Yang and Ding Ma ()
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Hao Yan: China University of Petroleum (East China)
Jie Li: China University of Petroleum (East China)
Zhiqiang Rao: Peking University
Ying Liao: China University of Petroleum (East China)
Yaqian Li: China University of Petroleum (East China)
Xin Zhou: Ocean University of China
Fanchun Meng: Chinese Academy of Sciences
Lina Li: Chinese Academy of Sciences
Bin Zhang: Chinese Academy of Sciences
Yong Qin: Chinese Academy of Sciences
Hui Zhao: China University of Petroleum (East China)
Yibin Liu: China University of Petroleum (East China)
Xiaobo Chen: China University of Petroleum (East China)
Xiang Feng: China University of Petroleum (East China)
Chen De: Norwegian University of Science and Technology
Chaohe Yang: China University of Petroleum (East China)
Ding Ma: Peking University

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract The polyol oxidation to dicarboxylic acid, a crucial value-accretive reaction, is still challenging due to the paradoxical relationship between efficient activation of C-H bond and rapid desorption of carboxylic acid. Herein, we break this contradiction by constructing fully exposed Ptn cluster supported on hydroxyapatite (Ptn/HAP) to promote two primary hydroxyl groups of polyol oxidation to dicarboxylic acid. Such fully exposed Ptn cluster with an average Pt-Pt coordination number of ∼3.4 exhibits unique electronic properties between Pt1 single atom and nanoparticle Ptp. Specifically, gradient charge distribution in fully exposed Ptn cluster shows a special synergistic effect in the C-H bond activation. Moreover, the d-band centre of fully exposed Ptn cluster moderately far from the Fermi level weakens the adsorption of C = O bond in dicarboxylic acid product. As a result, fully exposed Ptn/HAP with better catalytic activity (turnover frequency: 619.1 h−1) shows nearly 10 times and 1.5 times of tartronic acid selectivity than Pt1 single atom and nanoparticle Ptp catalysts, respectively. The system is also applicable to other polyol oxidation to dicarboxylic acids with noteworthy catalytic results.

Date: 2025
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DOI: 10.1038/s41467-025-62192-0

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