Phosphate‐Mediated Immobilization of High‐Performance AuPd Nanoparticles for Dehydrogenation of Formic Acid at Room Temperature

Abstract

Dehydrogenation of formic acid (FA) is a promising alternative to fossil fuels, to provide clean energy for the future energy economy. The synthesis of highly active catalysts for FA dehydrogenation at room temperature has attracted a lot of attention. Herein, for the first time, highly active aurum-palladium nano particles (AuPd NPs) immobilized on nitrogen (N)-doped porous carbon are fabricated through a phosphate-mediation approach. The N-doped carbon anchored with phosphate, which can be removed in alkaline solution during the reduction process of metal ions, shows an enhanced performance of absorbing and dispersion of both Au and Pd ions, which is a key to the synthesis of highly dispersed ultrafine AuPd NPs. The as-prepared catalyst (designated as Au 2 Pd 3 @(P)N-C) exhibits an extraordinarily high turnover frequency of 5400 h −1 and a 100% H 2 selectivity for FA dehydrogenation at 30 °C. This phosphate-mediation approach provides a new way to fabricate highly active metal NPs for catalytic application, pushing heterogeneous catalysts forward for practical usage in energy storage and conversion.

Hydrogen Production from Formic Acid Attained by Bimetallic Heterogeneous PdAg Catalytic Systems

“…In this sense, there is an increasing number of publications reporting on the investigation of catalytic systems able to catalyse the reaction while exploring the features of either support or metal active phase. Special mention should be made of those breakthroughs achieved Xu et al [29][30][31][32][33][34], and Bulushev et al [47][48][49][50][51][52][53][54][55][56][57].Most of the heterogeneous catalysts used are based on metal nanoparticles immobilised on supports of diverse nature (i.e. carbon materials, MOF, zeolites, resins, etc.)…”

Ambient sunlight-driven photothermal methanol dehydrogenation for syngas production with 32.9 % solar-to-hydrogen conversion efficiency

“…This result indicates that the CH 3 OH decomposition is kinetically more favorable on Pt s -CeO 2 . The high adsorption ability and low energy barrier lead to the high activity of Pt s -CeO 2 for methanol dehydrogenation ( Lin et al., 2017 ; Wang et al., 2019 ).…”

Nanopore‐Supported Metal Nanocatalysts for Efficient Hydrogen Generation from Liquid‐Phase Chemical Hydrogen Storage Materials

“…[ 15c,83 ] Significantly, the heteroatoms, such as N, P, and metal species could be doped simultaneously on porous carbon supports after thermal treatment in an inert gas atmosphere, which could improve the dispersibility of metal NPs and enhance the catalytic performance. [ 15b,56–60,84 ] Recently, Xu and co‐workers prepared a hierarchically nitrogen‐doped porous carbon from the carbonization of an Al‐based MOF (Al‐MIL‐101‐NH 2 ) that was built up from 2‐aminoterephthalic acid ligands and Al clusters, followed by activation under ultrasonication in the KOH solution. [ 56 ] The Brunauer–Emmett–Teller (BET) specific surface area increased gradually with the increase of carbonization temperatures from 600 to 900 °C but decreased at 1000 °C.…”

“…Among the MOF materials, the zeolitic imidazole‐based ZIF‐8 was one of the most commonly used sacrificial templates for the fabrication of nitrogen‐doped porous carbon materials, due to the simple synthetic procedure and relatively low synthetic cost. [ 57–59,84b ] For example, bimetallic Pd–Ag NPs with various molar ratios of Ag/Pd were immobilized on the ZIF‐8‐derived nitrogen‐doped porous carbon via a wet chemical reduction method. [ 57 ] The optimized Ag 1 Pd 4 @ZIF8‐C exhibited high catalytic activity of the FA dehydrogenation with a TOF of 936 h −1 at 80 °C.…”