文献类型：期刊文献

英文题名：Activating p-Blocking Centers in Perovskite for Efficient Water Splitting

作者：Hua, Bin[1];Li, Meng[1];Pang, Wanying[2];Tang, Weiqiang[3];Zhao, Shuangliang[3];Jin, Zhehui[2];Zeng, Yimin[4];Amirkhiz, Babak Shalchi[4];Luo, Jing-Li[1]

机构：[1]Univ Alberta, Dept Chem & Mat Engn, Edmonton, AB T6G 1H9, Canada;[2]Univ Alberta, Dept Civil & Environm Engn, Edmonton, AB T6G 1H9, Canada;[3]East China Univ Sci & Technol, Dept Chem Engn, Shanghai 200237, Peoples R China;[4]Nat Resources Canada, CanmetMAT, Hamilton, ON L8P 0A5, Canada

年份：2018

卷号：4

期号：12

起止页码：2902

外文期刊名：CHEM

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000453057600019)】；

基金：This work was supported by the Natural Sciences and Engineering Research Council of Canada (RGPIN-2016-05494) and the Canada First Research Excellence Fund.

语种：英文

摘要：Activation of the redox reaction is of prime importance for improving water-splitting reactions over transition-metal oxides with the crystal family of ABO(3) perovskites. Nowadays, much effort is being devoted to rationalizing the redox activities and searching for optimal compositions by changing the cations in A and B sites. Here, we show that different from general strategy, modification of the p-blocking centers through F-anion doping can provide opportunities to make a significant improvement in catalytic performance. Using this approach, we introduce an effective perovskite catalyst, La0.5Ba0.25Sr0.25CoO2.9-3F0.1, for water splitting. Through ab initio modeling, we show that F-anions help uplift the O p band center and activate the redox capability of the lattice O for electrocatalysis, which suggests the potential mechanisms for designing new materials. Additionally, our findings move beyond the conventional charge transfer steps on transition-metal sites and emphasize the importance of the lattice O redox mediation for electrocatalysis.