@article{10fc2970e3cf47b88c8955630138b79f,
title = "N8 stabilized single-atom Pd for highly selective hydrogenation of acetylene",
abstract = "Single-atom catalysts show a promising future in many reactions even though great challenges still remain such as facile synthesis and long stability. In this work, a single-atom Pd catalyst attached to a designed N8 Lewis base species (Pd1-N8/CNT) is synthesized with cyclic voltammetry (CV) method. The catalyst demonstrates long stability and enhanced C2H4 selectivity in selective hydrogenation of acetylene at 40 °C. CV is carried out in a three-electrode setup with PdO/CNT as the working electrode in NaN3 solution. HAADF-STEM confirms single-atom Pd sites are successfully isolated. XPS measurements and Bader charge calculations indicate N8 is effectively synthesized on CNT substrate after CV treatment while single-atom Pd is stabilized by attaching to the end N of N8. Acetylene-temperature programed desorption (C2H2-TPD) and density functional theory (DFT) calculations suggest C2H2 favors the π bonding on single Pd atom, while H2 dissociates on the N atom (next to Pd) instead of conventionally on Pd. The synergistic effect favors C2H4 formation but prevents full hydrogenation of acetylene to C2H6. This work opens up a new perspective to design and synthesize more selective catalysts with isolated single-atom sites.",
keywords = "Cyclic voltammetry, Density functional theory, Polynitrogen, Selective hydrogenation of acetylene, Single-atom catalyst",
author = "Maocong Hu and Zhiyi Wu and Zhenhua Yao and Joshua Young and Langli Luo and Yingge Du and Chongmin Wang and Zafar Iqbal and Xianqin Wang",
note = "Funding Information: This work was supported by an ACS-PRF 53582-ND10 and partially NSF CBET-1804949. C. Wang thanks the support of PNNL LDRD. The microscopic and XPS analysis in this work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE{\textquoteright}s Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for the Department of Energy under Contract DE-AC05-76RLO1830. M. Hu thanks the support from Science and Technology Research Project of Education Department of Hubei Province (B2020229). DFT calculations were performed using the Kong and Lochness High Performance Computing clusters at the New Jersey Institute of Technology. Funding Information: This work was supported by an ACS-PRF 53582-ND10 and partially NSF CBET-1804949. C. Wang thanks the support of PNNL LDRD. The microscopic and XPS analysis in this work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for the Department of Energy under Contract DE-AC05-76RLO1830. M. Hu thanks the support from Science and Technology Research Project of Education Department of Hubei Province (B2020229). DFT calculations were performed using the Kong and Lochness High Performance Computing clusters at the New Jersey Institute of Technology. Publisher Copyright: {\textcopyright} 2020 Elsevier Inc.",
year = "2021",
month = mar,
doi = "10.1016/j.jcat.2020.12.009",
language = "English (US)",
volume = "395",
pages = "46--53",
journal = "Journal of Catalysis",
issn = "0021-9517",
publisher = "Academic Press Inc.",
}