尿素电合成中多相反应物的共活化

IF 24.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Advanced Energy Materials Pub Date : 2023-05-24 DOI:10.1002/aenm.202300946
Zheng Lv, Shuanglong Zhou, Liang Zhao, Ziyi Liu, Jiaxin Liu, Wenxia Xu, Lei Wang, Jianping Lai
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引用次数: 1

摘要

氮气和二氧化碳固定是一种环保的废物转化为能源的技术,可以取代繁琐和苛刻的工业尿素生产过程。本文设计了具有尖端和空位结构的VN-Cu3N-300催化剂,用于尿素电合成过程中多相反应物的共活化。在环境条件下,尿素产率为81µg h−1 cm−2,这是高面积活性电催化剂的首次报道,相应的法拉第效率可达28.7%。全电池电解具有良好的稳定性,在2.1 V下提供0.7 mA cm−2的电流密度。连续电解48 h后的电解液经蒸发再结晶,经1H NMR测定尿素纯度可达100%。综合分析表明,尖端效应形成的局部电场能有效促进CO2的吸附和活化。表面氮空位的存在促进了*N N*中间体的形成,保证了C - _ - N的偶联,也优化了水的解离过程,为尿素的合成提供了质子供应。因此,速率决定步骤被改变,尿素的形成得到保证。
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Coactivation of Multiphase Reactants for the Electrosynthesis of Urea

N2 and CO2 fixation is an environmentally friendly waste-to-energy technology that can replace tedious and demanding industrial urea productive processes. Here, VN-Cu3N-300 catalysts with tip and vacancy structures are designed for the coactivation of multiphase reactants in the urea electrosynthesis process. Under environmental conditions, the urea yield is 81 µg h−1 cm−2, this is the first report of high area active electrocatalyst, and the corresponding Faraday efficiency is able to reach 28.7%. The full-cell electrolysis exhibits good stability, providing a current density of 0.7 mA cm−2 at 2.1 V. The electrolyte after continuous electrolysis for 48 h is subjected to being evaporated and recrystallized, and it is determined by 1H NMR that the purity of urea can reach 100%. Comprehensive analysis shows that the local electric field formed by the tip effect can effectively promote the adsorption and activation of CO2. The presence of surface nitrogen vacancies promotes the formation of *NN* intermediates, ensuring CN coupling, and also optimizing the dissociation process of water, providing a proton supply for the synthesis of urea. Thus, the rate-determining step is altered and the formation of urea is ensured.

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来源期刊
Advanced Energy Materials
Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
41.90
自引率
4.00%
发文量
889
审稿时长
1.4 months
期刊介绍: Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.
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