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胺功能化介孔硅限域的铬修饰钯纳米粒子用于甲酸的快速脱氢。

Chromic hydroxide-decorated palladium nanoparticles confined by amine-functionalized mesoporous silica for rapid dehydrogenation of formic acid.

机构信息

National Engineering Research Center for Carbohydrate Synthesis, Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, Key Laboratory of Energy Catalysis and Conversion of Nanchang, College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, China.

Key Laboratory for Environment and Energy Catalysis of Jiangxi Province, College of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China.

出版信息

J Colloid Interface Sci. 2023 Jan 15;630(Pt A):879-887. doi: 10.1016/j.jcis.2022.10.048. Epub 2022 Oct 19.

Abstract

Formic acid (FA), one of the products of biomass conversion and CO reduction, has attracted much attention as a renewable liquid hydrogen carrier with a high hydrogen content (4.4 wt%). Searching for efficient catalysts to realize hydrogen evolution from FA are highly desired but challenging. Herein, ultrafine and mono-dispersed Pd-Cr(OH) nanoparticles (1.3 nm) loaded on amine-functionalized mesoporous silica (AFMS) have been prepared and applied as an effective catalyst for rapid hydrogen production from additive-free FA. The as-synthesized Pd-Cr(OH)/AFMS catalysts exhibited efficient catalytic activity and 100% hydrogen selectivity and conversion toward FA dehydrogenation reaction without additives, giving an initial TOF value of 3112 h at 323 K, which is comparable to most of the highly efficient heterogeneous catalysts reported so far under similar reaction conditions. This work provides a feasible idea for the design metal hydroxide-modified Pd-based efficient heterogeneous catalyst, which is expected to enhance the application of FA in fuel cells.

摘要

甲酸(FA)是生物质转化和 CO 还原的产物之一,作为一种具有高氢含量(4.4wt%)的可再生液体储氢载体,引起了广泛关注。寻找高效催化剂以实现 FA 中的氢释放是非常需要的,但具有挑战性。本文制备了负载在胺功能化介孔硅(AFMS)上的超细微和单分散的 Pd-Cr(OH)纳米颗粒(1.3nm),并将其用作无添加剂 FA 快速制氢的有效催化剂。所合成的 Pd-Cr(OH)/AFMS 催化剂在无添加剂的 FA 脱氢反应中表现出高效的催化活性和 100%的氢气选择性和转化率,在 323K 下的初始 TOF 值为 3112h,与迄今为止在类似反应条件下报道的大多数高效多相催化剂相当。这项工作为设计金属氢氧化物改性 Pd 基高效多相催化剂提供了一个可行的思路,有望促进 FA 在燃料电池中的应用。

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