TY - JOUR
T1 - Hydrogenolysis of lignin to phenolic monomers over Ru based catalysts with different metal-support interactions
T2 - Effect of partial hydrogenation of C(sp2)-O/C
AU - Wu, Yishuang
AU - Lin, Zixiang
AU - Zhu, Xun
AU - Hu, Xun
AU - Gholizadeh, Mortaza
AU - Sun, Hongqi
AU - Huang, Yong
AU - Zhang, Shu
AU - Zhang, Hong
N1 - Funding Information:
This work was financially supported by the National Natural Science Foundation of China (Grant 51876093); an internationally collaborative project (BRICS2019-040) under BRICS STI Framework Programme with government funding organizations of Brazil CNPq (402849/2019-1), Russia RFBR (19-58-80016), India DST(CRG/2018/004610, DST/TDT/TDP-011/2017), China MOST (2018YFE0183600), and South Africa NRF (BRIC190321424123); the Talent Project from the “Double-Entrepreneurial Plan” in Jiangsu Province; and the Startup Fund for Scientific Research of Nanjing Forestry University (Grant GXL2018033). The BDE calculations were performed on the Linux cluster in the Key Laboratory of Environmental Theoretical Chemistry of Ministry of Education at South China Normal University.
Funding Information:
This work was financially supported by the National Natural Science Foundation of China (Grant 51876093 ); an internationally collaborative project (BRICS2019-040) under BRICS STI Framework Programme with government funding organizations of Brazil CNPq ( 402849/2019-1 ), Russia RFBR ( 19-58-80016 ), India DST ( CRG/2018/004610 , DST/TDT/TDP-011/2017 ), China MOST ( 2018YFE0183600 ), and South Africa NRF ( BRIC190321424123 ); the Talent Project from the “Double-Entrepreneurial Plan” in Jiangsu Province; and the Startup Fund for Scientific Research of Nanjing Forestry University (Grant GXL2018033 ). The BDE calculations were performed on the Linux cluster in the Key Laboratory of Environmental Theoretical Chemistry of Ministry of Education at South China Normal University .
Publisher Copyright:
© 2021 Elsevier Ltd
PY - 2021/10/15
Y1 - 2021/10/15
N2 - Catalytic hydrogenolysis of lignin to phenolic monomers has received a lot of attention, but it is still a challenge because the cleavage of the strong C(sp2)-O/C bonds between structural units is usually under harsh conditions, resulting in the presence of the competing reaction of hydrogenation. Herein, hydrogenolysis of an herbaceous lignin into phenolic monomers was performed over Ru supported on various (non)-functionalized graphitized carbon nanotubes (CNT, CNT-OH, CNT-COOH, and CNT-NH2), which were featured by different hydrogenation performances originally from the diverse metal-support interactions. Among the investigated supports, CNT-NH2 enables the formation of the finest Ru nanoparticles with an average size of 1.86 nm, leading to the highest yield of phenolic monomers from lignin hydrogenolysis. The best hydrogenolysis performance of Ru@CNT-NH2 was mainly from the partial hydrogenation of C(sp2)-O/C bonds to C(sp3)-O/C bonds in lignin, thus reducing their bond dissociation energy (BDE). The intimacy between hydrogenolysis and hydrogenation was further proved by depolymerization of a lignin β-O-4 model compound.
AB - Catalytic hydrogenolysis of lignin to phenolic monomers has received a lot of attention, but it is still a challenge because the cleavage of the strong C(sp2)-O/C bonds between structural units is usually under harsh conditions, resulting in the presence of the competing reaction of hydrogenation. Herein, hydrogenolysis of an herbaceous lignin into phenolic monomers was performed over Ru supported on various (non)-functionalized graphitized carbon nanotubes (CNT, CNT-OH, CNT-COOH, and CNT-NH2), which were featured by different hydrogenation performances originally from the diverse metal-support interactions. Among the investigated supports, CNT-NH2 enables the formation of the finest Ru nanoparticles with an average size of 1.86 nm, leading to the highest yield of phenolic monomers from lignin hydrogenolysis. The best hydrogenolysis performance of Ru@CNT-NH2 was mainly from the partial hydrogenation of C(sp2)-O/C bonds to C(sp3)-O/C bonds in lignin, thus reducing their bond dissociation energy (BDE). The intimacy between hydrogenolysis and hydrogenation was further proved by depolymerization of a lignin β-O-4 model compound.
KW - Hydrogenation
KW - Hydrogenolysis
KW - Lignin
KW - Phenolic monomer
UR - http://www.scopus.com/inward/record.url?scp=85107673135&partnerID=8YFLogxK
U2 - 10.1016/j.fuel.2021.121184
DO - 10.1016/j.fuel.2021.121184
M3 - Article
AN - SCOPUS:85107673135
SN - 0016-2361
VL - 302
JO - Fuel
JF - Fuel
M1 - 121184
ER -