Anchoring and Upgrading Ultrafine NiPd on Room‐Temperature‐Synthesized Bifunctional NH2‐N‐rGO toward Low‐Cost and Highly Efficient Catalysts for Selective Formic Acid Dehydrogenation
Anchoring and Upgrading Ultrafine NiPd on Room‐Temperature‐Synthesized Bifunctional NH2‐N‐rGO toward Low‐Cost and Highly Efficient Catalysts for Selective Formic Acid Dehydrogenation
复制标题
DOI：
10.1002/adma.201703038
复制
发表时间：
2018-03
影响因子：
29.4
通讯作者：
Jun-min Yan;Si‐Jia Li;Shasha Yi;Ba‐Ri Wulan;W. Zheng;Q. Jiang
中科院分区：
文献类型：
--
作者：
Jun-min Yan;Si‐Jia Li;Shasha Yi;Ba‐Ri Wulan;W. Zheng;Q. Jiang
氢被广泛认为是未来替代化石燃料的可持续和清洁能源。甲酸的氢含量高、无毒且在室温下呈液态，使其成为一种很有前景的氢载体。设计高效、低成本的多相催化剂是实现甲酸在燃料电池氢经济中实际应用的主要挑战。在此，提出了一种简单但有效且快速的策略，该策略演示了在室温下合成在NH2功能化和N掺杂的还原氧化石墨烯（NH2-N-rGO）上负载的NiPd双金属超细颗粒（UP）。在rGO中引入NH2N基团是形成超细且分散良好的Ni0.4Pd0.6 UPs（1.8 nm）、具有较大表面积和更多活性位点的关键原因。令人惊讶的是，所制备的低成本NiPd/NH2-N-rGO表现出优异的亲水性、100% H2选择性、100%转化率，即使在没有添加剂的情况下，在室温下对FA分解也具有显着的催化活性（高达954.3 mol H2（mol催化剂）−1 h−1），远高于迄今为止报道的最好的催化剂。
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 NH2‐functionalized and N‐doped reduced graphene oxide (NH2‐N‐rGO) at room temperature. The introduction of the NH2N group to rGO is the key reason for the formation of the ultrafine and well‐dispersed Ni0.4Pd0.6 UPs (1.8 nm) with relatively large surface area and more active sites. Surprisingly, the as‐prepared low‐cost NiPd/NH2‐N‐rGO dsiplays excellent hydrophilicity, 100% H2 selectivity, 100% conversion, and remarkable catalytic activity (up to 954.3 mol H2 (mol catalyst)−1 h−1) for FA decomposition at room temperature even with no additive, which is much higher than that of the best catalysts so far reported.