Luo Yixing, Yang Qifeng, Nie Wendan, Yao Qilu, Zhang Zhujun, Lu Zhang-Hui
Institute of Advanced Materials (IAM), College of Chemistry and Chemical Engineering , Jiangxi Normal University , Nanchang 330022 , China.
ACS Appl Mater Interfaces. 2020 Feb 19;12(7):8082-8090. doi: 10.1021/acsami.9b16981. Epub 2020 Feb 6.
Hydrogen (H), a regenerable and promising energy carrier, acts as an essential role in the construction of a sustainable energy system. Formic acid (HCOOH, FA), a natural biological metabolic products and also accessible through carbon dioxide (CO) reduction, has a great potential to serve as a prospective H supplier for the fuel cell. Herein, ultrafine and electron-rich IrPdAu alloy nanoparticles with a size of 1.4 nm are highly dispersed on amine-modified mesoporous SiO (NH-SBA-15) and used as a highly active and selective catalyst for fast H production from FA. The as-synthesized IrPdAu/NH-SBA-15 possesses superior catalytic activity and 100% H selectivity with initial turnover frequency values of 6316 h with the additive of sodium formate (SF) and 4737 h even without SF at 298 K, comparable to the most effective heterogeneous catalysts ever published. The excellent performance of IrPdAu/NH-SBA-15 was not only ascribed to the combination of the electronic synergistic effect of trimetallic alloys and the strong metal-support interaction effect but also attributed to the amine (-NH) alkaline groups grafted on SBA-15, which is beneficial to boost the split of the O-H bond of FA.
氢(H)作为一种可再生且前景广阔的能量载体,在可持续能源系统的构建中起着至关重要的作用。甲酸(HCOOH,FA)是一种天然的生物代谢产物,也可通过二氧化碳(CO)还原获得,具有作为燃料电池潜在氢供应源的巨大潜力。在此,尺寸为1.4 nm的超细且富电子的IrPdAu合金纳米颗粒高度分散在胺改性的介孔SiO(NH-SBA-15)上,并用作从FA快速制氢的高活性和选择性催化剂。所合成的IrPdAu/NH-SBA-15具有优异的催化活性和100%的氢选择性,在添加甲酸钠(SF)时初始周转频率值为6316 h,在298 K下即使不添加SF时也为4737 h,与已发表的最有效的多相催化剂相当。IrPdAu/NH-SBA-15的优异性能不仅归因于三金属合金的电子协同效应和强金属-载体相互作用效应的结合,还归因于接枝在SBA-15上的胺基(-NH)碱性基团,这有利于促进FA中O-H键的断裂。