Atom-Pair Catalysts Supported by N-Doped Graphene for the Nitrogen Reduction Reaction: d-Band Center-Based Descriptor.,The Journal of Physical Chemistry Letters

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Atom-Pair Catalysts Supported by N-Doped Graphene for the Nitrogen Reduction Reaction: d-Band Center-Based Descriptor.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-07-13 , DOI: 10.1021/acs.jpclett.0c01450
Ting Deng ₁ , Chao Cen _{1,

2} , Hujun Shen ₂ , Shuyi Wang _{1,

2} , Jingdong Guo ₂ , Shaohong Cai ₃ , Mingsen Deng _{2,

3}

Affiliation

Achieving an effective nitrogen reduction reaction (NRR) under mild conditions is a great challenge for industrial ammonia synthesis. NRR is often accompanied by a competing hydrogen evolution reaction (HER), which causes an extremely low Faraday efficiency. We systematically investigated the NRR reactivity of atom-pair catalysts (APCs) formed by 20 transition metal (TM) elements supported by N-doped graphene via three reaction pathways. By analyzing the correlation among the limiting potential, Gibbs free energy, and d-band center, we evaluated the activity trends of the TM APCs. Our computations revealed that the enzymatic pathway is the most suitable reaction pathway for the TM APCs, and the intrinsic activity trend of these APCs can be determined by the d-band center-based descriptor, which has a simple linear correlation with the bonding/antibonding orbital population. In addition, the NRR APCs with excellent performance have been screened out through selective analysis of the competing HER in the electrocatalytic NRR process.

中文翻译：

N掺杂石墨烯支持的氮原子还原反应的原子对催化剂：基于d带中心的描述子。

在温和条件下实现有效的氮还原反应（NRR）对于工业氨合成来说是一个巨大的挑战。NRR通常伴随着竞争性的析氢反应（HER），这会导致法拉第效率极低。我们系统地研究了由N掺杂石墨烯支撑的20种过渡金属（TM）元素通过三种反应途径形成的原子对催化剂（APC）的NRR反应性。通过分析极限电位，吉布斯自由能和d波段中心之间的相关性，我们评估了TM APC的活动趋势。我们的计算表明，酶促途径是TM APCs最合适的反应途径，这些APCs的内在活性趋势可以通过d来确定。带中心的描述符，它与键合/反键合轨道总体具有简单的线性相关性。此外，通过对电催化NRR过程中竞争性HER的选择性分析，筛选出了具有出色性能的NRR APC。

更新日期：2020-08-06

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