Catalytic pyrolysis of biomass with Ni/Fe-CaO-based catalysts for hydrogen-rich gas: DFT and experimental study

被引：48

作者：

Wang, Jingwei ^{[1
]}

Zhao, Baofeng ^{[1
]}

Liu, Suxiang ^{[1
]}

Zhu, Di ^{[1
]}

Huang, Fayuan ^{[2
]}

Yang, Huajian ^{[1
]}

Guan, Haibin ^{[1
]}

Song, Angang ^{[1
]}

Xu, Dan ^{[1
]}

Sun, Laizhi ^{[1
]}

Xie, Hongzhang ^{[1
]}

Wei, Wei ^{[1
]}

Zhang, Wei ^{[3
]}

Pederson, Thomas Helmer ^{[4
]}

机构：

[1] Qilu Univ Technol, Energy Res Inst, Shandong Acad Sci, Key Lab Biomass Gasificat Technol Shandong Prov, Jinan 250014, Peoples R China

[2] Aobo Particle Sci & Technol Res Inst, Nanchang 330000, Jiangxi, Peoples R China

[3] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China

[4] Aalborg Univ, Dept Energy Technol, DK-9000 Aalborg, Denmark

来源：

ENERGY CONVERSION AND MANAGEMENT | 2022年 / 254卷

基金：

国家重点研发计划;

关键词：

Biomass; Ni-based catalysts; Pyrolysis mechanism; DFT; H(2 )production; SHIFT REACTION; TEMPERATURE; MECHANISM; CRACKING; TAR; GASIFICATION; CELLULOSE;

D O I：

10.1016/j.enconman.2022.115246

中图分类号：

O414.1 [热力学];

学科分类号：

摘要：

The H-2-rich gas produced by biomass pyrolysis with Ni-based catalysts were studied by DFT, thermodynamic simulation, and pyrolysis experiment. The complex reaction between volatiles of biomass pyrolysis was clarified through DFT calculation. The results proved that the E-a of key reactions for H-2 production on Ni-Fe/CaO surface were lower than that on NC, which facilitates to produce H-2. The order of the E-a of the rate determining step on Ni-Fe/CaO surface is toluene cracking reaction < water-carbon reaction < Boudouard reaction < methane steam reforming reaction < methane dry reforming reaction < water gas shift reaction, indicating water gas shift reaction is the key control reaction. When the temperature is 650 & DEG;C, Ni-Fe/CaO can effectively adsorb CO2 to break the thermodynamic equilibrium of the water gas shift reaction and promote the forward reaction to generate H-2. Thermodynamic simulation and pyrolysis experiments determined that 650 & DEG;C and Ni-Fe/CaO are the most suitable reaction condition for H-2 formation. Under this condition, the liquid yield of biomass pyrolysis decreased by 18.32% and the gas yield was increased by 26.27% compared to that of Ni /CaO. More importantly, the H2 yield was increased by 18.29% to 453.34 mL/g-biomass.

引用

页数：11