In situ CO2-emission assisted synthesis of molybdenum carbonitride nanomaterial as hydrogen evolution electrocatalyst.
In situ CO2-emission assisted synthesis of molybdenum carbonitride nanomaterial as hydrogen evolution electrocatalyst.
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DOI：
10.1021/ja5114529
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发表时间：
2015-01
影响因子：
15
通讯作者：
Yong Zhao;K. Kamiya;K. Hashimoto;Shuji Nakanishi
中科院分区：
文献类型：
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作者：
Yong Zhao;K. Kamiya;K. Hashimoto;Shuji Nakanishi
报道了一种高效合成碳氮化钼（MoCN）纳米材料的新方法。该方案中的关键步骤是催化剂前体的制备，其通过在碳酸氢盐存在下聚合二氨基吡啶而获得。聚二氨基吡啶中丰富的氨基通过配位键与大量的钼物种结合，形成致密的钼活性中心。向合成混合物中加入碳酸氢盐导致CO2气体逸出，因为在聚合期间局部pH降低。原位形成的CO2气泡机械地将前体分解成具有高表面积的MoCN纳米材料。所合成的MoCN材料被证明是用于析氢反应（HER）的电催化剂。它表现出-0.05 V（相对于RHE）的HER起始电位和高的氢气产生速率（在-0.14 V相对于RHE，-10 mA cm（-2）），因此是迄今报道的最有效、低成本的HER催化剂之一。
We reported a novel protocol to efficiently synthesize molybdenum carbonitride (MoCN) nanomaterials with dense active sites and high surface area. The key step in this protocol is the preparation of the catalyst precursor, which was obtained by polymerizing diaminopyridine in the presence of hydrogen carbonate. The abundant amino groups in the poly diaminopyridine bound numerous Mo species via coordination bonds, resulting in the formation of dense Mo active sites. The addition of hydrogen carbonate to the synthesis mixture resulted in CO2 gas evolution as the local pH decreased during polymerization. The in situ evolved CO2 bubbles mechanically broke down the precursor into MoCN nanomaterials with a high surface area. The synthesized MoCN materials were demonstrated as an electrocatalyst for hydrogen evolution reaction (HER). It exhibited an HER onset potential of -0.05 V (vs RHE) and a high hydrogen production rate (at -0.14 V vs RHE, -10 mA cm(-2)) and is therefore one of the most efficient, low-cost HER catalysts reported to date.