Sanjaya Ari Susandy, Hakmi Yahia, Sanhoob Mohammed A, Nasser Galal, Rinaldi Ali, Muraza Oki, Mohamed Assem T, Benamor Abdelbaki, Khaled Mazen, Salih Kifah S M, Al-Hajri Rashid, Wibowo Arief C
Department of Chemical Engineering, Mulawarman University, Samarinda, East Kalimantan 75119, Indonesia.
Department of Chemistry, King Fahd University of Petroleum and Minerals, Dhahran 31261, Saudi Arabia.
ACS Omega. 2025 Apr 18;10(16):16102-16113. doi: 10.1021/acsomega.4c09539. eCollection 2025 Apr 29.
Dry reforming of methane (DRM) using a heterogeneous catalyst presents one of the CO mitigation pathways to address global warming and climate change challenges. Such a suitable DRM catalyst with optimum activity and stability is still under intense research. We herein present a facile, slightly modified version of the conventional wet impregnation method to synthesize a NiO-faujasite nanocatalyst for DRM with the help of aniline, judiciously chosen based on the hard-soft acid-base (HSAB) principle. The resulting catalyst was characterized by the N adsorption isotherm, PXRD, SEM/TEM, XPS, Si solid-state NMR, H-TPR, NH-TPD, and DRM reaction, and its results were compared with those without aniline assistance. A smaller NiO nanoparticle with better dispersion was observed for our aniline-assisted sample resulting in a significant increase in activity (peaking at 86% CH conversion with a H/CO ratio of 0.93) and stability for a 12 h time on stream. We hope that this work would pave the way to utilize the HSAB principle to synthesize more nanocatalysts with optimum overall performance.
使用多相催化剂进行甲烷干重整(DRM)是缓解二氧化碳排放以应对全球变暖和气候变化挑战的途径之一。目前仍在深入研究具有最佳活性和稳定性的合适DRM催化剂。在此,我们提出一种简便的、对传统湿浸渍法稍作改进的方法,借助基于软硬酸碱(HSAB)原理精心挑选的苯胺,合成用于DRM的NiO-八面沸石纳米催化剂。通过N吸附等温线、粉末X射线衍射(PXRD)、扫描电子显微镜/透射电子显微镜(SEM/TEM)、X射线光电子能谱(XPS)、硅固态核磁共振(Si solid-state NMR)、氢气程序升温还原(H-TPR)、氨气程序升温脱附(NH-TPD)以及DRM反应对所得催化剂进行表征,并将其结果与无苯胺辅助的情况进行比较。我们发现,苯胺辅助样品中的NiO纳米颗粒更小且分散性更好,从而使活性显著提高(CH转化率峰值为86%,H/CO比为0.93),并且在12小时的连续运行中具有稳定性。我们希望这项工作将为利用HSAB原理合成更多具有最佳综合性能的纳米催化剂铺平道路。