Dynamic oxygen adsorption on single-atomic Ruthenium catalyst with high performance for acidic oxygen evolution reaction

被引：599

作者：

Cao, Linlin ^{[1
]}

Luo, Qiquan ^{[2
]}

Chen, Jiajia ^{[2
]}

Wang, Lan ^{[3
]}

Lin, Yue ^{[2
]}

Wang, Huijuan ^{[4
]}

Liu, Xiaokang ^{[1
]}

Shen, Xinyi ^{[1
]}

Zhang, Wei ^{[1
]}

Liu, Wei ^{[1
]}

Qi, Zeming ^{[1
]}

Jiang, Zheng ^{[5
]}

Yang, Jinlong ^{[2
]}

Yao, Tao ^{[1
]}

机构：

[1] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China

[2] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China

[3] Southwest Univ Sci & Technol, Sch Natl Def Sci & Technol, Mianyang 621010, Sichuan, Peoples R China

[4] Univ Sci & Technol China, Expt Ctr Engn & Mat Sci, Hefei 230026, Anhui, Peoples R China

[5] Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201800, Peoples R China

来源：

NATURE COMMUNICATIONS | 2019年 / 10卷 / 1期

基金：

中国国家自然科学基金; 国家重点研发计划;

关键词：

WATER OXIDATION; REDUCTION REACTION; ACTIVE-SITES; HYDROGEN; ELECTROCATALYSTS; EFFICIENT; RU; CO; IDENTIFICATION; PHOTOCATALYST;

D O I：

10.1038/s41467-019-12886-z

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Achieving active and stable oxygen evolution reaction (OER) in acid media based on single-atom catalysts is highly promising for cost-effective and sustainable energy supply in proton electrolyte membrane electrolyzers. Here, we report an atomically dispersed Ru-1-N-4 site anchored on nitrogen-carbon support (Ru-N-C) as an efficient and durable electrocatalyst for acidic OER. The single-atom Ru-N-C catalyst delivers an exceptionally intrinsic activity, reaching a mass activity as high as 3571 A g(metal)(-1) and turnover frequency of 3348 O-2 h(-1) with a low overpotential of 267 mV at a current density of 10 mA cm(-2). The catalyst shows no evident deactivation or decomposition after 30-hour operation in acidic environment. Operando synchrotron radiation X-ray absorption spectroscopy and infrared spectroscopy identify the dynamic adsorption of single oxygen atom on Ru site under working potentials, and theoretical calculations demonstrate that the O-Ru-1-N-4 site is responsible for the high OER activity and stability.

引用

页数：9

共 56 条

[21] From ultrasoft pseudopotentials to the projector augmented-wave method [J].

Kresse, G ;

Joubert, D .

PHYSICAL REVIEW B, 1999, 59 (03) :1758-1775

[22] Synthesis and Activities of Rutile IrO2 and RuO2 Nanoparticles for Oxygen Evolution in Acid and Alkaline Solutions [J].

Lee, Youngmin ;

Suntivich, Jin ;

May, Kevin J. ;

Perry, Erin E. ;

Shao-Horn, Yang .

JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2012, 3 (03) :399-404

[23] Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells [J].

Li, Jiazhan ;

Chen, Mengjie ;

Cullen, David A. ;

Hwang, Sooyeon ;

Wang, Maoyu ;

Li, Boyang ;

Liu, Kexi ;

Karakalos, Stavros ;

Lucero, Marcos ;

Zhang, Hanguang ;

Lei, Chao ;

Xu, Hui ;

Sterbinsky, George E. ;

Feng, Zhenxing ;

Su, Dong ;

More, Karren L. ;

Wang, Guofeng ;

Wang, Zhenbo ;

Wu, Gang .

NATURE CATALYSIS, 2018, 1 (12) :935-945

[24] Boosting oxygen evolution of single-atomic ruthenium through electronic coupling with cobalt-iron layered double hydroxides [J].

Li, Pengsong ;

Wang, Maoyu ;

Duan, Xinxuan ;

Zheng, Lirong ;

Cheng, Xiaopeng ;

Zhang, Yuefei ;

Kuang, Yun ;

Li, Yaping ;

Ma, Qing ;

Feng, Zhenxing ;

Liu, Wen ;

Sun, Xiaoming .

NATURE COMMUNICATIONS, 2019, 10 (1)

[25] Water Oxidation on Pure and Doped Hematite (0001) Surfaces: Prediction of Co and Ni as Effective Dopants for Electrocatalysis [J].

Liao, Peilin ;

Keith, John A. ;

Carter, Emily A. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (32) :13296-13309

[26] Metal-free efficient photocatalyst for stable visible water splitting via a two-electron pathway [J].

Liu, Juan ;

Liu, Yang ;

Liu, Naiyun ;

Han, Yuzhi ;

Zhang, Xing ;

Huang, Hui ;

Lifshitz, Yeshayahu ;

Lee, Shuit-Tong ;

Zhong, Jun ;

Kang, Zhenhui .

SCIENCE, 2015, 347 (6225) :970-974

[27] Identification of single-site gold catalysis in acetylene hydrochlorination [J].

Malta, Grazia ;

Kondrat, Simon A. ;

Freakley, Simon J. ;

Davies, Catherine J. ;

Lu, Li ;

Dawson, Simon ;

Thetford, Adam ;

Gibson, Emma K. ;

Morgan, David J. ;

Jones, Wilm ;

Wells, Peter P. ;

Johnston, Peter ;

Catlow, C. Richard A. ;

Kiely, Christopher J. ;

Hutchings, Graham J. .

SCIENCE, 2017, 355 (6332) :1399-1402

[28] Benchmarking Hydrogen Evolving Reaction and Oxygen Evolving Reaction Electrocatalysts for Solar Water Splitting Devices [J].

McCrory, Charles C. L. ;

Jung, Suho ;

Ferrer, Ivonne M. ;

Chatman, Shawn M. ;

Peters, Jonas C. ;

Jaramillo, Thomas F. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (13) :4347-4357

[29] Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction [J].

McCrory, Charles C. L. ;

Jung, Suho ;

Peters, Jonas C. ;

Jaramillo, Thomas F. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (45) :16977-16987

[30] Structure of hydrous ruthenium oxides: Implications for charge storage [J].

McKeown, DA ;

Hagans, PL ;

Carette, LPL ;

Russell, AE ;

Swider, KE ;

Rolison, DR .

JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (23) :4825-4832

← 1 2 3 4 5 6 →