通过界面-局部耦合电场调节 d-轨道占用率，实现电催化 N2 固定

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-04 DOI:10.1016/j.apcatb.2024.123700

Xiaoxuan Wang , Jingxian Li , Yingjie Ji , Shuyuan Li , Shiyu Wang , Yanfei Sun , Xueying Gao , Zheng Tang , Huiying Zhang , Feike Zhang , Jiangzhou Xie , Zhiyu Yang , Yi-Ming Yan

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引用次数: 0

摘要

电催化氮还原反应（ENRR）为合成氨（NH3）提供了一种可持续且具有成本效益的策略。然而，ENRR 的广泛适用性目前受到催化剂界面吸附和活化 N2 的挑战的限制。为了解决这些问题，我们开发了一种创新方法，即构建一个界面电场，再加上由 W-N 键诱导的原子局部电场。这种界面-局部耦合电场可有效提高 W 活性位点的 dz2 占有率，从而显著增强 N2 的吸附和活化。这项研究深入揭示了界面-局部电场与 ENRR 高效执行之间的关系，为催化领域的未来探索和潜在突破铺平了道路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Modulating d-orbital occupancy via a coupled interfacial-local electric field for electrocatalytic N2 fixation

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Modulating d-orbital occupancy via a coupled interfacial-local electric field for electrocatalytic N2 fixation

The electrocatalytic nitrogen reduction reaction (ENRR) offers a sustainable and cost-effective strategy for ammonia (NH₃) synthesis. However, the broad applicability of ENRR is currently limited by challenges in the adsorption and activation of N₂ at the catalyst interface. Addressing these issues, we have developed an innovative approach that constructs an interfacial electric field, coupled with an atomically local electric field induced by W-N bonds. This coupled interfacial-local electric field effectively elevates the d_z² occupancy of W active sites, thereby significantly enhancing the adsorption and activation of N₂. This work provides profound insights into the relationship between the interfacial-local electric field and the efficient execution of ENRR, paving the way for future explorations and potential breakthroughs within catalytic field.

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.