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Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

Author

Listed:
  • Xiaohu Ge

    (East China University of Science and Technology)

  • Mingying Dou

    (East China University of Science and Technology)

  • Yueqiang Cao

    (East China University of Science and Technology)

  • Xi Liu

    (Shanghai Jiao Tong University)

  • Qiang Yuwen

    (East China University of Science and Technology)

  • Jing Zhang

    (East China University of Science and Technology)

  • Gang Qian

    (East China University of Science and Technology)

  • Xueqing Gong

    (East China University of Science and Technology)

  • Xinggui Zhou

    (East China University of Science and Technology)

  • Liwei Chen

    (Shanghai Jiao Tong University)

  • Weikang Yuan

    (East China University of Science and Technology)

  • Xuezhi Duan

    (East China University of Science and Technology)

Abstract

Mechanism driven catalyst design with atomically uniform ensemble sites is an important yet challenging issue in heterogeneous catalysis associated with breaking the activity-selectivity trade-off. Herein, a trimer Ni1Sb2 site in NiSb intermetallic featuring superior selectivity is elaborated for acetylene semi-hydrogenation via a theoretical guidance with a precise synthesis strategy. The trimer Ni1Sb2 site in NiSb intermetallic is predicted to endow acetylene reactant with an adequately but not excessively strong σ-adsorption mode while ethylene product with a weak π-adsorption one, where such compromise delivers higher ethylene formation rate. An in-situ trapping of molten Sb by Ni strategy is developed to realize the construction of Ni1Sb2 site in the intermetallic P63/mmc NiSb catalysts. Such catalyst exhibits ethylene selectivity up to 93.2% at 100% of acetylene conversion, significantly prevailing over the referred Ni catalyst. These insights shed new lights on rational catalyst design by taming active sites to energetically match targeted reaction pathway.

Suggested Citation

  • Xiaohu Ge & Mingying Dou & Yueqiang Cao & Xi Liu & Qiang Yuwen & Jing Zhang & Gang Qian & Xueqing Gong & Xinggui Zhou & Liwei Chen & Weikang Yuan & Xuezhi Duan, 2022. "Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33250-8
    DOI: 10.1038/s41467-022-33250-8
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    1. Aijuan Han & Jian Zhang & Wenming Sun & Wenxing Chen & Shaolong Zhang & Yunhu Han & Quanchen Feng & Lirong Zheng & Lin Gu & Chen Chen & Qing Peng & Dingsheng Wang & Yadong Li, 2019. "Isolating contiguous Pt atoms and forming Pt-Zn intermetallic nanoparticles to regulate selectivity in 4-nitrophenylacetylene hydrogenation," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    2. Fei Huang & Yuchen Deng & Yunlei Chen & Xiangbin Cai & Mi Peng & Zhimin Jia & Jinglin Xie & Dequan Xiao & Xiaodong Wen & Ning Wang & Zheng Jiang & Hongyang Liu & Ding Ma, 2019. "Anchoring Cu1 species over nanodiamond-graphene for semi-hydrogenation of acetylene," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
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    Cited by:

    1. Wangwang Zhang & Kelechi Uwakwe & Jingting Hu & Yan Wei & Juntong Zhu & Wu Zhou & Chao Ma & Liang Yu & Rui Huang & Dehui Deng, 2024. "Ambient-condition acetylene hydrogenation to ethylene over WS2-confined atomic Pd sites," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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