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Core@shell structured Au@SnO2 nanoparticles with improved N2 adsorption/activation and electrical conductivity for efficient N2 fixation
Science Bulletin ( IF 18.8 ) Pub Date : 2019-12-23 , DOI: 10.1016/j.scib.2019.12.019
Pengtang Wang 1 , Yujin Ji 2 , Qi Shao 1 , Youyong Li 2 , Xiaoqing Huang 1
Affiliation  

The design of electrocatalysts with enhanced adsorption and activation of nitrogen (N2) is critical for boosting the electrochemical N2 reduction (ENR). Herein, we developed an efficient strategy to facilitate N2 adsorption and activation for N2 electroreduction into ammonia (NH3) by vacancy engineering of [email protected] structured [email protected]2 nanoparticles (NPs). We found that the ultrathin amorphous SnO2 shell with enriched oxygen vacancies was conducive to adsorb N2 as well as promoted the N2 activation, meanwhile the metallic Au core ensured the good electrical conductivity for accelerating electrons transport during the electrochemical N2 reduction reaction, synergistically boosting the N2 electroreduction catalysis. As confirmed by the 15N-labeling and controlled experiments, the [email protected] [email protected] SnO2 NPs with abundant oxygen vacancies show the best performance for N2 electroreduction with the NH3 yield rate of 21.9 μg h-1 mg-1cat and faradaic efficiency of 15.2% at -0.2 VRHE, which surpass the [email protected] SnO2 NPs, individual Au NPs and all reported Au-based catalysts for ENR.



中文翻译:

核@壳结构的 Au@SnO2 纳米粒子具有改进的 N2 吸附/活化和导电性,可实现高效的 N2 固定

设计具有增强的氮 (N 2 ) 吸附和活化的电催化剂对于促进电化学 N 2还原 (ENR) 至关重要。在此,我们开发了一种有效的策略,通过 [email protected] 结构化 [email protected] 2纳米粒子 (NPs)的空位工程促进 N 2吸附和活化以将 N 2电还原为氨 (NH 3 )。我们发现富氧空位的超薄非晶SnO 2壳有利于吸附N 2并促进N 2活化,同时金属Au核确保良好的导电性以加速电化学N 2还原反应中的电子传输,协同促进N 2电还原催化。正如15 N-标记和对照实验所证实的那样,具有丰富氧空位的 [email protected] [email protected] SnO 2 NPs 显示出最佳的 N 2电还原性能,NH 3产率为 21.9 μg h -1 mg - 1 cat和法拉第效率在 -0.2 V RHE时为 15.2% ,超过了 [email protected] SnO 2NP、单个 Au NP 和所有报道的用于 ENR 的 Au 基催化剂。

更新日期:2019-12-23
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