Bimodal nanoporous Pd3Cu1 alloy with restrained hydrogen evolution for stable and high yield electrochemical nitrogen reduction
Bimodal nanoporous Pd3Cu1 alloy with restrained hydrogen evolution for stable and high yield electrochemical nitrogen reduction
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抑制析氢的双峰纳米多孔 Pd3Cu1 合金可实现稳定、高产率的电化学氮还原
DOI：
10.1016/j.nanoen.2019.02.019
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发表时间：
2019-04-01
期刊：
影响因子：
17.6
通讯作者：
Ding, Yi
中科院分区：
文献类型：
--
作者：
Pang, Fangjie;Wang, Zhifeng;Ding, Yi
常温常压下的电催化氮还原反应（NRR）具有很好的应用前景，但活性中心密度低、反应动力学缓慢，导致产物收率低。在这项工作中，双峰纳米多孔PdCu合金，具有三维分级互连的多孔网络和定制的Pd/Cu原子比的设计和用于电催化NRR在室温和常压下具有高的NH3产率。Pd 3Cu 1合金具有用于高活性位点密度的大表面积、用于有效反应物可接近性的双峰多孔结构以及用于受约束的析氢反应的所需电子结构，其表现出39.9 μ g h（-1）mg（cat）（-1）的高NH 3产率，这是最近报道的具有高负载量的NRR电催化剂的最高值之一。即使在相对于可逆氢电极（vsRHE）的-0.15V的低过电位下，该合金仍然可以提供超过10 μ g h（-1）mg（cat）（-1）的NRR产率。此外，Pd 3Cu 1合金的结构完整性使其成为一种高度稳定的NRR电催化剂，在18 h操作后保持100%的原始活性，保留了其具有前景的NRR电催化的巨大潜力。双峰纳米孔结构和合金策略的协同组合可用于设计用于广泛反应的高效催化剂。
Electrocatalytic nitrogen reduction reaction (NRR) under ambient temperature and pressure holds a great promise for NH3 production while it is still impeded by the low active site density and sluggish kinetics, leading to a low product yield rate. In this work, bimodal nanoporous PdCu alloys that have three-dimensional hierarchical interconnected porous network and tailored Pd/Cu atomic ratios are designed and used for electro-catalytic NRR with high NH3 yield rate at room temperature and atmosphere pressure. The Pd3Cu1 alloy that has large surface area for high active site density, bimodal porous structure for efficient reactant accessibility as well as desired electronic structure for restrained hydrogen evolution reaction exhibits a high NH3 yield rate of 39.9 mu g h(-1) mg(cat)(-1), which is among the highest values for recently reported NRR electrocatalysts with high loading amount. Even at a low overpotential of -0.15 V versus reversible hydrogen electrode (vs RHE), the alloy can still deliver a NRR yield rate of more than 10 mu g h(-1) mg(cat)(-1). Moreover, structural integrity of the Pd3Cu1 alloy makes it a highly stable NRR electrocatalyst that keeps 100% of its original activity after 18 h operation, retaining its great potential for promising NRR electrocatalysis. The synergistic combination of bimodal nanoporous structure and alloy strategy could be used to design efficient catalysts for a wide range of reactions.