Xu Haiyang, Shen Zhangfeng, Zhang Siqian, Chen Gang, Pan Hu, Ge Zhigang, Zheng Zheng, Wang Yanqin, Wang Yangang, Li Xi
College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing, Zhejiang 314001, China; Department of Environmental Science and Engineering, Fudan University, Shanghai 200433, China.
College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing, Zhejiang 314001, China.
J Colloid Interface Sci. 2021 Oct;599:650-660. doi: 10.1016/j.jcis.2021.04.112. Epub 2021 Apr 30.
Steam reforming is an effective measure for biomass tar elimination as well as H-rich syngas (H + CO) production. However, the granular or powdery Ni-based catalysts are prone to deactivation, which is caused by inappropriate mass transfer and clogging of catalyst bed. Herein, monolithic wood carbon (WC) with low-tortuosity microchannels is armed with a carbon-coated mesoporous nickel-silica nanocomposite (Ni-SiO@C) layer via an evaporation-induced self-assembly and calcination procedure for toluene (tar model compound) steam reforming. The quality of the Ni-SiO@C layer growing on the surface of WC microchannel is affected by the molar ratios of Si/Ni feed. A uniform thin-layer coverage is obtained on the Ni-15SiO@C/WC (Si/Ni = 15) catalyst, where highly dispersed Ni nanoparticles (average size of 6.6 nm) with appropriate metal-support interaction and remarkable mechanical strength are achieved. The mass transfer, coke resistance, and hydrothermal stability of the Ni-15SiO@C/WC catalyst were significantly improved by the multilevel structure assembled from the WC microchannels and the secondary ordered SiO mesopores. A stable toluene conversion over 97% with an H yield of 135 μmol/min was obtained at 600 °C on the Ni-15SiO@C/WC catalyst. This work opens a new window for facilely constructing high-performance wood carbon-based monolithic tar reforming catalyst.
蒸汽重整是消除生物质焦油以及生产富含氢气的合成气（H₂ + CO）的有效措施。然而，颗粒状或粉末状的镍基催化剂容易失活，这是由传质不当和催化剂床堵塞引起的。在此，具有低曲折度微通道的整体式木碳（WC）通过蒸发诱导自组装和煅烧程序，负载了一层碳包覆的介孔镍 - 二氧化硅纳米复合材料（Ni - SiO₂@C）层，用于甲苯（焦油模型化合物）蒸汽重整。在WC微通道表面生长的Ni - SiO₂@C层的质量受硅/镍进料摩尔比的影响。在Ni - 15SiO₂@C/WC（Si/Ni = 15）催化剂上获得了均匀的薄层覆盖，其中实现了具有适当金属 - 载体相互作用和显著机械强度的高度分散的镍纳米颗粒（平均尺寸为6.6 nm）。由WC微通道和二级有序SiO₂介孔组装而成的多级结构显著提高了Ni - 15SiO₂@C/WC催化剂的传质、抗焦性和水热稳定性。在Ni - 15SiO₂@C/WC催化剂上，600℃时甲苯转化率稳定超过97%，氢气产率为135 μmol/min。这项工作为轻松构建高性能木碳基整体式焦油重整催化剂打开了一扇新窗口。
