The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon-Based Catalysts for Electrocatalytic Nitrogen Reduction.,Angewandte Chemie International Edition

当前位置： X-MOL 学术 › Angew. Chem. Int. Ed. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon-Based Catalysts for Electrocatalytic Nitrogen Reduction.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-02-03 , DOI: 10.1002/anie.201915001
Yuanyuan Yang ₁ , Lifu Zhang ₂ , Zhenpeng Hu ₂ , Yao Zheng ₃ , Cheng Tang ₃ , Ping Chen ₄ , Ruguang Wang ₁ , Kangwen Qiu ₁ , Jing Mao ₁ , Tao Ling ₁ , Shi-Zhang Qiao _{1,

3}

Affiliation

Cost-effective carbon-based catalysts are promising for catalyzing the electrochemical N2 reduction reaction (NRR). However, the activity origin of carbon-based catalysts towards NRR remains unclear, and regularities and rules for the rational design of carbon-based NRR electrocatalysts are still lacking. Based on a combination of theoretical calculations and experimental observations, chalcogen/oxygen group element (O, S, Se, Te) doped carbon materials were systematically evaluated as potential NRR catalysts. Heteroatom-doping-induced charge accumulation facilitates N2 adsorption on carbon atoms and spin polarization boosts the potential-determining step of the first protonation to form *NNH. Te-doped and Se-doped C catalysts exhibited high intrinsic NRR activity that is superior to most metal-based catalysts. Establishing the correlation between the electronic structure and NRR performance for carbon-based materials paves the pathway for their NRR application.

中文翻译：

电荷积聚和自旋极化在活化碳基催化剂用于电催化氮还原中的关键作用。

具有成本效益的碳基催化剂有望用于催化电化学N2还原反应（NRR）。但是，碳基催化剂对NRR的活性来源尚不清楚，并且仍然缺乏合理设计碳基NRR电催化剂的规则和规则。基于理论计算和实验观察的结合，系统地评估了硫族/氧族元素（O，S，Se，Te）掺杂的碳材料作为潜在的NRR催化剂的能力。杂原子掺杂引起的电荷积累促进了N2在碳原子上的吸附，并且自旋极化增强了第一个质子化形成* NNH的电势确定步骤。掺Te和掺Se的C催化剂表现出高的固有NRR活性，这优于大多数基于金属的催化剂。

更新日期：2020-02-14

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南