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Heteroatom-Doped Flash Graphene

Journal Article · · ACS Nano

Heteroatom doping can effectively tailor the local structures and electronic states of intrinsic two-dimensional materials, and endow them with modified optical, electrical, and mechanical properties. Recent studies have shown the feasibility of preparing doped graphene from graphene oxide and its derivatives via some post-treatments, including solid-state and solvothermal methods, but they require reactive and harsh reagents. However, direct synthesis of various heteroatom-doped graphene in larger quantities and high purity through bottom-up methods remains challenging. Here, we report catalyst-free and solvent-free direct synthesis of graphene doped with various heteroatoms in bulk via flash Joule heating (FJH). Seven types of heteroatom-doped flash graphene (FG) are synthesized through millisecond flashing, including single-element-doped FG (boron, nitrogen, oxygen, phosphorus, sulfur), two-element-co-doped FG (boron and nitrogen), as well as three-element-co-doped FG (boron, nitrogen, and sulfur). Here, a variety of low-cost dopants, such as elements, oxides, and organic compounds are used. The graphene quality of heteroatom-doped FG is high, and similar to intrinsic FG, the material exhibits turbostraticity, increased interlayer spacing, and superior dispersibility. Electrochemical oxygen reduction reaction of different heteroatom-doped FG is tested, and sulfur-doped FG shows the best performance. Lithium metal battery tests demonstrate that nitrogen-doped FG exhibits a smaller nucleation overpotential compared to Cu or undoped FG. The electrical energy cost for the synthesis of heteroatom-doped FG synthesis is only 1.2 to 10.7 kJ g–1, which could render the FJH method suitable for low-cost mass production of heteroatom-doped graphene.

Research Organization:
Rice Univ., Houston, TX (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
FE0031794
OSTI ID:
1881491
Journal Information:
ACS Nano, Journal Name: ACS Nano Journal Issue: 4 Vol. 16; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (43)

Synthesis, Structure, and Properties of Boron- and Nitrogen-Doped Graphene journal August 2009
Laser‐Induced Silicon Oxide for Anode‐Free Lithium Metal Batteries journal July 2020
What Can be Expected from “Anode‐Free” Lithium Metal Batteries? journal March 2021
“Metal-Free” Catalytic Oxygen Reduction Reaction on Heteroatom-Doped Graphene is Caused by Trace Metal Impurities journal November 2013
Lithiophilic Sites in Doped Graphene Guide Uniform Lithium Nucleation for Dendrite-Free Lithium Metal Anodes journal May 2017
Crystal‐Field Tuning of Photoluminescence in Two‐Dimensional Materials with Embedded Lanthanide Ions journal January 2018
Measuring disorder in graphene with the G and D bands journal August 2010
Turbostratic boron nitride (BNt) under high pressures and temperatures journal March 1986
Manganese deception on graphene and implications in catalysis journal June 2018
Why some carbons may or may not graphitize? The point of view of thermodynamics journal August 2019
Converting plastic waste pyrolysis ash into flash graphene journal April 2021
Flash graphene from rubber waste journal June 2021
N-Doped Graphitized Carbon Nanohorns as a Forefront Electrocatalyst in Highly Selective O2 Reduction to H2O2 journal January 2018
Application of SAXS and SANS in evaluation of porosity, pore size distribution and surface area of coal journal August 2004
Sulphur and nitrogen co-doped graphene-based electrocatalysts for oxygen reduction reaction in alkaline medium journal December 2019
Boron-Doped Graphene for Electrocatalytic N2 Reduction journal August 2018
Synthesis of boron and nitrogen co-doped graphene nano-platelets using a two-step solution process and catalytic properties for oxygen reduction reaction journal July 2014
Designed Catalytic Protocol for Enhancing Hydrogen Evolution Reaction Performance of P, N-Co-Doped Graphene: The Correlation of Manipulating the Dopant Allocations and Heteroatomic Structure journal November 2020
Boosting Multiple Interfaces by Co-Doped Graphene Quantum Dots for High Efficiency and Durability Perovskite Solar Cells journal February 2020
Oxidized Activated Charcoal Nanoparticles as Catalytic Superoxide Dismutase Mimetics: Evidence for Direct Participation of an Intrinsic Radical journal June 2020
Hydrogen Peroxide Generation with 100% Faradaic Efficiency on Metal-Free Carbon Black journal February 2021
Flash Graphene Morphologies journal September 2020
Flash Graphene from Plastic Waste journal October 2020
Millisecond Conversion of Metastable 2D Materials by Flash Joule Heating journal January 2021
Ultrafast and Controllable Phase Evolution by Flash Joule Heating journal June 2021
Flexible Boron-Doped Laser-Induced Graphene Microsupercapacitors journal May 2015
Will Any Crap We Put into Graphene Increase Its Electrocatalytic Effect? journal January 2020
Turbostratic 1 Boron Nitride, Thermal Transformation to Ordered-layer-lattice Boron Nitride journal December 1962
Planarized Triarylboranes: Stabilization by Structural Constraint and Their Plane-to-Bowl Conversion journal February 2012
Tunable Band Gaps and p-Type Transport Properties of Boron-Doped Graphenes by Controllable Ion Doping Using Reactive Microwave Plasma journal February 2012
Bidirectional and reversible tuning of the interlayer spacing of two-dimensional materials journal October 2021
Thermoelectric properties and performance of flexible reduced graphene oxide films up to 3,000 K journal February 2018
Gram-scale bottom-up flash graphene synthesis journal January 2020
Synthesis of boron doped graphene for oxygen reduction reaction in fuel cells journal January 2012
Heteroatom-doped graphene materials: syntheses, properties and applications journal January 2014
Doping graphene with boron: a review of synthesis methods, physicochemical characterization, and emerging applications journal January 2016
The effect of doped heteroatoms (nitrogen, boron, phosphorus) on inhibition thermal oxidation of reduced graphene oxide journal January 2016
Nitrogen and boron doped monolayer graphene by chemical vapor deposition using polystyrene, urea and boric acid journal January 2012
Quantitative characterization of defect size in graphene using Raman spectroscopy journal December 2014
Crystallite growth in graphitizing and non-graphitizing carbons journal October 1951
Solid Solution of Boron in Graphite journal March 1967
Carbothermal shock synthesis of high-entropy-alloy nanoparticles journal March 2018
Structural and Electronic Properties of Graphene Oxide and Reduced Graphene Oxide Papers Prepared by High Pressure and High Temperature Treatment journal November 2014

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