Double-atom catalysts as a molecular platform for heterogeneous oxygen evolution electrocatalysis

被引：0
作者：
Lichen Bai
Chia-Shuo Hsu
Duncan T. L. Alexander
Hao Ming Chen
Xile Hu
机构：
[1] Laboratory of Inorganic Synthesis and Catalysis,Department of Chemistry
[2] Institute of Chemical Sciences and Engineering,undefined
[3] Ecole Polytechnique Fédérale de Lausanne (EPFL),undefined
[4] EPFL-ISIC-LSCI,undefined
[5] BCH 3305,undefined
[6] National Taiwan University,undefined
[7] Interdisciplinary Centre for Electron Microscopy (CIME),undefined
[8] Ecole Polytechnique Fédérale de Lausanne (EPFL),undefined
[9] Electron Spectrometry and Microscopy Laboratory (LSME),undefined
[10] Institute of Physics,undefined
[11] Ecole Polytechnique Fédérale de Lausanne (EPFL),undefined
[12] National Synchrotron Radiation Research Center (NSRRC),undefined
来源：
Nature Energy | 2021年 / 6卷
关键词：
D O I：
暂无
中图分类号：
学科分类号：
摘要：
The oxygen evolution reaction (OER) is an essential anode reaction for the generation of fuels through water splitting or CO2 electroreduction. Mixed metal oxides containing Co, Fe or Ni have proved to be the most promising OER electrocatalysts in alkaline media. However, the active sites and reaction mechanisms of these catalysts are difficult to study due to their heterogeneous nature. Here we describe a general synthesis of Co-, Fe- and Ni-containing double-atom catalysts from their single-atom precursors via in situ electrochemical transformation. Characterization reveals molecule-like bimetallic active sites for these supported catalysts. For each catalyst, we propose a catalytic cycle; all exhibit bimetallic cooperation and follow a similar O–O bond-forming step. However, the mechanisms diverge in the site and source of OH− for O–O bond formation, as well as the order of proton and electron transfer. Our work demonstrates double-atom catalysts as an attractive platform for fundamental studies of heterogeneous OER electrocatalysts.
引用
收藏
页码：1054 / 1066
页数：12
相关论文
共 123 条
  • [41] Källne E(2011)Efficient water oxidation catalysts based on readily available iron coordination complexes ChemCatChem. 3 1159-13530
  • [42] Noreland E(2015)Operando analysis of NiFe and Fe oxyhydroxide electrocatalysts for water oxidation: detection of Fe Energy Environ. Sci. 8 661-13570
  • [43] Manne R(2017) by Mossbauer spectroscopy Nat. Commun. 8 13521-10299
  • [44] Calas G(2013)The importance of nickel oxyhydroxide deprotonation on its activity towards electrochemical water oxidation J. Am. Chem. Soc. 135 13567-318
  • [45] Petiau J(2013)Unraveling oxygen evolution on iron-doped beta-nickel oxyhydroxide: the key role of highly active molecular-like sites Angew. Chem. Int. Ed. 52 10295-6098
  • [46] Schmidt H(2019)Time-resolved observations of water oxidation intermediates on a cobalt oxide nanoparticle catalyst Angew. Chem. Int. Ed. 58 313-1752
  • [47] Asztalos A(2016)Identification of stabilizing high-valent active sites by operando high-energy resolution fluorescence-detected X-ray absorption spectroscopy for high-efficiency water oxidation J. Am. Chem. Soc. 138 6088-6397
  • [48] Bok F(2017)Probing edge site reactivity of oxidic cobalt water oxidation catalysts Chem. Soc. Rev. 46 1727-1018
  • [49] Voigt W(2008)Homogeneous photocatalytic water oxidation with a dinuclear Co(III)-pyridylmethylamine complex Inorg. Chem. 47 6386-391
  • [50] Burke MS(2014)In situ spectroscopic identification of mu-OO bridging on spinel Co Inorg. Chem. 53 1014-undefined
12345678910