School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832003, China.
College of Chemistry and Chemical Engineering, Yantai University, Yantai 264010, China.
Molecules. 2023 Jan 18;28(3):956. doi: 10.3390/molecules28030956.
The poor stability of carbon materials doped with nitrogen limited their development in acetylene hydrochlorination. Therefore, investigating the deactivation reasons of carbon catalysts and researching regeneration methods became the research focus. Herein, carbon-nitrogen materials were synthesized by one-step pyrolysis, which using biomass materials with high nitrogen content, the synthesized material was used in an acetylene hydrochlorination reaction. The acetylene conversion rate of D-GH-800 catalyst was up to 99%, but the catalytic activity decreased by 30% after 60 h reaction. Thermogravimetric analysis results showed that the coke content was 5.87%, resulting in catalyst deactivation. Temperature-programmed desorption verified that the deactivation was due to the strong adsorption and difficult desorption of acetylene by the D-GH-800 catalyst, resulting in the accumulation of acetylene on the catalyst surface to form carbon polymers and leading to the pore blockage phenomenon. Furthermore, based on the catalyst deactivation by carbon accumulation, we proposed a new idea of regeneration by ZnCl activation to eliminate carbon deposition in the pores of the deactivated catalyst. As a result, the activity of D-GH-800 was recovered, and lifetime was also extended. Our strategy illustrated the mechanism of carbon deposition, and the recoverability of the catalyst has promising applications.
氮掺杂碳材料的稳定性较差,限制了其在乙炔氯化反应中的发展。因此,研究碳催化剂的失活原因和研究再生方法成为研究的重点。本文采用一步热解法合成了碳氮材料,该方法使用了含氮量高的生物质材料,所合成的材料用于乙炔氯化反应。D-GH-800 催化剂的乙炔转化率高达 99%,但反应 60 h 后催化活性下降了 30%。热重分析结果表明,焦炭含量为 5.87%,导致催化剂失活。程序升温脱附实验验证了 D-GH-800 催化剂失活是由于乙炔的强吸附和难脱附,导致乙炔在催化剂表面积累形成碳聚合物,从而导致孔堵塞现象。此外,基于催化剂因积碳而失活的情况,我们提出了一种通过 ZnCl 活化进行再生的新方法,以消除失活催化剂孔内的积碳。结果表明,D-GH-800 的活性得到恢复,寿命也得到延长。我们的策略说明了积碳的机理,催化剂的可恢复性具有广阔的应用前景。