Facile construction of a highly dispersed PdCo nanocatalyst supported on NH2-UiO-66-derived N/O co-doped carbon for hydrogen evolution from formic acid. (June 2022)

• Record Type: Journal Article
• Authors: Deng, M.; Ma, J.; Yang, C.; Cao, T.; Yao, M.; Liu, F.; Chen, H.; Wang, X.
• Is Part Of: Materials today chemistry. Volume 24(2022)
• Publication Date: 2022-06
• Subjects: MOF-Mediated synthesis -- PdCo nanoparticles -- N/O co-doped -- Formic acid -- Dehydrogenation; Chemistry -- Periodicals; Materials -- Research -- Periodicals; Materials science -- Periodicals; Chemistry; Materials -- Research; Electronic journals; Periodicals; 660.282
• DOI: 10.1016/j.mtchem.2022.101001
• Languages: English
• ISSNs: 2468-5194

Abstract

Abstract: Rational design of catalysts with a high activity and low cost is crucial but still challenging for formic acid (FA) as a hydrogen storage material. Herein, PdCo-bimetallic particles were evenly dispersed on N/O co-doped porous carbon, which is achieved through the one-step pyrolysis NH2 -UiO-66 strategy. The evaluation test demonstrated that the prepared catalysts had high activity and selectivity for the decomposition of FA. The turnover frequency (TOF) of FA decomposition catalyzed by Pd4 Co1 /CN – O -800 at 30 °C was 2425 h −1 (TOF at 50 °C was 4587 h −1 ) and the selectivity of hydrogen was 100%. Structural characterizations combined with detailed theoretical calculation results reveal that the constructed N/O co-doped system endows the bimetallic catalyst with abundant catalytic sites and strong metal-support interaction, thereby achieving remarkable catalytic performance. The results provide ideas for the design of efficient FA dehydrogenation catalysts and offer theoretical guidance to N/O co-doped carbon materials. Graphical abstract: In order to prepare high performance catalyst for formic acid dehydrogenation, Pd4 Co1 cluster deposit on a N/O co-doped carbons, which prepared by carbonization of N/O-containing NH2 -UiO-66. The synergistic effect of N/O affects the active sites, which makes the prepared catalyst have excellent catalytic performance. The Pd4 Co1 /CN – O -800 have the best catalytic activity and 100% hydrogen selectivity. Image 1 Highlights: N/O co-doped carbon derived from NH2 -UiO-66 were prepared by one-step method. Highly dispersed PdCo nanoparticles were dispersed on N/O co-doped carbon. The synergistic effect of N and O affects the properties of PdCo nanoparticles. O-species regulate the PdCo nanoparticles indirectly by interacting with carbon. The as-prepared catalyst has high performance in dehydrogenation of formic acid.