Atomic Defects Engineering Boosts Urea Synthesis toward Carbon Dioxide and Nitrate Coelectroreduction.

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-09-18 Epub Date: 2024-09-09 DOI:10.1021/acs.nanolett.4c03451

Zifan Xu, Zhengwu Yang, Huan Lu, Jiangchen Zhu, Junlin Li, Ming-Hui Fan, Zhi Zhao, Xiangdong Kong, Ke Wang, Zhigang Geng

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Abstract

The atomic defect engineering could feasibly decorate the chemical behaviors of reaction intermediates to regulate catalytic performance. Herein, we created oxygen vacancies on the surface of In(OH)₃ nanobelts for efficient urea electrosynthesis. When the oxygen vacancies were constructed on the surface of the In(OH)₃ nanobelts, the faradaic efficiency for urea reached 80.1%, which is 2.9 times higher than that (20.7%) of the pristine In(OH)₃ nanobelts. At -0.8 V versus reversible hydrogen electrode, In(OH)₃ nanobelts with abundant oxygen vacancies exhibited partial current density for urea of -18.8 mA cm^-2. Such a value represents the highest activity for urea electrosynthesis among recent reports. Density functional theory calculations suggested that the unsaturated In sites adjacent to oxygen defects helped to optimize the adsorbed configurations of key intermediates, promoting both the C-N coupling and the activation of the adsorbed CO₂NH₂ intermediate. In-situ spectroscopy measurements further validated the promotional effect of the oxygen vacancies on urea electrosynthesis.

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原子缺陷工程促进尿素合成，实现二氧化碳和硝酸盐共电还原。

原子缺陷工程可以装饰反应中间产物的化学行为，从而调节催化性能。在此，我们在 In(OH)3 纳米颗粒表面制造了氧空位，以实现高效尿素电合成。在 In(OH)3 纳米颗粒表面形成氧空位后，尿素的远红外效率达到 80.1%，是原始 In(OH)3 纳米颗粒的 2.9 倍（20.7%）。与可逆氢电极相比，在-0.8 V电压下，具有丰富氧空位的In(OH)3纳米颗粒对尿素的部分电流密度为-18.8 mA cm-2。这一数值代表了近期报道的最高尿素电合成活性。密度泛函理论计算表明，与氧缺陷相邻的不饱和 In 位点有助于优化关键中间产物的吸附构型，促进 C-N 偶联和吸附的 CO2NH2 中间产物的活化。原位光谱测量进一步验证了氧空位对尿素电合成的促进作用。

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

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.