TY - JOUR

T1 - One-pot functionalization of catalytically derived carbon nanostructures with heteroatoms for toxic-free environment

AU - Brzhezinskaya, Maria

AU - Mishakov, Ilya V.

AU - Bauman, Yury I.

AU - Shubin, Yury V.

AU - Maksimova, Tatyana A.

AU - Stoyanovskii, Vladimir O.

AU - Yu. Gerasimov, Evgeny

AU - Vedyagin, Aleksey A.

N1 - Funding Information: The present research was partially supported by Ministry of Science and Higher Education of the Russian Federation (projects AAAA-A21-121011390054-1 and N121031700315-2). Funding Information: The authors are grateful to the Helmholtz-Zentrum Berlin (HZB) for allocation of synchrotron radiation beamtime for the experiments at the RGBL beamline of BESSY II of HZB. M.B. acknowledges Dmitry Smirnov for technical support during experiments at RGBL. Characterization of the samples was performed using the equipment of the Center of Collective Use ?National Center of Catalysts Research?. The present research was partially supported by Ministry of Science and Higher Education of the Russian Federation (projects AAAA-A21-121011390054-1 and N121031700315-2). The raw/processed data required to reproduce these findings cannot be shared at this time as the data also forms part of an ongoing study. Publisher Copyright: © 2022 Elsevier B.V.

PY - 2022/7/15

Y1 - 2022/7/15

N2 - Nowadays, catalytic methods of utilization of industrial organic wastes are widely developing. Chlorinated hydrocarbons represent the most important class of substances, which should be efficiently converted into value-added product, e.g., carbon nanostructures. Present work demonstrates results of comprehensive investigation and characterization of the electronic state of all elements composing the structure of functionalized carbon nanomaterials obtained via catalytic decomposition of 1,2-C2H4Cl2 and co-substrates (acetonitrile, ethanol, NH4OH) over Ni-Pd alloy using high-resolution synchrotron-based X-ray photoelectron spectroscopy along with NEXAFS spectroscopy. This study is focused on a deeper understanding of reactions proceeding on surface of catalytic particles. Obtained data make it possible for the transition from the description of the nature of chemical reactions to target and controllable tailoring of the molecular structure of carbon nanostructures emergent as a result of complex chemical process realization. The maximum content of chlorine atoms bound to carbon was observed for the sample obtained via decomposition of pure 1,2-C2H4Cl2. Presence of C2H5OH slightly decreases the proportion of Cl-atoms chemically bound to carbon. A more considerable effect was observed when CH3CN vapors were added. The strongest impact on process and defectiveness of the carbon material was ascertained for NH4OH, when the number of C-Cl atoms reached 75.1%.

AB - Nowadays, catalytic methods of utilization of industrial organic wastes are widely developing. Chlorinated hydrocarbons represent the most important class of substances, which should be efficiently converted into value-added product, e.g., carbon nanostructures. Present work demonstrates results of comprehensive investigation and characterization of the electronic state of all elements composing the structure of functionalized carbon nanomaterials obtained via catalytic decomposition of 1,2-C2H4Cl2 and co-substrates (acetonitrile, ethanol, NH4OH) over Ni-Pd alloy using high-resolution synchrotron-based X-ray photoelectron spectroscopy along with NEXAFS spectroscopy. This study is focused on a deeper understanding of reactions proceeding on surface of catalytic particles. Obtained data make it possible for the transition from the description of the nature of chemical reactions to target and controllable tailoring of the molecular structure of carbon nanostructures emergent as a result of complex chemical process realization. The maximum content of chlorine atoms bound to carbon was observed for the sample obtained via decomposition of pure 1,2-C2H4Cl2. Presence of C2H5OH slightly decreases the proportion of Cl-atoms chemically bound to carbon. A more considerable effect was observed when CH3CN vapors were added. The strongest impact on process and defectiveness of the carbon material was ascertained for NH4OH, when the number of C-Cl atoms reached 75.1%.

KW - Core-level spectroscopies

KW - Heteroatom-doped carbon nanofibers

KW - Metal dusting

KW - One-pot functionalization

KW - Self-organizing catalyst

KW - Toxic free environment

UR - http://www.scopus.com/inward/record.url?scp=85126851784&partnerID=8YFLogxK

U2 - 10.1016/j.apsusc.2022.153055

DO - 10.1016/j.apsusc.2022.153055

M3 - Article

AN - SCOPUS:85126851784

VL - 590

JO - Applied Surface Science

JF - Applied Surface Science

SN - 0169-4332

M1 - 153055

ER -