Activity origin and catalyst design principles for electrocatalytic hydrogen evolution on heteroatom-doped graphene
Activity origin and catalyst design principles for electrocatalytic hydrogen evolution on heteroatom-doped graphene
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DOI：
10.1038/nenergy.2016.130
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发表时间：
2016-09-12
期刊：
影响因子：
56.7
通讯作者：
Qiao, Shi-Zhang
中科院分区：
文献类型：
--
作者：
Jiao, Yan;Zheng, Yao;Qiao, Shi-Zhang
析氢反应是电催化中的一个基本过程，在水分解制氢的能量转换过程中起着重要的作用。HER的有效候选者通常基于贵金属或过渡金属二卤化物，而基于碳基的无金属电催化剂通常表现出较差的活性。本文结合光谱表征、电化学测量和密度泛函理论计算，对一系列杂原子掺杂石墨烯材料作为高效的HER电催化剂进行了评价。理论计算的结果与实验观察到的本征电催化活性和HER反应机理是一致的。因此，我们建立了石墨烯材料的HER活性趋势，并探索了它们的反应性来源，以指导更高效的电催化剂的设计。我们预测，通过合理地修改特定的实验上可以实现的物理化学特性，一种实际可实现的基于石墨烯的材料将有可能超过基于金属的基准材料的性能。
The hydrogen evolution reaction (HER) is a fundamental process in electrocatalysis and plays an important role in energy conversion through water splitting to produce hydrogen. Effective candidates for HER are often based on noble metals or transition metal dichalcogenides, while carbon-based metal-free electrocatalysts generally demonstrate poorer activity. Here we report evaluation of a series of heteroatom-doped graphene materials as efficient HER electrocatalysts by combining spectroscopic characterization, electrochemical measurements, and density functional theory calculations. Results of theoretical computations are shown to be in good agreement with experimental observations regarding the intrinsic electrocatalytic activity and the HER reaction mechanism. As a result, we establish a HER activity trend for graphene-based materials, and explore their reactivity origin to guide the design of more efficient electrocatalysts. We predict that by rationally modifying particular experimentally achievable physicochemical characteristics, a practically realizable graphene-based material will have the potential to exceed the performance of the metal-based benchmark for HER.