Ni Bing, He Peng, Liao Wenxin, Chen Shuangming, Gu Lin, Gong Yue, Wang Kai, Zhuang Jing, Song Li, Zhou Gang, Wang Xun
Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University, Beijing, 100084, China.
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.
Small. 2018 Apr;14(14):e1703749. doi: 10.1002/smll.201703749. Epub 2018 Feb 22.
Although much attention has been paid to the exploration of highly active electrocatalysts, especially catalysts for hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR), the development of multifunctional catalysts remains a challenge. Here, we utilize AuNi heterodimers as the starting materials to achieve high activities toward HER, OER and ORR. The HER and ORR activities in an alkali environment are similar to those of Pt catalysts, and the OER activity is very high and better than that of commercial IrO . Both the experimental and calculated results suggest that the surface oxidation under oxidative conditions is the main reason for the different activities. The NiO/Ni interface which exists in the as-synthesized heterodimers contributes to high HER activity, the Ni(OH) -Ni-Au interface and the surface Ni(OH) obtained in electrochemical conditons gives rise to promising ORR and OER activities, respectively. As a comparison, a Au@Ni core-shell structure is also synthesized and examined. The core-shell structure shows lower activities for HER and OER than the heterodimers, and reduces O selectively to H O . The work here allows for the development of a method to design multifunctional catalysts via the partial oxidation of a metal surface to create different active centers.
尽管人们对高活性电催化剂的探索给予了大量关注,尤其是析氢反应(HER)、析氧反应(OER)和氧还原反应(ORR)的催化剂,但多功能催化剂的开发仍然是一项挑战。在此,我们利用金镍异二聚体作为起始材料,以实现对HER、OER和ORR的高活性。在碱性环境中的HER和ORR活性与铂催化剂相似,且OER活性非常高,优于商业IrO 。实验和计算结果均表明,氧化条件下的表面氧化是活性不同的主要原因。合成的异二聚体中存在的NiO/Ni界面有助于高HER活性,电化学条件下获得的Ni(OH) -Ni-Au界面和表面Ni(OH)分别产生了有前景的ORR和OER活性。作为对比,还合成并研究了Au@Ni核壳结构。核壳结构对HER和OER的活性低于异二聚体,且将O选择性还原为H O 。本文的工作为通过金属表面的部分氧化来设计多功能催化剂以创建不同活性中心开发了一种方法。