TY - JOUR

T1 - Catalytic conversion of 1,2-dichloroethane over Ni-Pd system into filamentous carbon material

AU - Bauman, Yurii I.

AU - Shorstkaya, Yuliya V.

AU - Mishakov, Ilya V.

AU - Plyusnin, Pavel E.

AU - Shubin, Yury V.

AU - Korneev, Denis V.

AU - Stoyanovskii, Vladimir O.

AU - Vedyagin, Aleksey A.

PY - 2017/9/15

Y1 - 2017/9/15

N2 - The alloyed Ni-Pd system with Pd content of 3 wt.% was prepared by coprecipitation method followed by reduction in hydrogen atmosphere at 800 °C. The formation of single-phase solid solution with unit cell parameter a = 3.532(1) Å (determined by (331) reflex at 2θ ≈ 145°) corresponding to NiPd alloy with weight ratio 97:3 was confirmed by XRD analysis. Kinetic studies on catalytic conversion of 1,2-dichloroethane (DCE) over NiPd alloy into carbon nanomaterial (CNM) were performed in a flow reactor equipped with McBain balances in a temperature range of 580–700 °C. It was shown that interaction of DCE with NiPd system results in a fast disintegration of pristine alloy with formation of submicron (0.2-0.9 μm) particles, which efficiently catalyze the growth of segmented carbon filaments. According to Raman spectroscopy and transmission electron microscopy data, hydrogen concentration in reaction mixture strongly affects the structural features and density of segmented filaments. The average values of inter-segmental distance calculated from TEM micrographs of carbon filaments were found to be 96, 46, 16 nm for hydrogen concentration of 23, 36 and 47 vol.%, respectively. Strongly chemisorbed chlorine species were suggested to be responsible for the cyclic perturbations in carbon transfer and deposition. Obtained carbon nanomaterials were characterized with comparatively high specific surface area (300–400 m2/g) and extremely low bulk density (<0.03 g/ml).

AB - The alloyed Ni-Pd system with Pd content of 3 wt.% was prepared by coprecipitation method followed by reduction in hydrogen atmosphere at 800 °C. The formation of single-phase solid solution with unit cell parameter a = 3.532(1) Å (determined by (331) reflex at 2θ ≈ 145°) corresponding to NiPd alloy with weight ratio 97:3 was confirmed by XRD analysis. Kinetic studies on catalytic conversion of 1,2-dichloroethane (DCE) over NiPd alloy into carbon nanomaterial (CNM) were performed in a flow reactor equipped with McBain balances in a temperature range of 580–700 °C. It was shown that interaction of DCE with NiPd system results in a fast disintegration of pristine alloy with formation of submicron (0.2-0.9 μm) particles, which efficiently catalyze the growth of segmented carbon filaments. According to Raman spectroscopy and transmission electron microscopy data, hydrogen concentration in reaction mixture strongly affects the structural features and density of segmented filaments. The average values of inter-segmental distance calculated from TEM micrographs of carbon filaments were found to be 96, 46, 16 nm for hydrogen concentration of 23, 36 and 47 vol.%, respectively. Strongly chemisorbed chlorine species were suggested to be responsible for the cyclic perturbations in carbon transfer and deposition. Obtained carbon nanomaterials were characterized with comparatively high specific surface area (300–400 m2/g) and extremely low bulk density (<0.03 g/ml).

KW - 1,2-dichloroethane

KW - Carbon nanomaterial

KW - Catalytic decomposition

KW - Metal dusting

KW - Ni-Pd alloy

KW - Segmented filaments

KW - OXIDATION

KW - PALLADIUM

KW - TRICHLOROETHYLENE

KW - PARTICLES

KW - DECOMPOSITION

KW - GRAPHITE

KW - CHLOROBENZENE

KW - HYDRODECHLORINATION

KW - CHLORINATED HYDROCARBONS

KW - SUPPORTED PD

UR - http://www.scopus.com/inward/record.url?scp=85006817520&partnerID=8YFLogxK

U2 - 10.1016/j.cattod.2016.11.020

DO - 10.1016/j.cattod.2016.11.020

M3 - Article

AN - SCOPUS:85006817520

VL - 293-294

SP - 23

EP - 32

JO - Catalysis Today

JF - Catalysis Today

SN - 0920-5861

ER -