A robust design of Ru quantum dot/N-doped holey graphene for efficient Li–O <sub>2</sub>batteries

Author(s): Masoud Nazarian-Samani ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Hee-Dae Lim ⁶ ^, ⁷ ^, ⁸ ^, ⁹ ^, ¹⁰ , Safa Haghighat-Shishavan ⁶ ^, ¹¹ ^, ¹² ^, ¹³ ^, ¹⁰ , Hyun-Kyung Kim ¹⁴ ^, ¹⁵ ^, ¹⁶ ^, ¹⁷ , Youngmin Ko ⁶ ^, ⁷ ^, ⁸ ^, ⁹ ^, ¹⁰ , Myeong-Seong Kim ⁶ ^, ¹¹ ^, ¹² ^, ¹³ ^, ¹⁰ , Suk-Woo Lee ⁶ ^, ¹¹ ^, ¹² ^, ¹³ ^, ¹⁰ , Seyed Farshid Kashani-Bozorg ¹ ^, ² ^, ³ ^, ⁴ ^, ⁵ , Majid Abbasi ¹⁸ ^, ¹⁹ ^, ²⁰ ^, ¹⁰ ^, ²¹ , Hwan-Uk Guim ²² ^, ²³ ^, ²⁴ ^, ¹⁰ , Dong-Ik Kim ¹⁸ ^, ¹⁹ ^, ²⁰ ^, ¹⁰ , Kwang-Chul Roh ²⁵ ^, ²⁶ ^, ²⁷ ^, ²⁸ ^, ¹⁰ , Kisuk Kang ⁶ ^, ⁷ ^, ⁸ ^, ⁹ ^, ¹⁰ , Kwang-Bum Kim ⁶ ^, ¹¹ ^, ¹² ^, ¹³ ^, ¹⁰

Publication date (Electronic): 2017

Journal: Journal of Materials Chemistry A

Publisher: Royal Society of Chemistry (RSC)

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Abstract

We present a facile, up-scalable and cost-effective strategy to prepare defect-laden holey graphene counterparts for energy-related applications.

Abstract

Herein, we report a simple, versatile, defect-engineered method to fabricate Ru quantum dots (Ru QDs) uniformly anchored on a nitrogen-doped holey graphene (NHG) monolith. It uses in situpyrolysis of mixed glucose, dicyandiamide (DCDA), and RuCl ₃, followed by an acid treatment, and a final heat treatment to introduce in-plane holes of various sizes. A novel transmission method in scanning electron microscopy was successfully implemented to directly visualize the holes with color contrast. A low accelerating voltage of 5 kV enabled prolonged observation without significant electron beam damage. The mechanisms of hole creation were examined in detail using various characterization techniques as well as control experiments. The Ru QDs had significant catalytic activity and resulted in larger in-plane holes through the graphene sheets. The mechanical strain and the chemical reactivity of Ru QDs significantly diminished the activation energy barrier for the oxidation of CC bonds in the graphene structure. The Ru QD/NHG hybrid material was utilized as an electrocatalyst for the oxygen evolution reaction in Li–O ₂batteries, showing much lower charge overpotentials compared to the bare NHG counterpart. The defect-laden holey graphene counterpart can be highly functionalized for multiple applications, leading to a new method of nanoengineering based on atomic scale defects.

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Most cited references 84

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Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984)

K. S. W. Sing (1985)

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Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

Wee-Jun Ong, Lling-Lling Tan, Yun Ng … (2016)

