Xie Liangbo, Wang Pengfei, Li Yi, Zhang Dongpeng, Shang Denghui, Zheng Wenwen, Xia Yuguo, Zhan Sihui, Hu Wenping
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China.
Tianjin Key Lab Clean Energy & Pollutant Control, School of Energy and Environmental Engineering, Hebei University of Technology, Tianjin, 300130, China.
Nat Commun. 2022 Sep 22;13(1):5560. doi: 10.1038/s41467-022-33149-4.
Due to environmentally friendly operation and on-site productivity, electrocatalytic singlet oxygen (O) production via O gas is of immense interest in environment purification. However, the side-on configuration of O on the catalysts surface will lead to the formation of HO, which seriously limits the selectivity and activity of O production. Herein, we show a robust N-doped CuO (N-CuO) with Pauling-type (end-on) adsorption of O at the N-Cu-O sites for the selective generation of O under direct-current electric field. We propose that Pauling-type configuration of O not only lowers the overall activation energy barrier, but also alters the reaction pathway to form O instead of HO, which is the key feature determining selectivity for the dissociation of Cu-O bonds rather than the O-O bonds. The proposed N dopant strategy is applicable to a series of transition metal oxides, providing a universal electrocatalysts design scheme for existing high-performance electrocatalytic O production.
由于环境友好的操作和现场生产力,通过氧气气体进行电催化单线态氧(O)生成在环境净化方面具有极大的吸引力。然而,催化剂表面上O的侧基构型会导致过氧化氢(HO)的形成,这严重限制了O生成的选择性和活性。在此,我们展示了一种坚固的氮掺杂氧化铜(N-CuO),其在N-Cu-O位点具有鲍林型(端基)O吸附,用于在直流电场下选择性地生成O。我们提出,O的鲍林型构型不仅降低了整体活化能垒,还改变了反应途径以形成O而不是HO,这是决定Cu-O键而非O-O键解离选择性的关键特征。所提出的氮掺杂策略适用于一系列过渡金属氧化物,为现有的高性能电催化O生成提供了一种通用的电催化剂设计方案。