Promoting Electroreduction of CO2 and NO3− to Urea via Tandem Catalysis of Zn Single Atoms and In2O3-x

IF 24.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Advanced Energy Materials Pub Date : 2024-08-16 DOI:10.1002/aenm.202402309

Ying Zhang, Zhuohang Li, Kai Chen, Xing Yang, Hu Zhang, Xijun Liu, Ke Chu

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Abstract

Urea electrosynthesis from co-electrolysis of CO₂ and NO₃⁻ (UECN) offers an innovative route for converting waste CO₂/NO₃⁻ into valuable urea. Herein, Zn single atoms anchored on oxygen vacancy (OV)-rich In₂O_3-x (Zn₁/In₂O_3-x) are developed as a highly active and selective UECN catalyst, delivering the highest urea yield rate of 41.6 mmol h⁻¹ g⁻¹ and urea-Faradaic efficiency of 55.8% at −0.7 V in flow cell, superior to most previously reported UECN catalysts. In situ spectroscopic measurements and theoretical calculations unveil the synergy of In/Zn₁ sites and OVs in promoting the UECN process via a tandem catalysis mechanism, where Zn₁-OV site activates NO₃⁻ to form ^*NH₂ while In-OV site activates CO₂ to form ^*CO. The formed ^*CO spontaneously migrates from the In-OV site to the nearby Zn₁-OV site and then couples with ^*NH₂ to generate ^*CONH₂ which is ultimately converted into urea.

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通过 Zn 单原子和 In2O3-x 的串联催化促进 CO2 和 NO3- 电还原为尿素

二氧化碳和三氧化二氮共电解尿素电合成（UECN）为将废弃的二氧化碳/三氧化二氮转化为有价值的尿素提供了一条创新途径。在这里，锚定在富氧空位（OV）In2O3-x（Zn1/In2O3-x）上的 Zn 单原子被开发成一种高活性、高选择性的 UECN 催化剂，在流动池中-0.7 V 的电压下，尿素产率最高达 41.6 mmol h-1 g-1，尿素-法拉第效率为 55.8%，优于之前报道的大多数 UECN 催化剂。原位光谱测量和理论计算揭示了 In/Zn1 位点和 OV 在通过串联催化机制促进 UECN 过程中的协同作用，其中 Zn1-OV 位点激活 NO3- 生成 *NH2，而 In-OV 位点激活 CO2 生成 *CO。形成的 *CO 自发地从 In-OV 位点迁移到附近的 Zn1-OV 位点，然后与 *NH2 结合生成 *CONH2，最终转化为尿素。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

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.