合理设计共价有机骨架修饰的氧空位TiO2增强电催化氮还原为氨

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-10-13 DOI:10.1016/j.apcatb.2023.123395

Biswajit Mishra , Swayamprakash Biswal , Mohd. Ussama , M. Ali Haider , Bijay P. Tripathi

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引用次数: 0

摘要

本研究的重点是合理设计基于蒽醌的共价有机骨架（TiO2−x@COF-Aq）上均匀分布的氧空位TiO2−x纳米颗粒，旨在解决Haber Bosch工艺的挑战。Ti的亲N性质和TiO2−x@COF-Aq上存在丰富的氧空位，促进了氮的吸附，促进了电催化NRR过程。理论研究表明，TiO2−x@COF-Aq抑制H+的吸附，促进氧空位的形成，并有利于N2在氧空位的吸附。合成的纳米催化剂表现出比本体氧空位TiO2−x高出数倍的电化学NRR活性，氨产量为～30μg mg-1 h–1，法拉第效率为～16%。长期稳定性研究表明了催化剂的稳健性和工业意义。通过实验和理论发现，稳定的纳米颗粒和功能化的COF之间的整体协同作用建立了对N2固定的质子耦合电子转移的基本理解。

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Rationally designed oxygen vacant TiO2 decorated with covalent organic framework for enhanced electrocatalytic nitrogen reduction to ammonia

This study focuses on the rational design of uniformly distributed oxygen vacant TiO_2−x nanoparticles supported on an anthraquinone-based covalent organic framework (TiO_2−x@COF-Aq), aiming to address the challenges of Haber-Bosch process. The N-philic nature of Ti and the presence of abundant oxygen vacant sites on the TiO_2−x@COF-Aq promote the adsorption of nitrogen, facilitating the electrocatalytic NRR process. The theoretical study reveals that TiO_2−x@COF-Aq suppresses the H⁺ adsorption, facilitates oxygen vacancy formation and favors the N₂ adsorption at oxygen vacant sites. The synthesized nanocatalyst exhibits many folds higher electrochemical NRR activity than bulk oxygen vacant TiO_2−x with an ammonia yield of ∼30 μg mg^-1 h^–1 and ∼16% Faradaic efficiency. Long term stability study manifests the robustness and industrial significance of the catalyst. The overall synergism between the stabilized nanoparticle and functionalized COF has established the fundamental understanding of the proton coupled electron transfer for N₂ fixation through experiments and theoretical findings.

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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.