A General Method to Probe Oxygen Evolution Intermediates at Operating Conditions

Tao，Hua Bing1; Xu，Yinghua3; Huang，Xiang5; Chen，Jiazang4; Pei，Linjuan4; Zhang，Junming1; Chen，Jingguang G.2; Liu，Bin1

2019-06-19

10.1016/j.joule.2019.03.012

Joule   影响因子和分区

25424351

2542-4351

Reducing high overpotential for the oxygen evolution reaction (OER) is an important challenge for the utilization of clean and renewable energy resources. An obstacle that badly impedes the design of efficient OER catalysts is the weak understanding of the oxygen intermediates. Because of the aqueous reaction environment of OER, direct detection of oxygen intermediates is very challenging. Herein, we develop a general method for operando probing OER intermediates under real working conditions. We proved that the electrochemically generated oxygen intermediates of OER, e.g., OH*, are electrophiles, which could be probed by reaction with nucleophiles such as alcohol molecules. The exceptional generality of this method is demonstrated in different reaction mediums (alkaline and acid) and on various types of materials (oxides and hydroxides). The new insights of the surface chemistry on OER catalysts from the experimental approach will benefit the design of new catalysts to reduce the cost of hydrogen production. Observation of oxygen intermediates is the key to reveal the factors that limit the OER activity and thus to design better catalysts. However, the liquid reaction environment makes it very challenging to probe oxygen intermediates at operating conditions. Although several in-situ techniques have been reported for detection of intermediates on some catalysts, these methods apply only to certain circumstances. Therefore, so far, the most knowledge of oxygen intermediates is still derived from theoretical simulations. Herein, we develop a general and feasible method to probe oxygen intermediates. By employing alcohols as probing reagents, the oxygen intermediates can be readily captured. The method is so general and feasible that it can be adopted by every electrochemical laboratory. Besides the guidance for catalyst design, the chemical nature of oxygen intermediates revealed from this work also opens up new opportunities for applying OER electrode in other reactions. To develop new OER catalysts to improve efficiency for renewable energy storage, observing oxygen intermediates is essential yet challenging. Herein, based on the electronic structure and chemical property of oxygen intermediates, we design a chemical method to probe oxygen intermediates at operating conditions of OER. Alcohols are demonstrated to be excellent probing molecules to detect oxygen intermediates over various types of catalysts at different reaction media. The general and feasible method could be widely used in every electrochemical laboratory.

alcohol chemical method electrophilicity general method operando operating conditions oxygen evolution reaction oxygen intermediates

EI ; SCI

英语

ESI高被引

其他

National Natural Science Foundation of China[21576238] ; National Natural Science Foundation of China[21773285] ; National Natural Science Foundation of China[91545116] ; Ministry of Education - Singapore[MOE2016-T2-2-004] ; Ministry of Education - Singapore[RG115/17] ; Ministry of Education - Singapore[RG115/18] ; Ministry of Education - Singapore[RG9/17]

Chemistry ; Energy & Fuels ; Materials Science

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary

WOS:000472067900016

Cell Press

20192507057658

Alcohols ; Alkalinity ; Catalysts ; Electronic structure ; Hydrogen production ; Molecules ; Oxygen ; Renewable energy resources ; Surface chemistry

Gas Fuels:522 ; Energy Resources and Renewable Energy Issues:525.1 ; Chemistry, General:801.1 ; Physical Chemistry:801.4 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Atomic and Molecular Physics:931.3

2-s2.0-85067194905

Scopus

1.School of Chemical and Biomedical EngineeringNanyang Technological University,Singapore,62 Nanyang Drive,637459,Singapore
2.Department of Chemical EngineeringColumbia University,New York,10027,United States
3.State Key Laboratory Breeding Base of Green Chemistry-Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of Technology,Hangzhou,310032,China
4.State Key Laboratory of Coal ConversionInstitute of Coal ChemistryChinese Academy of Sciences,Taiyuan,030001,China
5.Department of PhysicsSouthern University of Science and Technology,Shenzhen,518055,China

Tao，Hua Bing,Xu，Yinghua,Huang，Xiang,et al. A General Method to Probe Oxygen Evolution Intermediates at Operating Conditions[J]. Joule,2019,3(6):1498-1509.

Tao，Hua Bing.,Xu，Yinghua.,Huang，Xiang.,Chen，Jiazang.,Pei，Linjuan.,...&Liu，Bin.(2019).A General Method to Probe Oxygen Evolution Intermediates at Operating Conditions.Joule,3(6),1498-1509.

Tao，Hua Bing,et al."A General Method to Probe Oxygen Evolution Intermediates at Operating Conditions".Joule 3.6(2019):1498-1509.