TY - JOUR
T1 - Structural evolution of ZIF-67-derived catalysts for furfural hydrogenation
AU - Lee, Jun Gyeong
AU - Yoon, Sinmyung
AU - Yang, Euiseob
AU - Lee, Jae Hwa
AU - Song, Kyung
AU - Moon, Hoi Ri
AU - An, Kwangjin
N1 - Publisher Copyright:
© 2020 Elsevier Inc.
PY - 2020/12
Y1 - 2020/12
N2 - Zeolitic imidazolate framework-67 (ZIF-67) can be converted to metallic Co nanoparticles supported on N-doped carbon (Co/NC) through reduction. However, its unique properties, including extremely high surface area, isoreticular pore structure, and regular metal–organic network, disappear after high-temperature (>500 °C) reduction. Aggregated CoOx particles reduce the number of surface-active sites, resulting in poor catalytic activity. If the original ZIF-67 structure is maintained after the high-temperature reduction, promoting the uniform distribution of active sites in the porous carbon, the catalytic performance can be further improved. Herein, the correlation between the catalytic furfural hydrogenation performance, Co/NC morphology, and oxidation state of Co was investigated as a function of the H2 reduction temperature and time. The reduction of ZIF-67 at 400 °C for 6 h yields a highly dispersed Co/NC catalyst, while preserving the overall morphology. The resulting Co/NC-400-6 catalyst exhibits the highest activity, promoting high selectivity toward 2-methylfuran. The product selectivity can be further altered by incorporating Cu into ZIF-67 to produce furfuryl alcohol. With proper H2 treatment to minimize the damage to the intrinsic surface area and pore structure, metal–organic frameworks can be utilized as high-performance heterogeneous catalysts by maximizing the distribution of active sites.
AB - Zeolitic imidazolate framework-67 (ZIF-67) can be converted to metallic Co nanoparticles supported on N-doped carbon (Co/NC) through reduction. However, its unique properties, including extremely high surface area, isoreticular pore structure, and regular metal–organic network, disappear after high-temperature (>500 °C) reduction. Aggregated CoOx particles reduce the number of surface-active sites, resulting in poor catalytic activity. If the original ZIF-67 structure is maintained after the high-temperature reduction, promoting the uniform distribution of active sites in the porous carbon, the catalytic performance can be further improved. Herein, the correlation between the catalytic furfural hydrogenation performance, Co/NC morphology, and oxidation state of Co was investigated as a function of the H2 reduction temperature and time. The reduction of ZIF-67 at 400 °C for 6 h yields a highly dispersed Co/NC catalyst, while preserving the overall morphology. The resulting Co/NC-400-6 catalyst exhibits the highest activity, promoting high selectivity toward 2-methylfuran. The product selectivity can be further altered by incorporating Cu into ZIF-67 to produce furfuryl alcohol. With proper H2 treatment to minimize the damage to the intrinsic surface area and pore structure, metal–organic frameworks can be utilized as high-performance heterogeneous catalysts by maximizing the distribution of active sites.
KW - Catalyst
KW - Furfural hydrogenation
KW - In situ characterization
KW - Metal-organic framework (MOF)
KW - Zeolitic imidazolate framework-67 (ZIF-67)
UR - http://www.scopus.com/inward/record.url?scp=85096176242&partnerID=8YFLogxK
U2 - 10.1016/j.jcat.2020.10.014
DO - 10.1016/j.jcat.2020.10.014
M3 - Article
AN - SCOPUS:85096176242
SN - 0021-9517
VL - 392
SP - 302
EP - 312
JO - Journal of Catalysis
JF - Journal of Catalysis
ER -