当前位置：
X-MOL 学术
›
J. Am. Chem. Soc.
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Oxygen Vacancy-Mediated Selective C–N Coupling toward Electrocatalytic Urea Synthesis
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-06-24 , DOI: 10.1021/jacs.2c03452 Xiaoxiao Wei 1, 2 , Xiaojian Wen 2 , Yingying Liu 1 , Chen Chen 1 , Chao Xie 1 , Dongdong Wang 1 , Mengyi Qiu 1 , Nihan He 1 , Peng Zhou 1, 2 , Wei Chen 1 , Jun Cheng 3 , Hongzhen Lin 4 , Jianfeng Jia 5 , Xian-Zhu Fu 2 , Shuangyin Wang 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-06-24 , DOI: 10.1021/jacs.2c03452 Xiaoxiao Wei 1, 2 , Xiaojian Wen 2 , Yingying Liu 1 , Chen Chen 1 , Chao Xie 1 , Dongdong Wang 1 , Mengyi Qiu 1 , Nihan He 1 , Peng Zhou 1, 2 , Wei Chen 1 , Jun Cheng 3 , Hongzhen Lin 4 , Jianfeng Jia 5 , Xian-Zhu Fu 2 , Shuangyin Wang 1
Affiliation
|
The electrocatalytic C–N coupling for one-step urea synthesis under ambient conditions serves as the promising alternative to the traditional urea synthetic protocol. However, the hydrogenation of intermediate species hinders the efficient urea synthesis. Herein, the oxygen vacancy-enriched CeO2 was demonstrated as the efficient electrocatalyst with the stabilization of the crucial intermediate of *NO via inserting into vacant sites, which is conducive to the subsequent C–N coupling process rather than protonation, whereas the poor selectivity of C–N coupling with protonation was observed on the vacancy-deficient catalyst. The oxygen vacancy-mediated selective C–N coupling was distinguished and validated by the in situ sum frequency generation spectroscopy. The introduction of oxygen vacancies tailors the common catalyst carrier into an efficient electrocatalyst with a high urea yield rate of 943.6 mg h–1 g–1, superior than that of partial noble-metal-based electrocatalysts. This work provides novel insights into the catalyst design and developments of coupling systems.
中文翻译：
氧空位介导的选择性C-N偶联电催化尿素合成
在环境条件下用于一步合成尿素的电催化 C-N 偶联是传统尿素合成方案的有希望的替代方案。然而，中间物质的加氢阻碍了尿素的有效合成。在此，富氧空位的CeO 2被证明是一种有效的电催化剂，通过插入空位来稳定*NO的关键中间体，这有利于随后的C-N偶联过程而不是质子化，而选择性较差在空位缺陷催化剂上观察到 C-N 与质子化偶联。氧空位介导的选择性 C-N 耦合通过原位识别和验证和频发生光谱。氧空位的引入使普通催化剂载体成为一种高效的电催化剂，尿素产率高达 943.6 mg h -1 g -1，优于部分贵金属基电催化剂。这项工作为耦合系统的催化剂设计和开发提供了新的见解。
更新日期：2022-06-24
中文翻译：
氧空位介导的选择性C-N偶联电催化尿素合成
在环境条件下用于一步合成尿素的电催化 C-N 偶联是传统尿素合成方案的有希望的替代方案。然而，中间物质的加氢阻碍了尿素的有效合成。在此，富氧空位的CeO 2被证明是一种有效的电催化剂，通过插入空位来稳定*NO的关键中间体，这有利于随后的C-N偶联过程而不是质子化，而选择性较差在空位缺陷催化剂上观察到 C-N 与质子化偶联。氧空位介导的选择性 C-N 耦合通过原位识别和验证和频发生光谱。氧空位的引入使普通催化剂载体成为一种高效的电催化剂，尿素产率高达 943.6 mg h -1 g -1，优于部分贵金属基电催化剂。这项工作为耦合系统的催化剂设计和开发提供了新的见解。
京公网安备 11010802027423号