Nature Communications ( IF 14.7 ) Pub Date : 2023-08-08 , DOI: 10.1038/s41467-023-40467-8 Jiannan Du 1 , Guokang Han 1 , Wei Zhang 1 , Lingfeng Li 1 , Yuqi Yan 1 , Yaoxuan Shi 1 , Xue Zhang 2 , Lin Geng 3 , Zhijiang Wang 1 , Yueping Xiong 1 , Geping Yin 1 , Chunyu Du 1
The two-electron oxygen reduction reaction in acid is highly attractive to produce H2O2, a commodity chemical vital in various industry and household scenarios, which is still hindered by the sluggish reaction kinetics. Herein, both density function theory calculation and in-situ characterization demonstrate that in dual-atom CoIn catalyst, O-affinitive In atom triggers the favorable and stable adsorption of hydroxyl, which effectively optimizes the adsorption of OOH on neighboring Co. As a result, the oxygen reduction on Co atoms shifts to two-electron pathway for efficient H2O2 production in acid. The H2O2 partial current density reaches 1.92 mA cm−2 at 0.65 V in the rotating ring-disk electrode test, while the H2O2 production rate is as high as 9.68 mol g−1 h−1 in the three-phase flow cell. Additionally, the CoIn-N-C presents excellent stability during the long-term operation, verifying the practicability of the CoIn-N-C catalyst. This work provides inspiring insights into the rational design of active catalysts for H2O2 production and other catalytic systems.
中文翻译:
CoIn双原子催化剂用于通过酸中的氧还原反应生产过氧化氢
酸中的双电子氧还原反应对于生产H 2 O 2非常有吸引力,H 2 O 2 是一种在各种工业和家庭场景中至关重要的商品化学品,但其仍然受到缓慢的反应动力学的阻碍。在此,密度函数理论计算和原位表征都表明,在双原子CoIn催化剂中,O-亲和In原子引发了羟基的有利且稳定的吸附,从而有效优化了OOH在邻近Co上的吸附。 Co原子上的氧还原转变为双电子途径,以在酸中高效生产H 2 O 2。旋转环盘电极测试中0.65 V时H 2 O 2部分电流密度达到1.92 mA cm -2 ,而三元循环中H 2 O 2产率高达9.68 mol g -1 h -1 。相流动池。此外,CoIn-NC在长期运行过程中表现出优异的稳定性,验证了CoIn-NC催化剂的实用性。这项工作为 H 2 O 2生产活性催化剂和其他催化系统的合理设计提供了启发性的见解。