Li Xueqin, Wang Zhiwei, Zhang Yanpeng, Zhang Wenkai, Zhang Hongxun, Liu Peng, Lei Tingzhou
School of Environmental Engineering, Henan University of Technology, Zhengzhou, Henan, 450001, China; Institute for Carbon Neutrality, Henan University of Technology, Zhengzhou, Henan, 450001, China.
School of Environmental Engineering, Henan University of Technology, Zhengzhou, Henan, 450001, China; Institute for Carbon Neutrality, Henan University of Technology, Zhengzhou, Henan, 450001, China.
J Environ Manage. 2025 Aug;389:126016. doi: 10.1016/j.jenvman.2025.126016. Epub 2025 Jun 2.
This paper studied the hydrogen-rich gas production from catalytic pyrolysis of biomass tar using catalysts derived from aluminum dross (AD) combined with HZSM-5 molecular sieve co-supported Ni-Fe in a two-stage fixed-bed reactor. It revealed that the carrier characteristics played an important role in determining the Ni and Fe species form, textural properties, and catalytic abilities of the resulting catalysts. The surface properties and pore structure of aluminum dross activated by 3 mol/L HSO (ASA) are improved. Especially, the hydrogen-rich gas production with the highest toluene conversion (91.96 %), highest gaseous efficiency (70.78 wt%), gas (H, CH, CO) yield was 110.5 mL/g, H ratio was 39.55 vol%, and the lowest solid yield (0.09 %) and carbon deposition (7.14 mg/g) by the assisted-CO at the reforming temperature of 800 °C with the catalyst amount of 16 %. CO conversion of 84.37 % by catalytic pyrolysis of toluene under the CO-assisted ASA combined with HZSM-5 co-supported Ni-Fe (Ni-Fe/ASA@HZSM-5) catalyst condition. The synergy factor of ASA and HZSM-5 molecular sieve as co-carriers on H and CO yield is 1.30 and 1.70, playing a dual role in improving the yields of H and CO, and realizes the coordinated regulation of catalytic action and thermal conversion action. Therefore, the Ni-Fe/ASA@HZSM-5 catalyst has good catalytic activity and stability, which realizes the recovery and utilization of waste resources, reduces the preparation cost of catalysts and provides a new idea for the preparation of catalysts used to catalyze cracking/reforming of biomass tar to produce hydrogen-rich gas.
本文研究了在两段固定床反应器中，使用由铝灰（AD）与HZSM-5分子筛共负载Ni-Fe衍生的催化剂，对生物质焦油进行催化热解制富氢气体。结果表明，载体特性在决定所得催化剂的Ni和Fe物种形态、织构性质及催化能力方面起着重要作用。经3 mol/L H₂SO₄活化的铝灰（ASA）的表面性质和孔结构得到改善。特别是，在800℃的重整温度、16%的催化剂量下，通过CO辅助，甲苯转化率最高（91.96%），气态效率最高（70.78 wt%），气体（H₂、CH₄、CO）产率为110.5 mL/g，H₂比例为39.55 vol%，固体产率最低（0.09%），积碳量最低（7.14 mg/g）。在CO辅助的ASA与HZSM-5共负载Ni-Fe（Ni-Fe/ASA@HZSM-5）催化剂条件下，甲苯催化热解的CO转化率为84.37%。ASA和HZSM-5分子筛作为共载体对H₂和CO产率的协同因子分别为1.30和1.70，在提高H₂和CO产率方面发挥双重作用，实现了催化作用和热转化作用的协同调控。因此，Ni-Fe/ASA@HZSM-5催化剂具有良好的催化活性和稳定性，实现了废弃物资源的回收利用，降低了催化剂的制备成本，为制备用于催化生物质焦油裂解/重整制富氢气体的催化剂提供了新思路。
