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Breaking scaling relationships in alkynol semi-hydrogenation by manipulating interstitial atoms in Pd with d-electron gain

Author

Listed:
  • Yang Yang

    (Shanghai Normal University)

  • Xiaojuan Zhu

    (Shanghai Normal University)

  • Lili Wang

    (Shanghai Normal University)

  • Junyu Lang

    (Shanghai Tech University)

  • Guohua Yao

    (Shanghai Normal University)

  • Tian Qin

    (Shanghai Jiao Tong University)

  • Zhouhong Ren

    (Shanghai Jiao Tong University)

  • Liwei Chen

    (Shanghai Jiao Tong University
    Shanghai Jiao Tong University)

  • Xi Liu

    (Shanghai Jiao Tong University)

  • Wei Li

    (Fudan University)

  • Ying Wan

    (Shanghai Normal University)

Abstract

Pd catalysts are widely used in alkynol semi-hydrogenation. However, due to the existence of scaling relationships of adsorption energies between the key adsorbed species, the increase in conversion is frequently accompanied by side reactions, thereby reducing the selectivity to alkenols. We report that the simultaneous increase in alkenol selectivity and alkynol conversion is achieved by manipulating interstitial atoms including B, P, C, S and N in Pd catalysts. A negative linear relationship is observed between the activation entropies of 2-methyl-3-butyn-2-ol and 2-methyl-3-buten-2-ol which is highly related to the filling of d-orbital of Pd catalysts by the modification of p-block elements. A catalyst co-modified by B and C atoms has the maximum d charge of Pd that achieves a 17-fold increase in the turn-over frequency values compared to the Lindlar catalysts in the semi-hydrogenation of 2-methyl-3-butyn-2-ol. When the conversion is close to 100%, the selectivity can be as high as 95%.

Suggested Citation

  • Yang Yang & Xiaojuan Zhu & Lili Wang & Junyu Lang & Guohua Yao & Tian Qin & Zhouhong Ren & Liwei Chen & Xi Liu & Wei Li & Ying Wan, 2022. "Breaking scaling relationships in alkynol semi-hydrogenation by manipulating interstitial atoms in Pd with d-electron gain," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30540-z
    DOI: 10.1038/s41467-022-30540-z
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    References listed on IDEAS

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    1. Xiaojuan Zhu & Qishui Guo & Yafei Sun & Shangjun Chen & Jian-Qiang Wang & Mengmeng Wu & Wenzhao Fu & Yanqiang Tang & Xuezhi Duan & De Chen & Ying Wan, 2019. "Optimising surface d charge of AuPd nanoalloy catalysts for enhanced catalytic activity," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
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    Cited by:

    1. Zhongzhe Wei & Zijiang Zhao & Chenglong Qiu & Songtao Huang & Zihao Yao & Mingxuan Wang & Yi Chen & Yue Lin & Xing Zhong & Xiaonian Li & Jianguo Wang, 2023. "Tripodal Pd metallenes mediated by Nb2C MXenes for boosting alkynes semihydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Jinqi Xiong & Shanjun Mao & Qian Luo & Honghui Ning & Bing Lu & Yanling Liu & Yong Wang, 2024. "Mediating trade-off between activity and selectivity in alkynes semi-hydrogenation via a hydrophilic polar layer," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Anubhab Acharya & Trimbak Baliram Mete & Nitee Kumari & Youngkwan Yoon & Hayoung Jeong & Taehyung Jang & Byeongju Song & Hee Cheul Choi & Jeong Woo Han & Yoonsoo Pang & Yongju Yun & Amit Kumar & In Su, 2023. "Ultrathin covalent organic overlayers on metal nanocrystals for highly selective plasmonic photocatalysis," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Hongqiang Jin & Kaixin Zhou & Ruoxi Zhang & Hongjie Cui & Yu Yu & Peixin Cui & Weiguo Song & Changyan Cao, 2023. "Regulating the electronic structure through charge redistribution in dense single-atom catalysts for enhanced alkene epoxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Jun Bu & Siyu Chang & Jinjin Li & Sanyin Yang & Wenxiu Ma & Zhenpeng Liu & Siying An & Yanan Wang & Zhen Li & Jian Zhang, 2023. "Highly selective electrocatalytic alkynol semi-hydrogenation for continuous production of alkenols," Nature Communications, Nature, vol. 14(1), pages 1-9, December.

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