As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and "earth-abundant" nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The construction and characteristics of each classification of the heterojunction system will be critically reviewed, namely metal-g-C3N4, semiconductor-g-C3N4, isotype g-C3N4/g-C3N4, graphitic carbon-g-C3N4, conducting polymer-g-C3N4, sensitizer-g-C3N4, and multicomponent heterojunctions. The band structures, electronic properties, optical absorption, and interfacial charge transfer of g-C3N4-based heterostructured nanohybrids will also be theoretically discussed based on the first-principles density functional theory (DFT) calculations to provide insightful outlooks on the charge carrier dynamics. Apart from that, the advancement of the versatile photoredox applications toward artificial photosynthesis (water splitting and photofixation of CO2), environmental decontamination, and bacteria disinfection will be presented in detail. Last but not least, this comprehensive review will conclude with a summary and some invigorating perspectives on the challenges and future directions at the forefront of this research platform. It is anticipated that this review can stimulate a new research doorway to facilitate the next generation of g-C3N4-based photocatalysts with ameliorated performances by harnessing the outstanding structural, electronic, and optical properties for the development of a sustainable future without environmental detriment.

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Li-O2 and Li-S batteries with high energy storage.

Peter G Bruce, Stefan A Freunberger, Laurence J. Hardwick … (2012)

Li-ion batteries have transformed portable electronics and will play a key role in the electrification of transport. However, the highest energy storage possible for Li-ion batteries is insufficient for the long-term needs of society, for example, extended-range electric vehicles. To go beyond the horizon of Li-ion batteries is a formidable challenge; there are few options. Here we consider two: Li-air (O(2)) and Li-S. The energy that can be stored in Li-air (based on aqueous or non-aqueous electrolytes) and Li-S cells is compared with Li-ion; the operation of the cells is discussed, as are the significant hurdles that will have to be overcome if such batteries are to succeed. Fundamental scientific advances in understanding the reactions occurring in the cells as well as new materials are key to overcoming these obstacles. The potential benefits of Li-air and Li-S justify the continued research effort that will be needed.

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Author and article information

Journal

Journal ID (publisher-id): JMCAET

Title: Journal of Materials Chemistry A

Abbreviated Title: J. Mater. Chem. A

Publisher: Royal Society of Chemistry (RSC)

ISSN (Print): 2050-7488

ISSN (Electronic): 2050-7496

Publication date Created: 2017

Publication date (Electronic): 2017

Volume: 5

Issue: 2

Pages: 619-631

Affiliations

[1 ]School of Metallurgy and Materials Engineering

[2 ]College of Engineering

[3 ]University of Tehran

[4 ]Tehran 11155-4563

[5 ]IR Iran

[6 ]Department of Materials Science and Engineering

[7 ]Research Institute of Advanced Materials (RIAM)

[8 ]Seoul National University (SNU)

[9 ]Seoul 151-742

[10 ]Republic of Korea

[11 ]Yonsei University

[12 ]134 Sinchon-dong

[13 ]Seoul 120-749

[14 ]Department of Materials Science and Metallurgy

[15 ]University of Cambridge

[16 ]Cambridge CB3 0FS

[17 ]UK

[18 ]High Temperature Energy Materials Research Center

[19 ]Korea Institute of Science and Technology (KIST)

[20 ]Seoul 136-791

[21 ]Global Technology Center

[22 ]Nano-Bio Electron Microscopy Research Team

[23 ]Korea Basic Science Institute (KBSI)

[24 ]Daejeon 305-333

[25 ]Energy Efficient Materials Team

[26 ]Energy and Environmental Division

[27 ]Korea Institute of Ceramic Engineering and Technology (KICET)

[28 ]Seoul 153-801

Article

DOI: 10.1039/C6TA08427C

SO-VID: 36551c0d-13c8-4b2a-8881-51249646ff97

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A robust design of Ru quantum dot/N-doped holey graphene for efficient Li–O ₂batteries

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Photoluminescent Nanomaterials

Most cited references 84

Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984)

Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

Li-O2 and Li-S batteries with high energy storage.

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Similar content 171

Cited by 16

Most referenced authors 1,501

A robust design of Ru quantum dot/N-doped holey graphene for efficient Li–O 2batteries

Read this article at

Photoluminescent Nanomaterials

Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984)

Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

Li-O2 and Li-S batteries with high energy storage.

Journal

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Article

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A robust design of Ru quantum dot/N-doped holey graphene for efficient Li–O ₂batteries