Anchoring IrPdAu Nanoparticles on NH₂-SBA-15 for Fast Hydrogen Production from Formic Acid at Room Temperature

Abstract

Hydrogen (H 2 ), 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 2 ) reduction, has a great potential to serve as a prospective H 2 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 2 (NH 2 -SBA-15) and used as a highly active and selective catalyst for fast H 2 production from FA. The as-synthesized IrPdAu/NH 2 -SBA-15 possesses superior catalytic activity and 100% H 2 selectivity with initial turnover frequency values of 6316 h −1 with the additive of sodium formate (SF) and 4737 h −1 even without SF at 298 K, comparable to the most effective heterogeneous catalysts ever published. The excellent performance of IrPdAu/NH 2 -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 2 ) alkaline groups grafted on SBA-15, which is beneficial to boost the split of the O−H bond of FA.

Ultrafine PdAg alloy nanoparticles anchored on NH2-functionalized 2D/2D TiO2 nanosheet/rGO composite as efficient and reusable catalyst for hydrogen release from additive-free formic acid at room temperature

“…According to our results and previous reports [55][56][57], a probable reaction pathway is proposed for hydrogen production from FA catalyzed by Pd 8 Ag 1 /NH 2 -TNS-rGO (Scheme 1). Generally, the FA molecule is close to the active sites of Pd 8 Ag 1 /NH 2 -TNS-rGO and adsorb on the surface of Pd 8 Ag 1 alloy nanoparticles.…”

The enhanced role of surface amination on the catalytic performance of polyacrylonitrile supported palladium nanoparticles in hydrogen generation from formic acid

“…Besides, the bridging structure of amidinate, which formed by the reaction between the amino groups in EDA and the cyano group in PAN, may also form additional coordination interaction with the introduced Pd species, thus playing positive role in the formation of ultra‐small Pd NPs with high stability. Furthermore, the basic features of the amidinate and amino groups may also be beneficial for the deprotonation of FA, which is believed a critical step for the dehydrogenation of FA 30,31 . Based on these phenomenon and the related reports, 8,12,27 the catalytic mechanism for FA dehydrogenation over the Pd/EDA‐PAN catalyst could be proposed as follows: The basic groups like amino, cyano and amidinate can first interact with the reactant of FA, which is conducive to the deprotonation of FA.…”

Decomposition of Additive-Free Formic Acid Using a Pd/C Catalyst in Flow: Experimental and CFD Modelling Studies

“…Luo et al [19] dispersed ultrafine and electron-rich IrPdAu alloy nanoparticles with a size of 1.4 nm on amine-modified mesoporous SiO 2 (NH 2 -SBA-15) and applied it as a highly active and selective catalyst for fast H 2 production from formic acid. The synthesized IrPdAu/NH 2 -SBA-15 holds exceptional catalytic activity and 100% selectivity towards H 2 with an initial TOF of 6316 h −1 with the additive of sodium formate (SF) and 4737 h −1 devoid of SF at 298 K, as opposed to most effective heterogeneous catalysts.…”