2026-04-02 中国科学院（CAS）
Catalyst structural characterization. (a) Synthesis schematic, (b-f) HAADF-STEM images and corresponding line intensity profiles, (g) Pd K-edge XANES spectra, (h-i) Pd EXAFS spectra and their fitting. (Image by IMR)
＜関連情報＞
- https://english.cas.cn/newsroom/research-news/202604/t20260402_1155060.shtml
- https://www.nature.com/articles/s41467-026-70107-w
Pd2二原子サイトによるアセチレン半水素化における活性選択性のトレードオフの打破 Breaking the activity-selectivity trade-off for acetylene semihydrogenation by Pd2 dual-atom site
Feng Hong,Hongqiu Chen,Jiawei Chen,Zhehan Ying,Mi Peng,Jingwang Zhang,Zuodong Yang,Guodong Wen,Jiangyong Diao,Bo Sun,Geng Sun,Ding Ma & Hongyang Liu
Nature Communications Published:25 March 2026
DOI:https://doi.org/10.1038/s41467-026-70107-w Unedited version
Abstract
Acetylene semihydrogenation is a critical process in the polyolefin industry by selectively removing trace acetylene from ethylene-rich reformate. However, this reaction is generally limited by the inherent activity-selectivity trade-off due to the thermodynamic advantage of overhydrogenation. Herein, we develop a facile and straightforward strategy to construct Pd2 dual-atom sites anchored on defect-rich surface-graphitized nanodiamond (ND@G) via the solvent-mediated dispersion of palladium carboxylate driven by the chelation of palladium precursors via carboxylate anion. Cs-corrected HAADF-STEM images coupled with XAS analysis unambiguously manifest the successful architecting of Pd2 dual-atom sites. Compared to Pd1 single-atom sites, the obtained Pd2/ND@G sample demonstrates superior catalytic performance in acetylene semihydrogenation, with the corresponding TOF values increased from 0.151 s−1 to 1.953 s−1, without the obvious decline of ethylene selectivity (93.2%, at full acetylene conversion). C2H2/C2H4-TPD, H2-D2 exchange reaction, isotope-labeled TPSR combined with DFT calculations confirm the effective co-activation of C2H2/H2 on Pd2 dual-atom sites while maintaining the weak adsorption of ethylene similar to that on its single-atom sites, which can break the activity-selectivity trade-off in acetylene semihydrogenation.
