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室温合成双功能 NH-N-rGO 上锚定和升级超细 NiPd 用于选择性甲酸脱氢的低成本高效催化剂。

Anchoring and Upgrading Ultrafine NiPd on Room-Temperature-Synthesized Bifunctional NH -N-rGO toward Low-Cost and Highly Efficient Catalysts for Selective Formic Acid Dehydrogenation.

机构信息

Key Laboratory of Automobile Materials, Ministry of Education, Department of Materials Science and Engineering, Jilin University, Changchun, 130022, China.

出版信息

Adv Mater. 2018 Mar;30(12):e1703038. doi: 10.1002/adma.201703038. Epub 2018 Feb 7.

Abstract

Hydrogen is widely considered to be a sustainable and clean energy alternative to the use of fossil fuels in the future. Its high hydrogen content, nontoxicity, and liquid state at room temperature make formic acid a promising hydrogen carrier. Designing highly efficient and low-cost heterogeneous catalysts is a major challenge for realizing the practical application of formic acid in the fuel-cell-based hydrogen economy. Herein, a simple but effective and rapid strategy is proposed, which demonstrates the synthesis of NiPd bimetallic ultrafine particles (UPs) supported on NH -functionalized and N-doped reduced graphene oxide (NH -N-rGO) at room temperature. The introduction of the NH N group to rGO is the key reason for the formation of the ultrafine and well-dispersed Ni Pd UPs (1.8 nm) with relatively large surface area and more active sites. Surprisingly, the as-prepared low-cost NiPd/NH -N-rGO dsiplays excellent hydrophilicity, 100% H selectivity, 100% conversion, and remarkable catalytic activity (up to 954.3 mol H (mol catalyst) h ) for FA decomposition at room temperature even with no additive, which is much higher than that of the best catalysts so far reported.

摘要

氢气被广泛认为是未来替代化石燃料的可持续清洁能源。甲酸因其高含氢量、无毒和室温下的液态形式,成为一种很有前途的储氢载体。设计高效、低成本的多相催化剂是实现甲酸在基于燃料电池的氢能经济中实际应用的主要挑战。在此,提出了一种简单但有效的快速策略,即在室温下合成负载在 NH 功能化和 N 掺杂还原氧化石墨烯(NH-N-rGO)上的 NiPd 双金属超细颗粒(UPs)。向 rGO 中引入 NH N 基团是形成具有较大表面积和更多活性位的超细和分散良好的 NiPd UPs(1.8nm)的关键原因。令人惊讶的是,所制备的低成本 NiPd/NH-N-rGO 在室温下对 FA 分解表现出优异的亲水性、100%H 选择性、100%转化率和显著的催化活性(高达 954.3mol H(mol 催化剂) h ),甚至在没有添加剂的情况下,其活性远高于迄今为止报道的最佳催化剂。

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